Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without ...Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without the dependence of antibiotic.Methods:Herein,we prepared ultrasound/magnetic field-responsive ferroferric oxide nanoparticles(Fe_(3)O_(4))/glucose oxidase microbubbles(FGMB)to form a cascade catalytic system for effective removing methicillin-resistant Staphylococcus aureus biofilms.FGMB were prepared through interfacial self-assembly of Fe_(3)O_(4) nanoparticles(NPs)and glucose oxidase(GOx)at the gas-liquid interface stabilized by surfactants.Under ultrasound/magnetic field stimulation,FGMB disrupted biofilm architecture through microbubble collapse-induced microjets and magnetically driven displacement.Simultaneously,ultrasound-triggered rupture of FGMB released GOx and Fe_(3)O_(4) NPs.Glucose can be oxidized by GOx to generate gluconic acid and hydrogen peroxide which was subsequently catalyzed into hydroxyl radicals by Fe_(3)O_(4) NPs,enabling chemical eradication of biofilm-embedded bacteria.Results:Optical microscopy images demonstrated that FGMB have spherical structure with average size of approximately 17μm.FGMB showed a 65.4%decrease in methicillin-resistant Staphylococcus aureus biofilm biomass and 1.1 log bacterial inactivation efficiency(91.2%),suggesting effective biofilm elimination.In vitro experimental results also indicate that FGMB have good biocompatibility.Conclusion:This antibiofilm strategy integrated dual modes of physical biofilm disruption with chemical bacteria-killing shows great potential as a versatile,non-resistant strategy for bacterial biofilm elimination.展开更多
Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespr...Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.展开更多
Lithium-sulfur(Li-S)batteries have great promise for next-generation energy storage devices due to the high theoretical specific capacity(1675 mAh g^(-1))of sulfur with chemical conversion for charge storage.However,t...Lithium-sulfur(Li-S)batteries have great promise for next-generation energy storage devices due to the high theoretical specific capacity(1675 mAh g^(-1))of sulfur with chemical conversion for charge storage.However,their practical use is hindered by the slow redox kinetics of sulfur and the“shuttle effect”arising from dissolved lithium polysulfides(LiPSs).In recent years,various carbon-based materials have served as sulfur hosts and catalysts for accelerating sulfur conversion redox kinetics and alleviating LiPS shuttling.However,they often suffer from irreversible passivation and structural changes that destroy their long-term performance.We consider the main problems limiting their stability,including excessive LiPS adsorption,passivation by insulating Li2S,and surface reconstruction,and clarify how these factors lead to capacity fade.We then outline effective strategies for achieving long-term sulfur catalysis,focusing on functional carbon,such as designing suitable carbon-supported catalyst interfaces,creating well-distributed active sites,adding cocatalysts to improve electron transfer,and using carbon-based protective layers to suppress unwanted side reactions.Using this information should enable the development of stable,high-activity catalysts capable of long-term operation under practical conditions in Li-S batteries.展开更多
China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technolo...China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technology can address certain technical,environmental,and cost problems during the extraction process,the catalysts often suffer from poor stability and low catalytic efficiency.In this study,a green and simple room-temperature stirring method was employed to synthesize a class of highly efficient and stable 2D MOF catalysts,which possess the capability to conduct in-situ catalytic pyrolysis of heavy oil and reduce the viscosity.Under the condition of 160℃,a catalyst concentration of 0.5 wt%,and a hydrogen donor(tetralin)concentration of 2 wt%,the viscosity-reduction rate of Fe-MOF is as high as 89.09%,and it can decrease the asphaltene content by 8.42%.In addition,through the structural identification and analysis of crude oil asphaltenes,the causes for the high viscosity of heavy oil are explained at the molecular level.Through the analysis of catalytic products and molecular dynamics simulation,the catalytic mechanism is studied.It is discovered that Fe-MOF can interact with heavy oil macromolecules via coordination and pore-channel effects,facilitating their cracking and dispersal.Furthermore,synergistic interactions between Fe-MOF and the hydrogen donor facilitates hydrogenation reactions and enhances the viscosity-reducing effect.This study provides a novel strategy for boosting heavy oil recovery and underscores the potential of 2D MOFs in catalytic pyrolysis applications.展开更多
MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x...MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x)/P84 catalytic filter with spherical catalytic interfaces(recorded as S-MnCeO_(x)/P84)exhibits the best catalytic denitration performance.The NO_(x)removal efficiency of S-MnCeO_(x)/P84 reaches the highest value of 98.6%at 160℃when the catalyst loading is 100 g/m^(2).At the same time,S-MnCeO_(x)/P84 exhibits good SO_(2)resistance and stability,achieving a NO_(x)removal rate of 83%at 190℃with 30 ppm SO_(2).The characterization results illustrate that the MnCeO_x active component in S-MnCeO_(x)/P84 is present in weak crystalline states,tightly wrapped around the surface of the filter fiber,and uniformly dispersed,and the mesopore is the main pore structure of the S-MnCeO_(x)/P84,which can provide a channel for the catalytic reaction to proceed.At the same time,transmission electron microscopy(TEM)characterization shows that y-MnO_(2)is the main form of MnO_(2)in the S-MnCeO_(x)/P84.Further analysis of H_(2)temperature programmed reduction(H_(2)-TPR).NH_(3)temperature programmed desorption(NH_(3)-TPD)and in-situ diffuse reflectance infrared spectra(DRIFTS)show that S-MnCeO_(x)/P84 has good redox ability at 100-200℃and has abundant Lewis acid sites and Bronsteds acid sites,which provides an important guarantee for its superior low-temperature NH_(3)-SCR denitration performance.展开更多
Quantitatively mapping enzyme sequence-catalysis landscapes remains a critical challenge in understanding enzyme function,evolution,and design.In this study,we leveraged emerging microfluidic technology to measure cat...Quantitatively mapping enzyme sequence-catalysis landscapes remains a critical challenge in understanding enzyme function,evolution,and design.In this study,we leveraged emerging microfluidic technology to measure catalytic constants-kcat and KM-for hundreds of diverse orthologs and mutants of adenylate kinase(ADK).We dissected this sequence-catalysis landscape's topology,navigability,and mechanistic underpinnings,revealing catalytically heterogeneous neighborhoods organized by domain architecture.展开更多
Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great c...Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great challenge.In present work,a new strategy of chloride anion intercalation in Bi_(2)O_(3)via one-pot hydrothermal process is proposed.The as-prepared Ta-BiOCl/Bi_(24)O_(31)Cl_(10)(TBB)heterojunctions are featured with Ta-Bi_(24)O_(31)Cl_(10)and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces.In this TBB heterojunctions,the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer andmultiple transfer paths,respectively,leading to enhanced visible light response and improved photogenerated charge separation.Meanwhile,a type-II heterojunction for photocharge separation has been obtained,in which photogenerated electrons are drove from the CB(conduction band)of Ta-Bi_(24)O_(31)Cl_(10)to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl,while the photogenerated holes are left on the VB(valence band)of Ta-Bi_(24)O_(31)Cl_(10),effectively hindering the recombination of photogenerated electron-hole pairs.Furthermore,the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species(·O_(2)^(−)).Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride(TCH)solution to Bi_(2)O_(3),Ta-BiOCl and Ta-Bi_(24)O_(31)Cl_(10).This work not only proposes a Ta-BiOCl/Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-Ⅱheterojunction for highly efficient photocatalytic activity,but offers a new insight into the design of highly efficient heterojunction through phasestructure synergistic transformation strategy.展开更多
Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various ele...Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various electrolysis technologies,the emerging anion exchange membrane water electrolyser(AEMWE)exhibits the most potential for green hydrogen production,offering a potentially costeffective and sustainable approach that combines the advantages of high current density and fast start from proton exchange membrane water electrolyser(PEMWE)and low-cost catalyst from traditional alkaline water electrolyser(AWE)systems.Due to its relatively recent emergence over the past decade,a series of efforts are dedicated to improving the electrochemical reaction performance to accelerate the development and commercialization of AEMWE technology.A catalytic electrode comprising a gas diffusion layer(GDL)and a catalyst layer(CL)is usually called a gas diffusion electrode(GDE)that serves as a fundamental component within AEMWE,and also plays a core role in enhancing mass transfer during the electrolysis process.Inside the GDEs,bubbles nucleate and grow within the CL and then are transported through the GDL before eventually detaching to enter the electrolyte in the flow field.The transfer processes of water,gas bubbles,charges,and ions are intricately influenced by bubbles.This phenomenon is referred to as bubble-associated mass transfer.Like water management in fuel cells,effective bubble management is crucial in electrolysers,as its failure can result in various overpotential losses,such as activation losses,ohmic losses,and mass transfer losses,ultimately degrading the AEMWE performance.Despite significant advancements in the development of new materials and techniques in AEMWE,there is an urgent need for a comprehensive discussion focused on GDEs,with a particular emphasis on bubbleassociated mass transfer phenomena.This review aims to highlight recent findings regarding mass transfer in GDEs,particularly the impacts of bubble accumulation;and presents the latest advancements in designing CLs and GDLs to mitigate bubble-related issues.It is worth noting that a series of innovative bubble-free-GDE designs for water electrolysis are also emphasized in this review.This review is expected to be a valuable reference for gaining a deeper understanding of bubble-related mass transfer,especially the complex bubble behavior associated with GDEs,and for developing innovative practical strategies to advance AEMWE for green hydrogen production.展开更多
Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin f...Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.展开更多
The integration of surface filtration and catalytic decomposition functions in catalytic bags enables the synergistic removal of multiple pollutants(such as dust,nitrogen oxide,acid gases,and dioxins)in a single react...The integration of surface filtration and catalytic decomposition functions in catalytic bags enables the synergistic removal of multiple pollutants(such as dust,nitrogen oxide,acid gases,and dioxins)in a single reactor,thus effectively reducing the cost and operational difficulties associated with flue gas treatment.In this study,Mn-Ce-Sm-Sn(MCSS)catalysts were prepared and loaded onto hightemperature resistant polyimide(P84)filter through ultrasonic impregnation to create composite catalytic filter.The results demonstrate that the NO conversion rates of the composite catalytic filter consistently achieve above 95%within the temperature range of 160-260℃,with a chlorobenzene T_(90)value of 230℃.The ultrasonic impregnation method effectively loaded the catalyst onto the filter,ensuring high dispersion both on the surface and inside the filter.This increased exposure of catalyst active sites enhances the catalytic activity of the composite catalytic filter.Additionally,increasing the catalyst loading leads to a gradual decrease in permeability,an increase in pressure drops and the long residence time of the flue gas,thereby improving catalytic activity.Compared to ordinary impregnation methods,ultrasonic impregnation improves the bonding strength between the catalyst and filter,as well as the permeability of the composite catalytic filter under the same loading conditions.Overall,this study presents a novel approach to prepare composite catalytic filter for the simultaneous removal of NO and chlorobenzene at low temperatures.展开更多
Catalytic destruction is an ascendant technology for the abatement of volatile organic compounds(VOCs)originating fromsolvent-based industrial processes.The varied composition tends to influence each VOC’s catalytic ...Catalytic destruction is an ascendant technology for the abatement of volatile organic compounds(VOCs)originating fromsolvent-based industrial processes.The varied composition tends to influence each VOC’s catalytic behavior in the reaction mixture.We investigated the catalytic destruction of multi-component VOCs including dichloromethane(DCM)and ethyl acetate(EA),as representatives from pharmaceutical waste gases,over co-supported HxPO_(4)-RuOx/CeO_(2) catalyst.A mutual inhibitory effect relating to concentrations because of competitive adsorption was verified in the binary VOCs oxidation and EA posed a more negative effect on DCM oxidation owing to EA’s superior adsorption capacity.Preferential adsorption of EA on acidic sites(HxPO_(4)/CeO_(2))promoted DCM activation on basic sites(O^(2−))and the dominating EA oxidation blocked DCM’s access to oxidation centers(RuOx/CeO_(2)),resulting in boosted monochloromethane yield and increased chlorine deposition for DCM oxidation.The impaired redox ability of Ru species owing to chlorine deposition in turn jeopardized deep oxidation of EA and its by-products,leading to increased gaseous by-products such as acetic acid originating fromEA pyrolysis.Notably,DCM at low concentration slightly promoted EA conversion at low temperatures with or without water,consistent with the enhanced EA adsorption in co-adsorption analyses.This was mainly due to that DCM impeded the shielding effect of hydrolysate deposition from rapid EA hydrolysis depending on the decreased acidity.Moreover,water benefited EA hydrolysis but decreased CO_(2) selectivity while the generated water derived from EA was likely to affect DCM transformation.This work may provide theoretical guidance for the promotion of applied catalysts toward industrial applications.展开更多
Owing to the complexity of multicomponent gases,developing multifunctional catalysts for synergistic removal of benzene and toluene remains challenging.The spinel MMn_(2)O_(4)(M=Co,Ni,or Cu)catalysts were successfully...Owing to the complexity of multicomponent gases,developing multifunctional catalysts for synergistic removal of benzene and toluene remains challenging.The spinel MMn_(2)O_(4)(M=Co,Ni,or Cu)catalysts were successfully synthesized via the sol–gel method and tested for their catalytic performance for simultaneous degradation of benzene and toluene.The CuMn_(2)O_(4)sample exhibited the best catalytic performance,the conversion of benzene reached 100%at 350℃,and toluene conversion reached 100%at 250℃.XRD,N_(2)adsorption-desorption,HRTEM-EDS,ED-XRF,Raman spectroscopy,H_(2)-TPR,NH_(3)-TPD,O_(2)-TPD and XPS were used to characterize the physical and chemical properties of MMn_(2)O_(4)catalysts.The excellent redox properties,high concentration of surface Mn4+,and adsorption of oxygen species over the CuMn_(2)O_(4)sample facilitated the simultaneous and efficient removal of benzene and toluene.Additionally,in situ DRIFTS illustrated the intermediate species and reaction mechanism for the synergetic catalytic oxidation of benzene and toluene.Notably,as an effective catalytic material,spinel oxide exhibited excellent synergistic degradation performance for benzene and toluene,providing some insight for the development of efficient multicomponent VOC catalysts.展开更多
Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herei...Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herein,dynamic regulations of hydrogen bonding networks and solvation structures are realized by designing an asymmetric bilayer membrane consisting of a bacterial cellulose/carbon nanotube/Co_(2)(OH)_(2)CO_(3)nanorod top layer and a bacterial cellulose/Co_(2)(OH)_(2)CO_(3)nanorod(BCH)bottom layer.Crucially,the hydrogen bonding networks inside the membrane can be tuned by the rich surface–OH groups of the bacterial cellulose and Co_(2)(OH)_(2)CO_(3)as well as the ions and radicals in situ generated during the catalysis process.Moreover,both SO_(4)^(2−)and HSO_(5)−can regulate the solvation structure of Na^(+)and be adsorbed more preferentially on the evaporation surface than Cl^(−),thus hindering the de-solvation of the solvated Na^(+)and subsequent nucleation/growth of NaCl.Furthermore,the heat generated by the solar-thermal energy conversion can accelerate the reaction kinetics and enhance the catalytic degradation efficiency.This work provides a flow-bed water purification system with an asymmetric solar-thermal and catalytic membrane for synergistic solar thermal desalination of seawater/brine and catalytic degradation of organic pollutants.展开更多
BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degradi...BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degrading Rhodamine B(RhB)unde mechanical vibrations,they exhibit superior activity compared to pure ZnO.The 40wt%ZnO/BiVO_(4)heterojunction composite displayed the highest activity,along with good stability and recyclability.The enhanced piezoelectric catalytic activity can be attributed to the form ation of an I-scheme heterojunction structure,which can effectively inhibit the electron-hole recombination.Furthermore,hole(h+)and superoxide radical(·O_(2)^(-))are proved to be the primary active species.Therefore,ZnO/BiVO_(4)stands as an efficient and stable piezoelectric catalyst with broad potential application in the field of environmental water pollution treatment.展开更多
Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The developme...Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.展开更多
The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste g...The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.展开更多
Ruthenium （Ru）‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analys...Ruthenium （Ru）‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analysis of their basic properties and oxidation behavior. There is particular emphasis on Ru‐catalyzed gas‐solid catalytic reactions, including the catalytic oxidation of VOCs, preferential oxidation of CO, synthesis of ammonia, oxidation of HCl and partial oxidation of CH4. Recent litera‐ture on catalysis is summarized and compared. Finally, we describe current challenges in the field and propose approaches for future development of Ru‐based catalysts.展开更多
The practical application of lithium-sulfur(Li-S)batteries is hindered by the sluggish redox kinetics of sulfur,significant volume expansion,and the shuttle effect of lithium polysulfides(LiPSs).To address these chall...The practical application of lithium-sulfur(Li-S)batteries is hindered by the sluggish redox kinetics of sulfur,significant volume expansion,and the shuttle effect of lithium polysulfides(LiPSs).To address these challenges,this study utilizes hollow carbon spheres(HCS)as a matrix,incorporating a heterojunction of transition metal sulfides(CoS_(2)/MoS_(2))as the sulfur host.The HCS,with their ultrahigh specific surface area,effectively mitigate structural damage to the cathode caused by sulfur’s volume expansion during charge and discharge cycles.Meanwhile,the CoS_(2)/MoS_(2)heterojunction provides abundant chemical adsorption and reaction sites,which accelerate the redox kinetics of sulfur and alleviating the shuttle effect of LiPSs.Density functional theory(DFT)calculations reveal that the coupling effect at the CoS_(2)/MoS_(2)heterointerface significantly enhances charge transfer and adsorption interactions between CoS_(2)/MoS_(2)and LiPSs.Experimental results demonstrate that Li-S batteries with S/CoS_(2)/MoS_(2)@HCS composites as the cathode exhibit an exceptionally low capacity decay rate of only 0.023%per cycle after 1200 cycles at 2.0 C.Even with high sulfur loading(7.9 mg cm^(−2))and a low electrolyte-to-sulfur(E/S)ratio(6.0μL mg^(−1)),the battery achieves an outstanding areal capacity of 6.86 mA h cm^(−2).This study develops a highly efficient CoS_(2)/MoS_(2)heterojunction within HCS for the adsorption and conversion of LiPSs,providing valuable insights into the design of high-performance cathode materials for Li-S batteries.展开更多
The efficient mineralization of phenol and its derivatives in wastewater remains a great challenge.In this study,the bimetallic CuCeO_(2)-BTC was screened from a series of MOFs-derived MCeO_(2)-BTC(M=La,Cu,Co,Fe,and M...The efficient mineralization of phenol and its derivatives in wastewater remains a great challenge.In this study,the bimetallic CuCeO_(2)-BTC was screened from a series of MOFs-derived MCeO_(2)-BTC(M=La,Cu,Co,Fe,and Mn)catalysts,and the influence of the Cu/Ce ratio on phenol removal by catalytic ozonation was carefully examined.The results indicate that Cu_(2)Ce_(1)O_(y)-BTC was the best among the Cu_(x)Ce_(1)O_(y)-BTC(x=0,1,2,and 3)catalysts,with a phenol mineralization efficiency reaching close to 100%within 200 min,approximately 30.1%higher than CeO_(2)-BTC/O_(3)and 70.3%higher than O_(3)alone.The order of mineralization efficiency of phenol was Cu_(2)Ce_(1)O_(y)-BTC>Cu_(3)Ce_(1)O_(y)-BTC>Cu_(1)Ce_(1)O_(y)-BTC>CeO_(2)-BTC.CeO_(2)-BTC exhibited a broccoli-like morphology,and Cu_(x)Ce_(1)O_(y)-BTC(x=1,2,and 3)exhibited an urchin-like morphology.Compared with Cu_(x)Ce_(1)O_(y)-BTC(x=0,1,and 3),Cu_(2)Ce_(1)O_(y)-BTC exhibited a larger specific surface area and pore volume.This characteristic contributed to the availability of more active sites for phenol degradation.The redox ability was greatly enhanced as well.Besides,the surface of Cu_(2)Ce_(1)O_(y)-BTC exhibited a higher concentration of Ce^(3+)species and hydroxyl groups,which facilitated the dissociation of ozone and the generation of active radicals.Based on the results of radical quenching experiments and the intermediates detected by LC-MS,a potential mechanism for phenol degradation in the Cu_(2)Ce_(1)O_(y)-BTC/O_(3)system was postulated.This study offers novel perspectives on the advancement of MOFs-derived catalysts for achieving the complete mineralization of phenol in wastewater through catalytic ozonation.展开更多
A comparative study of products of thermal and thermocatalytic cracking of polypropylene(PP) in the presence of potassium polytitanate(PPT) synthesized by treatment of TiO_(2)(rutile) powder with molten mixture of KOH...A comparative study of products of thermal and thermocatalytic cracking of polypropylene(PP) in the presence of potassium polytitanate(PPT) synthesized by treatment of TiO_(2)(rutile) powder with molten mixture of KOH and KNO_(3) taken in a weight ratio of 30∶30∶40 has been carried out.It was shown that the studied type of PPT powder exhibits catalytic properties in the reaction of thermal decomposition of PP,compared to the effect of commercial zeolite catalyst CBV-780 traditionally used for this purpose.Based on the analysis performed,the differences in the mechanism of catalytic action of PPT and the zeolite were considered.The reasons for the observed differences in the composition of PP cracking products and in the rate of coke formation on the surface of studied catalysts were analyzed.Considering the obtained results,it has been proposed that the CBV-780 catalyst promoted more intensive production of the gaseous hydrocarbons compared to PPT,due to higher specific surface area(internal surface) accessible for relatively light and small-sized hydrocarbon products of cracking.However,intensive coke formation on the outer surface of the microporous zeolite contributes to the blocking of transport channels and the rapid loss of catalytic action.At the same time,PPT,which initially has a smaller specific surface area,retains its catalytic activity significantly longer due to slit-shaped flat pores and higher transport accessibility of the inner surface.展开更多
基金supported by the National Natural Science Foundation of China(22375101)the Natural Science of Colleges and Universities in Jiangsu Province(24KJB430027).
文摘Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without the dependence of antibiotic.Methods:Herein,we prepared ultrasound/magnetic field-responsive ferroferric oxide nanoparticles(Fe_(3)O_(4))/glucose oxidase microbubbles(FGMB)to form a cascade catalytic system for effective removing methicillin-resistant Staphylococcus aureus biofilms.FGMB were prepared through interfacial self-assembly of Fe_(3)O_(4) nanoparticles(NPs)and glucose oxidase(GOx)at the gas-liquid interface stabilized by surfactants.Under ultrasound/magnetic field stimulation,FGMB disrupted biofilm architecture through microbubble collapse-induced microjets and magnetically driven displacement.Simultaneously,ultrasound-triggered rupture of FGMB released GOx and Fe_(3)O_(4) NPs.Glucose can be oxidized by GOx to generate gluconic acid and hydrogen peroxide which was subsequently catalyzed into hydroxyl radicals by Fe_(3)O_(4) NPs,enabling chemical eradication of biofilm-embedded bacteria.Results:Optical microscopy images demonstrated that FGMB have spherical structure with average size of approximately 17μm.FGMB showed a 65.4%decrease in methicillin-resistant Staphylococcus aureus biofilm biomass and 1.1 log bacterial inactivation efficiency(91.2%),suggesting effective biofilm elimination.In vitro experimental results also indicate that FGMB have good biocompatibility.Conclusion:This antibiofilm strategy integrated dual modes of physical biofilm disruption with chemical bacteria-killing shows great potential as a versatile,non-resistant strategy for bacterial biofilm elimination.
基金supports from the National Natural Science Foundation of China(Grant Nos.12305372 and 22376217)the National Key Research&Development Program of China(Grant Nos.2022YFA1603802 and 2022YFB3504100)+1 种基金the projects of the key laboratory of advanced energy materials chemistry,ministry of education(Nankai University)key laboratory of Jiangxi Province for persistent pollutants prevention control and resource reuse(2023SSY02061)are gratefully acknowledged.
文摘Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.
文摘Lithium-sulfur(Li-S)batteries have great promise for next-generation energy storage devices due to the high theoretical specific capacity(1675 mAh g^(-1))of sulfur with chemical conversion for charge storage.However,their practical use is hindered by the slow redox kinetics of sulfur and the“shuttle effect”arising from dissolved lithium polysulfides(LiPSs).In recent years,various carbon-based materials have served as sulfur hosts and catalysts for accelerating sulfur conversion redox kinetics and alleviating LiPS shuttling.However,they often suffer from irreversible passivation and structural changes that destroy their long-term performance.We consider the main problems limiting their stability,including excessive LiPS adsorption,passivation by insulating Li2S,and surface reconstruction,and clarify how these factors lead to capacity fade.We then outline effective strategies for achieving long-term sulfur catalysis,focusing on functional carbon,such as designing suitable carbon-supported catalyst interfaces,creating well-distributed active sites,adding cocatalysts to improve electron transfer,and using carbon-based protective layers to suppress unwanted side reactions.Using this information should enable the development of stable,high-activity catalysts capable of long-term operation under practical conditions in Li-S batteries.
基金supported by the National Natural Science Foundation of China(52174047)Sinopec Project(No.P23138).
文摘China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technology can address certain technical,environmental,and cost problems during the extraction process,the catalysts often suffer from poor stability and low catalytic efficiency.In this study,a green and simple room-temperature stirring method was employed to synthesize a class of highly efficient and stable 2D MOF catalysts,which possess the capability to conduct in-situ catalytic pyrolysis of heavy oil and reduce the viscosity.Under the condition of 160℃,a catalyst concentration of 0.5 wt%,and a hydrogen donor(tetralin)concentration of 2 wt%,the viscosity-reduction rate of Fe-MOF is as high as 89.09%,and it can decrease the asphaltene content by 8.42%.In addition,through the structural identification and analysis of crude oil asphaltenes,the causes for the high viscosity of heavy oil are explained at the molecular level.Through the analysis of catalytic products and molecular dynamics simulation,the catalytic mechanism is studied.It is discovered that Fe-MOF can interact with heavy oil macromolecules via coordination and pore-channel effects,facilitating their cracking and dispersal.Furthermore,synergistic interactions between Fe-MOF and the hydrogen donor facilitates hydrogenation reactions and enhances the viscosity-reducing effect.This study provides a novel strategy for boosting heavy oil recovery and underscores the potential of 2D MOFs in catalytic pyrolysis applications.
基金Project supported by the National Natural Science Foundation of China(51902166)the Natural Science Foundation of Jiangsu Province(BK20190786)+1 种基金Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology(CICAEET)Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control。
文摘MnCeO_(x)/P84 catalytic filters with spherical,flower-like,cubic and rod-like catalytic interfaces were synthesized respectively,and their catalytic activities in the NH_(3)-SCR reaction were investigated.The MnCeO_(x)/P84 catalytic filter with spherical catalytic interfaces(recorded as S-MnCeO_(x)/P84)exhibits the best catalytic denitration performance.The NO_(x)removal efficiency of S-MnCeO_(x)/P84 reaches the highest value of 98.6%at 160℃when the catalyst loading is 100 g/m^(2).At the same time,S-MnCeO_(x)/P84 exhibits good SO_(2)resistance and stability,achieving a NO_(x)removal rate of 83%at 190℃with 30 ppm SO_(2).The characterization results illustrate that the MnCeO_x active component in S-MnCeO_(x)/P84 is present in weak crystalline states,tightly wrapped around the surface of the filter fiber,and uniformly dispersed,and the mesopore is the main pore structure of the S-MnCeO_(x)/P84,which can provide a channel for the catalytic reaction to proceed.At the same time,transmission electron microscopy(TEM)characterization shows that y-MnO_(2)is the main form of MnO_(2)in the S-MnCeO_(x)/P84.Further analysis of H_(2)temperature programmed reduction(H_(2)-TPR).NH_(3)temperature programmed desorption(NH_(3)-TPD)and in-situ diffuse reflectance infrared spectra(DRIFTS)show that S-MnCeO_(x)/P84 has good redox ability at 100-200℃and has abundant Lewis acid sites and Bronsteds acid sites,which provides an important guarantee for its superior low-temperature NH_(3)-SCR denitration performance.
文摘Quantitatively mapping enzyme sequence-catalysis landscapes remains a critical challenge in understanding enzyme function,evolution,and design.In this study,we leveraged emerging microfluidic technology to measure catalytic constants-kcat and KM-for hundreds of diverse orthologs and mutants of adenylate kinase(ADK).We dissected this sequence-catalysis landscape's topology,navigability,and mechanistic underpinnings,revealing catalytically heterogeneous neighborhoods organized by domain architecture.
基金supported by the National Natural Science Foundation of China(Nos.22208262,52271228,52202298,52201279,51834009,and 51801151)the Natural Science Foundation of Shaanxi Province(Nos.2021JQ-468,2020JZ-47)+3 种基金the Natural Science Foundation of Shaanxi Provincial Department of Education(No.21JP086)the Postdoctoral Research Foundation of China(Nos.2020M683528 and 2018M633643XB)the Young Talent Fund of Association for Science and Technology in Shaanxi,China(No.20230625)the Hundred Talent Program of Shaanxi Province.
文摘Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great challenge.In present work,a new strategy of chloride anion intercalation in Bi_(2)O_(3)via one-pot hydrothermal process is proposed.The as-prepared Ta-BiOCl/Bi_(24)O_(31)Cl_(10)(TBB)heterojunctions are featured with Ta-Bi_(24)O_(31)Cl_(10)and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces.In this TBB heterojunctions,the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer andmultiple transfer paths,respectively,leading to enhanced visible light response and improved photogenerated charge separation.Meanwhile,a type-II heterojunction for photocharge separation has been obtained,in which photogenerated electrons are drove from the CB(conduction band)of Ta-Bi_(24)O_(31)Cl_(10)to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl,while the photogenerated holes are left on the VB(valence band)of Ta-Bi_(24)O_(31)Cl_(10),effectively hindering the recombination of photogenerated electron-hole pairs.Furthermore,the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species(·O_(2)^(−)).Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride(TCH)solution to Bi_(2)O_(3),Ta-BiOCl and Ta-Bi_(24)O_(31)Cl_(10).This work not only proposes a Ta-BiOCl/Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-Ⅱheterojunction for highly efficient photocatalytic activity,but offers a new insight into the design of highly efficient heterojunction through phasestructure synergistic transformation strategy.
基金support from the National Natural Science Foundation of China(Grant No.52006029)the Promotion Foundation for Young Science and Technology Talents in Jilin Province(Grant No.QT202113)+2 种基金the Special Foundation of Industrial Innovation in Jilin Province(Grant No.2019C056-2)the Special Foundation for Outstanding Young Talents Training in Jilin(Grant No.20200104107)the UK EPSRC(EP/W03784X/1)。
文摘Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various electrolysis technologies,the emerging anion exchange membrane water electrolyser(AEMWE)exhibits the most potential for green hydrogen production,offering a potentially costeffective and sustainable approach that combines the advantages of high current density and fast start from proton exchange membrane water electrolyser(PEMWE)and low-cost catalyst from traditional alkaline water electrolyser(AWE)systems.Due to its relatively recent emergence over the past decade,a series of efforts are dedicated to improving the electrochemical reaction performance to accelerate the development and commercialization of AEMWE technology.A catalytic electrode comprising a gas diffusion layer(GDL)and a catalyst layer(CL)is usually called a gas diffusion electrode(GDE)that serves as a fundamental component within AEMWE,and also plays a core role in enhancing mass transfer during the electrolysis process.Inside the GDEs,bubbles nucleate and grow within the CL and then are transported through the GDL before eventually detaching to enter the electrolyte in the flow field.The transfer processes of water,gas bubbles,charges,and ions are intricately influenced by bubbles.This phenomenon is referred to as bubble-associated mass transfer.Like water management in fuel cells,effective bubble management is crucial in electrolysers,as its failure can result in various overpotential losses,such as activation losses,ohmic losses,and mass transfer losses,ultimately degrading the AEMWE performance.Despite significant advancements in the development of new materials and techniques in AEMWE,there is an urgent need for a comprehensive discussion focused on GDEs,with a particular emphasis on bubbleassociated mass transfer phenomena.This review aims to highlight recent findings regarding mass transfer in GDEs,particularly the impacts of bubble accumulation;and presents the latest advancements in designing CLs and GDLs to mitigate bubble-related issues.It is worth noting that a series of innovative bubble-free-GDE designs for water electrolysis are also emphasized in this review.This review is expected to be a valuable reference for gaining a deeper understanding of bubble-related mass transfer,especially the complex bubble behavior associated with GDEs,and for developing innovative practical strategies to advance AEMWE for green hydrogen production.
基金supported by the Fundamental Research Funds for the Central Universities(QNTD202302)National Natural Science Foundation of China(22378024)the Foreign expert program(G2022109001L).
文摘Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.
基金Project supported by the National Key Research and Development Program of China(2021YFB3500600,2021YFB3500605)Natural Science Foundation of Jiangsu Province(BK20220365)+5 种基金Key R&D Program of Jiangsu Province(BE2022142)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB610002)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_1419)Science and Technology Plan of Yangzhou(YZ2022030,YZ2023020)the State Key Laboratory of Clean and Efficient Coal-fired Power Generation and Pollution Control(D2022FK098)。
文摘The integration of surface filtration and catalytic decomposition functions in catalytic bags enables the synergistic removal of multiple pollutants(such as dust,nitrogen oxide,acid gases,and dioxins)in a single reactor,thus effectively reducing the cost and operational difficulties associated with flue gas treatment.In this study,Mn-Ce-Sm-Sn(MCSS)catalysts were prepared and loaded onto hightemperature resistant polyimide(P84)filter through ultrasonic impregnation to create composite catalytic filter.The results demonstrate that the NO conversion rates of the composite catalytic filter consistently achieve above 95%within the temperature range of 160-260℃,with a chlorobenzene T_(90)value of 230℃.The ultrasonic impregnation method effectively loaded the catalyst onto the filter,ensuring high dispersion both on the surface and inside the filter.This increased exposure of catalyst active sites enhances the catalytic activity of the composite catalytic filter.Additionally,increasing the catalyst loading leads to a gradual decrease in permeability,an increase in pressure drops and the long residence time of the flue gas,thereby improving catalytic activity.Compared to ordinary impregnation methods,ultrasonic impregnation improves the bonding strength between the catalyst and filter,as well as the permeability of the composite catalytic filter under the same loading conditions.Overall,this study presents a novel approach to prepare composite catalytic filter for the simultaneous removal of NO and chlorobenzene at low temperatures.
基金supported by the National Natural Science Foundation of China (Nos.21906087 and 52070168)the Key R&D Plan of Zhejiang Province (No.2023C03127)the Fundamental Research Funds for the Central Universities (No.226-2022-00150).
文摘Catalytic destruction is an ascendant technology for the abatement of volatile organic compounds(VOCs)originating fromsolvent-based industrial processes.The varied composition tends to influence each VOC’s catalytic behavior in the reaction mixture.We investigated the catalytic destruction of multi-component VOCs including dichloromethane(DCM)and ethyl acetate(EA),as representatives from pharmaceutical waste gases,over co-supported HxPO_(4)-RuOx/CeO_(2) catalyst.A mutual inhibitory effect relating to concentrations because of competitive adsorption was verified in the binary VOCs oxidation and EA posed a more negative effect on DCM oxidation owing to EA’s superior adsorption capacity.Preferential adsorption of EA on acidic sites(HxPO_(4)/CeO_(2))promoted DCM activation on basic sites(O^(2−))and the dominating EA oxidation blocked DCM’s access to oxidation centers(RuOx/CeO_(2)),resulting in boosted monochloromethane yield and increased chlorine deposition for DCM oxidation.The impaired redox ability of Ru species owing to chlorine deposition in turn jeopardized deep oxidation of EA and its by-products,leading to increased gaseous by-products such as acetic acid originating fromEA pyrolysis.Notably,DCM at low concentration slightly promoted EA conversion at low temperatures with or without water,consistent with the enhanced EA adsorption in co-adsorption analyses.This was mainly due to that DCM impeded the shielding effect of hydrolysate deposition from rapid EA hydrolysis depending on the decreased acidity.Moreover,water benefited EA hydrolysis but decreased CO_(2) selectivity while the generated water derived from EA was likely to affect DCM transformation.This work may provide theoretical guidance for the promotion of applied catalysts toward industrial applications.
基金supported by the National Natural Science Foundation of China(Nos.22206146,22006079,and U21A20524)the Fundamental Research Funds for the Central Universities,the Youth Innovation Promotion Association of Chinese Academy of Sciences,the Fundamental Research Program of Shanxi Province(No.202103021223280)+1 种基金the Special Fund for Science and Technology Innovation Teams of Shanxi Province(No.202204051002026)the Natural Science Foundation of Shandong Province(No.ZR2021QB133).
文摘Owing to the complexity of multicomponent gases,developing multifunctional catalysts for synergistic removal of benzene and toluene remains challenging.The spinel MMn_(2)O_(4)(M=Co,Ni,or Cu)catalysts were successfully synthesized via the sol–gel method and tested for their catalytic performance for simultaneous degradation of benzene and toluene.The CuMn_(2)O_(4)sample exhibited the best catalytic performance,the conversion of benzene reached 100%at 350℃,and toluene conversion reached 100%at 250℃.XRD,N_(2)adsorption-desorption,HRTEM-EDS,ED-XRF,Raman spectroscopy,H_(2)-TPR,NH_(3)-TPD,O_(2)-TPD and XPS were used to characterize the physical and chemical properties of MMn_(2)O_(4)catalysts.The excellent redox properties,high concentration of surface Mn4+,and adsorption of oxygen species over the CuMn_(2)O_(4)sample facilitated the simultaneous and efficient removal of benzene and toluene.Additionally,in situ DRIFTS illustrated the intermediate species and reaction mechanism for the synergetic catalytic oxidation of benzene and toluene.Notably,as an effective catalytic material,spinel oxide exhibited excellent synergistic degradation performance for benzene and toluene,providing some insight for the development of efficient multicomponent VOC catalysts.
基金Financial support from the National Natural Science Foundation of China(51972016)the Fundamental Research Funds for the Central Universities(JD2417)is gratefully acknowledged.
文摘Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic pollutants.Herein,dynamic regulations of hydrogen bonding networks and solvation structures are realized by designing an asymmetric bilayer membrane consisting of a bacterial cellulose/carbon nanotube/Co_(2)(OH)_(2)CO_(3)nanorod top layer and a bacterial cellulose/Co_(2)(OH)_(2)CO_(3)nanorod(BCH)bottom layer.Crucially,the hydrogen bonding networks inside the membrane can be tuned by the rich surface–OH groups of the bacterial cellulose and Co_(2)(OH)_(2)CO_(3)as well as the ions and radicals in situ generated during the catalysis process.Moreover,both SO_(4)^(2−)and HSO_(5)−can regulate the solvation structure of Na^(+)and be adsorbed more preferentially on the evaporation surface than Cl^(−),thus hindering the de-solvation of the solvated Na^(+)and subsequent nucleation/growth of NaCl.Furthermore,the heat generated by the solar-thermal energy conversion can accelerate the reaction kinetics and enhance the catalytic degradation efficiency.This work provides a flow-bed water purification system with an asymmetric solar-thermal and catalytic membrane for synergistic solar thermal desalination of seawater/brine and catalytic degradation of organic pollutants.
基金financially supported by the National Natural Science Foundation of China(No.22272151)Public Welfare Technology Application Research Project of Jinhua City,China(No.2023-4-022)。
文摘BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degrading Rhodamine B(RhB)unde mechanical vibrations,they exhibit superior activity compared to pure ZnO.The 40wt%ZnO/BiVO_(4)heterojunction composite displayed the highest activity,along with good stability and recyclability.The enhanced piezoelectric catalytic activity can be attributed to the form ation of an I-scheme heterojunction structure,which can effectively inhibit the electron-hole recombination.Furthermore,hole(h+)and superoxide radical(·O_(2)^(-))are proved to be the primary active species.Therefore,ZnO/BiVO_(4)stands as an efficient and stable piezoelectric catalyst with broad potential application in the field of environmental water pollution treatment.
基金supported by the National Natural Science Foundation of China(21325731,51478241,21221004)~~
文摘Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.
基金supported by the National Natural Science Foundation of China(22178295,21706225)Natural Science Foundation of Hunan Province(2025JJ50085)Hunan Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.
文摘The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.
基金supported by Beijing Natural Science Foundation (8164063)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB05050100)~~
文摘Ruthenium （Ru）‐based catalysts are widely employed in several types of gas‐solid reactions because of their high catalytic activities. This review provides theoretical research on Ru‐based catalysts and an analysis of their basic properties and oxidation behavior. There is particular emphasis on Ru‐catalyzed gas‐solid catalytic reactions, including the catalytic oxidation of VOCs, preferential oxidation of CO, synthesis of ammonia, oxidation of HCl and partial oxidation of CH4. Recent litera‐ture on catalysis is summarized and compared. Finally, we describe current challenges in the field and propose approaches for future development of Ru‐based catalysts.
基金supported in part by the Institute for Advanced Study of Central South University and the High Performance Computing Center of Central South University。
文摘The practical application of lithium-sulfur(Li-S)batteries is hindered by the sluggish redox kinetics of sulfur,significant volume expansion,and the shuttle effect of lithium polysulfides(LiPSs).To address these challenges,this study utilizes hollow carbon spheres(HCS)as a matrix,incorporating a heterojunction of transition metal sulfides(CoS_(2)/MoS_(2))as the sulfur host.The HCS,with their ultrahigh specific surface area,effectively mitigate structural damage to the cathode caused by sulfur’s volume expansion during charge and discharge cycles.Meanwhile,the CoS_(2)/MoS_(2)heterojunction provides abundant chemical adsorption and reaction sites,which accelerate the redox kinetics of sulfur and alleviating the shuttle effect of LiPSs.Density functional theory(DFT)calculations reveal that the coupling effect at the CoS_(2)/MoS_(2)heterointerface significantly enhances charge transfer and adsorption interactions between CoS_(2)/MoS_(2)and LiPSs.Experimental results demonstrate that Li-S batteries with S/CoS_(2)/MoS_(2)@HCS composites as the cathode exhibit an exceptionally low capacity decay rate of only 0.023%per cycle after 1200 cycles at 2.0 C.Even with high sulfur loading(7.9 mg cm^(−2))and a low electrolyte-to-sulfur(E/S)ratio(6.0μL mg^(−1)),the battery achieves an outstanding areal capacity of 6.86 mA h cm^(−2).This study develops a highly efficient CoS_(2)/MoS_(2)heterojunction within HCS for the adsorption and conversion of LiPSs,providing valuable insights into the design of high-performance cathode materials for Li-S batteries.
基金supported by the National Natural Science Foundation of China(No.22206013).
文摘The efficient mineralization of phenol and its derivatives in wastewater remains a great challenge.In this study,the bimetallic CuCeO_(2)-BTC was screened from a series of MOFs-derived MCeO_(2)-BTC(M=La,Cu,Co,Fe,and Mn)catalysts,and the influence of the Cu/Ce ratio on phenol removal by catalytic ozonation was carefully examined.The results indicate that Cu_(2)Ce_(1)O_(y)-BTC was the best among the Cu_(x)Ce_(1)O_(y)-BTC(x=0,1,2,and 3)catalysts,with a phenol mineralization efficiency reaching close to 100%within 200 min,approximately 30.1%higher than CeO_(2)-BTC/O_(3)and 70.3%higher than O_(3)alone.The order of mineralization efficiency of phenol was Cu_(2)Ce_(1)O_(y)-BTC>Cu_(3)Ce_(1)O_(y)-BTC>Cu_(1)Ce_(1)O_(y)-BTC>CeO_(2)-BTC.CeO_(2)-BTC exhibited a broccoli-like morphology,and Cu_(x)Ce_(1)O_(y)-BTC(x=1,2,and 3)exhibited an urchin-like morphology.Compared with Cu_(x)Ce_(1)O_(y)-BTC(x=0,1,and 3),Cu_(2)Ce_(1)O_(y)-BTC exhibited a larger specific surface area and pore volume.This characteristic contributed to the availability of more active sites for phenol degradation.The redox ability was greatly enhanced as well.Besides,the surface of Cu_(2)Ce_(1)O_(y)-BTC exhibited a higher concentration of Ce^(3+)species and hydroxyl groups,which facilitated the dissociation of ozone and the generation of active radicals.Based on the results of radical quenching experiments and the intermediates detected by LC-MS,a potential mechanism for phenol degradation in the Cu_(2)Ce_(1)O_(y)-BTC/O_(3)system was postulated.This study offers novel perspectives on the advancement of MOFs-derived catalysts for achieving the complete mineralization of phenol in wastewater through catalytic ozonation.
文摘A comparative study of products of thermal and thermocatalytic cracking of polypropylene(PP) in the presence of potassium polytitanate(PPT) synthesized by treatment of TiO_(2)(rutile) powder with molten mixture of KOH and KNO_(3) taken in a weight ratio of 30∶30∶40 has been carried out.It was shown that the studied type of PPT powder exhibits catalytic properties in the reaction of thermal decomposition of PP,compared to the effect of commercial zeolite catalyst CBV-780 traditionally used for this purpose.Based on the analysis performed,the differences in the mechanism of catalytic action of PPT and the zeolite were considered.The reasons for the observed differences in the composition of PP cracking products and in the rate of coke formation on the surface of studied catalysts were analyzed.Considering the obtained results,it has been proposed that the CBV-780 catalyst promoted more intensive production of the gaseous hydrocarbons compared to PPT,due to higher specific surface area(internal surface) accessible for relatively light and small-sized hydrocarbon products of cracking.However,intensive coke formation on the outer surface of the microporous zeolite contributes to the blocking of transport channels and the rapid loss of catalytic action.At the same time,PPT,which initially has a smaller specific surface area,retains its catalytic activity significantly longer due to slit-shaped flat pores and higher transport accessibility of the inner surface.
