The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunct...The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunctional evaporators and elucidating the freshwater-electricity co-generation mechanism remain challenging.In this work,we prepare porous carbon from waste polyester through a metalorganic framework(MOF)-assisted carbonization strategy and subsequently fabricate a bifunctional evaporator for freshwater-hydroelectricity co-generation.The porous carbon contains rich oxygen-containing groups and shows hierarchical micro-and mesopores with a high specific surface area of 904 m^(2)g^(-1).The porous carbon-based evaporator shows broadband and high light absorption,localized thermal management,good hydrophilicity,and high flexibility.Benefiting from these merits,it achieves high-performance freshwater and hydroelectricity co-generation,with the opencircuit voltage of 250 mV,the short-circuit current of 14μA,and the evaporation rate of 2.34 kg m^(-2)h^(-1).Hence,it is ranked among the most efficient freshwater-hydroelectricity co-generator.Additionally,the weakened hydrogen-bonding network reduces water evaporation enthalpy to 1.7 kJ g^(-1).Mechanistic investigations reveal that selective Na+interaction induces differential ion migration rate to generate streaming potential,as evidenced by molecular dynamics simulations.Meanwhile,the photothermal effect enhances voltage output by promoting interfacial ion concentration gradients.During the outdoor freshwater-electricity co-generation,it shows the voltage output of 250 mV and freshwater production of 2.34 kg m-2.This work not only puts forward a new platform to fabricate advanced evaporators from low-cost waste plastics but also unravels the freshwater-electricity co-generation mechanism,offering scalable strategies to tackle freshwater and energy crises.展开更多
Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporti...Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporting molybdenum complex on C_(3)N_(4)-K and characterized by FT-IR,XRD,SEM,XPS and ICP-OES.Heterogeneous CN–Mo-Bpy catalyst can be applied to the direct amination of nitroarenes and arylboronic acid,thus constructing various valuable diarylamines in high to excellent yields with a wide substrate scope and good functional group tolerance.It is worth noting that this heterogeneous catalyst has high chemical stability and can be recycled for at least five times without reducing its activity.展开更多
Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to add...Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to address these issues.However,the high interfacial resistance of rigid ceramic electrolytes and the limited ionic conductivity of polymer electrolytes remain significant challenges,further complicated by the substantial volume expansion of Si.In this work,we chemically grafted a flame-retardant,self-healing polyurethane-thiourea polymer onto Li_(7)P_(3)S_(11)(SHPUSB-40%LPS)via nucleophilic addition,creating an electrolyte with exceptional ionic conductivity,high elasticity,and strong compatibility with Si anodes.We observed that FSI^(-)was strongly adsorbed onto the LPS surface through electrostatic interactions with sulfur vacancies,enhancing Li^(+)transport.Furthermore,SHPUSB-40%LPS exhibits dynamic covalent disulfide bonds and hydrogen bonds,enabling self-assembly of the electrolyte at the interface.This dynamic bonding provides a self-healing mechanism that mitigates structural changes during Si expansion and contraction cycles.As a result,the Si anode with SHPUSB-40%LPS presents excellent cycling stability,retaining nearly 53.5%of its capacity after 300 cycles.The practical applicability of this design was validated in a 2 Ah all-solid-state Si‖LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)pouch cell,which maintained a stable Li-ion storage capacity retention of 76.3%after 350cycles at 0.5C.This novel solid-state electrolyte with selfhealing properties offers a promising strategy to address fundamental interfacial and performance challenges associated with Si anodes.展开更多
The dual system capable of solar-driven interfacial steam production and all-weather hydropower generation is emerging as a potential way to alleviate freshwater shortage and energy crisis.However,the intrinsic mechan...The dual system capable of solar-driven interfacial steam production and all-weather hydropower generation is emerging as a potential way to alleviate freshwater shortage and energy crisis.However,the intrinsic mechanism of hydroelectricity generation powered by the interaction between seawater and material structure is vague,and it remains challenging to develop dual-functional evaporators with high photothermal conversion efficiency and ionic selectivity.Herein,an all-weather dual-function evaporator based on porous carbon fiber-like(PCF)is acquired through the pyrolysis of barium-based metal-organic framework(Ba-BTEC),which is originated from waste polyimide.The PCF-based evaporator/device exhibits a high steam generation rate of 2.93 kg m^(-2)h^(-1)in seawater under 1 kW m^(-2)irradiation,along with the notable opencircuit voltage of 0.32 V,owing to the good light absorption ability,optimal wettability,and suitable aperture size.Moreover,molecular dynamics simulation result reveals that Na+tends to migrate rapidly within the nanoporous channels of PCF,owing to a strong affinity between oxygen-containing functional group and water molecules.This work not only proposes an eco-friendly strategy for constructing low-cost fulltime freshwater-hydroelectric co-generation device,but also contributes to the understanding of evaporation-driven energy harvesting technology.展开更多
Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,thi...Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,this photocatalytic reaction process includes the following steps:First,the semiconductor photocatalyst is photoexcited to generate photoinduced excitons on a femtosecond timescale.Next,the photoinduced excitons are separated into photogenerated electrons and holes,occurring within a femtosecond to picosecond timescale.Subsequently,only a small fraction of the photogenerated electrons and holes can overcome kinetic barriers,such as phonon scattering and bulk defects,to migrate to the surface。展开更多
Metal-Supported Solid Oxide Fuel Cells(MS-SOFCs)hold significant potential for driving the energy transition.These electrochemical devices represent the most advanced generation of Solid Oxide Fuel Cell(SOFCs)and can ...Metal-Supported Solid Oxide Fuel Cells(MS-SOFCs)hold significant potential for driving the energy transition.These electrochemical devices represent the most advanced generation of Solid Oxide Fuel Cell(SOFCs)and can pave the way for mass production and wider adoption than Proton Exchange Membrane Fuel Cells(PEMFCs)due to their fuel flexibility,higher power density and the absence of noble metals in the fabrication processes.This review examines the state-of-the-art of SOFCs and MS-SOFCs,presenting perspectives and research directions for these key technological devices,highlighting novel materials,techniques,architectures,devices,and degradation mechanisms to address current challenges and future opportunities.Techniques such as infiltration/impregnation,ex-solution catalyst synthesis,and the use of a pre-catalytic reformer layer are discussed as their impact on efficiency and prolonged activity.These concepts are also described and connected with well-dispersed nano particles,hindrance of coarsening,and an increased number of Triple Phase Boundaries(TPBs).This review also describes the synergistic use of reformers with MS-SOFCs to compose solutions in energy generation from readily available fuels.Lastly,the End-of-Life(EoL),recycling,and life-cycle assessments(LCAs)of the Fuel Cell Hybrid Electric Vehicles(FCHEVs)were discussed.LCAs comparing Fuel Cell Electric Vehicles(FCEVs)equipped with(PEMFCs)and FCHEVs equipped with MS-SOFCs,both powered with hydrogen(H_(2))generated by different routes were compared.This review aims to provide valuable insights into these key technological devices,emphasizing the importance of robust research and development to enhance performance and lifespan while reducing costs and environmental impact.展开更多
Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that...Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.展开更多
Skin sensitization is a common adverse effect of a wide range of small reactive chemicals,leading to allergic contact dermatitis(ACD),the most frequent manifestation of immunotoxicity in humans.The prevalence of ACD i...Skin sensitization is a common adverse effect of a wide range of small reactive chemicals,leading to allergic contact dermatitis(ACD),the most frequent manifestation of immunotoxicity in humans.The prevalence of ACD is increasing,affecting up to 20%of the Western European population.This trend was particularly pronounced in high-risk occupational sectors,including healthcare,food services,metal and construction workers,and hairdressers[1].The skin sensitization adverse outcome pathway(AOP)comprises 11 elements,with four designated key events(KEs):formation of proteinhapten complexes(KE-1),inflammatory keratinocyte response(KE-2),dendritic cell(DC)activation(KE-3),and T-cell proliferation(KE-4)[2].As there is no cure for ACD,preventive strategies are of great relevance.In addition to avoiding exposure,preventive measures,such as the use of latex gloves,barrier creams,emollients,and moisturizers,often have limited effectiveness[3].展开更多
Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were ...Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were generat-ed with internal excitation by multiphoton photolysis of CHBr_(3)at 248 nm,and its rotational temperature was found to relax to the flow temperature in a few microseconds by colliding with bath gas.The relaxation rate coefficients for CH(X^(2)Π,v=0)radical in He,Ar,and N_(2)flow were obtained by time-resolved laser-induced fluorescence measurements,ranging from 10^(-12)cm^(3)·molecule^(-1)·s^(-1)to 10^(-11)cm^(3)·molecule^(-1)·s^(-1).The N_(2)flow exhibits the highest relax-ation rate for CH(X^(2)Π)radical due to its additional rovibrational levels,which allow for more efficient energy dissipation during collisions compared to monoatomic gases.The Ar flow shows a larger relaxation rate than He flow due to its greater polarizability and stronger long-range interaction with the CH(X^(2)Π)radical.展开更多
In this work,atomic Co catalysts are anchored on a three-dimensional(3D)interconnected g-C_(3)N_(4)(SACo-CN)through Co-N coordination,which exhibit efficient charge carrier transition and low activation energy barrier...In this work,atomic Co catalysts are anchored on a three-dimensional(3D)interconnected g-C_(3)N_(4)(SACo-CN)through Co-N coordination,which exhibit efficient charge carrier transition and low activation energy barriers for peroxymonosulfate(PMS).The incorporation of Co atoms extends the absorption spectrum and enhances the photoelectron-hole separation efficiency of the SACo-CN samples.The 3D interconnected structure,combined with the synergistic interplay between Co-N coordination and visible light irradiation,results in SACo-CN catalysts demonstrating excellent catalytic activity and stability for PMS activation.This leads to a degradation rate of 98.8%for oxytetracycline(OTC)within 30 min under visible light.The research proposes three potential mineralization pathways with eight intermediates,leading to a significant decrease in the toxicity of the intermediates.This work provides a facile and promising approach for the preparation of metal single atom catalysts with highly efficient PMS activation performance.展开更多
This study delves into the pivotal role of sulfur vulcanization in defining the mechanical characteristics of natural rubber(NR)latex-dipped products.Utilizing sulfur vulcanization,known for its operational simplicity...This study delves into the pivotal role of sulfur vulcanization in defining the mechanical characteristics of natural rubber(NR)latex-dipped products.Utilizing sulfur vulcanization,known for its operational simplicity and cost-effectiveness,we examine its ability to enhance product elasticity and mechanical strength through various sulfidic bond formations such as mono-,di-,and polysulfidic bonds.Different vulcanization systems and sulfur contents were evaluated for their influence on the mechanical attributes of latex films,employing three types of NR latex,namely concentrated NR(CNR),deproteinized NR(DPNR),and small rubber particle NR(SRP),each representing distinct non-rubber components(NRCs).The study utilized advanced atomic force microscopy(AFM)equipped with PeakForce Quantitative Nanomechanical Mapping(QNM)to visualize and measure Young’s modulus distribution across the film of pre-vulcanized latex.Our findings reveal that films by CNR processed using the conventional vulcanization(CV)system exhibited enhanced tensile strength and elongation at break.It even showed a lower crosslink density than those processed using the efficient vulcanization(EV)system.Interestingly,DPNR films showed a more uniform distribution of Young’s modulus,correlating well with their superior mechanical strength.In contrast,SRP films showed excessive network structure formation in the particles due to accelerated vulcanization rates,hampering subsequent post-vulcanization interparticle crosslinking in film formation and remaining more rigid.The overall results Illustrate clearly that the ultimate mechanical properties of the latex films are strongly dependent on the type of sulfidic bonds formed.This research reveals further the very intricate relationship between the vulcanization methods,sulfur content,and latex type in optimizing the mechanical performance of NR latex products.It provides valuable insights for industry practices aimed at improving the quality and performance of latex-dipped goods.展开更多
Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of pho...Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of photogenerated charge carriers.Simultaneously increasing the number of active sites and improving charge separation efficiency has proven difficult.In this study,we present a novel approach combining molybdenum(Mo) monoatomic doping and size engineering to produce a series of Mo-ReS_(2) quantum dots(MR QDs) with controllable dimensions.High-resolution structural characterization,first-principle calculations,and piezo force microscopy reveal that Mo monoatomic doping enhances the lattice asymmetry,thereby improving the piezoelectric properties.The resulting piezoelectric polarization and the generated built-in electric field significantly improve charge separation efficiency,leading to optimized photocatalytic performance.Additionally,the doping strategy increases the number of active sites and improves the adsorption of intermediate radicals,substantially boosting photo-sterilization efficiency.Our results demonstrate the elimination of 99.95% of Escherichia coli and 100.00% of Staphylococcus aureus within 30 min.Furthermore,we developed a self-purification system simulating water drainage,utilizing low-frequency water streams to trigger the piezoelectric behavior of MR QDs,achieving piezoelectric synergistic photodegradation.This innovative approach provides a more environmentally friendly and economical method for water self-purification,paving the way for advanced water treatment technologies.展开更多
We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond f...We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond fission is the dominant fragmentation pathway at these wavelengths,yielding SD fragments in both the ground(X)and excited(A)electronic states.Most S(^(1)D)atoms arising via 21A′21A′the rival S atom elimination channel when exciting at~139.1 nm are formed with D_(2)partners,in a wide range of rovibrational levels.The partially resolved structure in the total translational energy distributions,P(ET),derived from the S(^(1)D)atom images,implies two dynamical routes into S(^(1)D)+D_(2)products following non-adiabatic coupling from the photo-excited Rydberg state to the dissociative potential energy surface(PES).Similar D_(2)products are evident in the P(ET)spectra derived from analysis of S(^(1)D)images from D_(2)S photolysis at~129.1 nm,but their contribution is overshadowed by a feature attributable to three-body dissociation to S(^(1)D)+2D fragments.These atomic products are deemed to arise via a natural extension of the dynamics responsible for the previously observed highly rotationally excited SD(A)fragments arising via the rival S–D bond fission pathway:asymmetric bond extension together with a dramatic opening of the interbond angle driven by torques generated after coupling to the highly anisotropic 2^(1)A′PES,leading to a centripetally-driven break-up.展开更多
Natural products play a crucial role in new drug development,but their druggability is often limited by uncertain molecular targets and insufficient research on mechanisms of action.In this study,we developed a new RP...Natural products play a crucial role in new drug development,but their druggability is often limited by uncertain molecular targets and insufficient research on mechanisms of action.In this study,we developed a new RPL19-TRAP^(KI)-seq method,combining CRISPR/Cas9 and TRAP technologies,to investigate these mechanisms.We identified and validated seven ribosomal large subunit surface proteins suitable for TRAP,selecting RPL19 for its high enrichment.We successfully established a stable cell line expressing EGFP-RPL19 using CRISPR knock-in and verified its efficiency and specificity in enriching ribosomes and translating mRNA.Integrated with next-generation sequencing,this method allows precise detection of translating mRNA.We validated RPL19-TRAP^(KI)-seq by investigating rapamycin,an mTOR inhibitor,yielding results consistent with previous reports.This optimized TRAP technology provides an accurate representation of translating mRNA,closely reflecting protein expression levels.Furthermore,we investigated SBF-1,a 23-oxa-analog of natural saponin OSW-1 with significant anti-tumor activity but an unclear mechanism.Using RPL19-TRAP^(KI)-seq,we found that SBF-1 exerts its cytotoxic effects on tumor cells by disturbing cellular oxidative phosphorylation.In conclusion,our method has been proven to be a promising tool that can reveal the mechanisms of small molecules with greater accuracy,setting the stage for future exploration of small molecules and advancing the fields of pharmacology and therapeutic development.展开更多
Understanding phosphorus sorption phenomena in different wetland sediments is important in controlling the P output in headstream watersheds. The pond chain structure （PCS） is widespread in the headstream agricultur...Understanding phosphorus sorption phenomena in different wetland sediments is important in controlling the P output in headstream watersheds. The pond chain structure （PCS） is widespread in the headstream agricultural watersheds in the southeast of China. Phosphorus sorption characteristics were determined for pond surface sediments （0-12 cm） along a pond chain structure in Liuchahe watershed of Chaohu Lake. Results showed that P sorption capacities （expressed by P sorption index （PSI）） varied both with the landscape position of the ponds and sediment depth. From foothill ponds to riverside ponds the P sorption capacities indicated a significant gradient variability. The higher elevation ponds showed greater sorption capacities, and with the pond elevation decline, P sorption capacities gradually decreased. Some physico-chemical properties, such as pH, oxalate-extractable Fe （Feox）, organic matter （TOC） and Mehlich l-extractable Ca, Mg of pond sediments also indicated significant gradient variability from high elevation ponds to low elevation ponds. Feox was the sediment parameters most highly positively correlated with PSI and was the key factor in controlling P sorption capacity in the pond chain structure （r=0.92, p〈0.001）. Long-term hydrologic and sediment inputs can affect the distribution of sediment constituents and further affect the P sorption capacity. Making the best of the spatial difference of sorption capacities of ponds in watersheds to control nonpoint source P pollutant is necessary.展开更多
A reversible storage-release process switched by a temperature difference of 10 ℃ around room temperature can be realized. This fast, recyclable, energy efficient, low cost and green system within a wide range of tem...A reversible storage-release process switched by a temperature difference of 10 ℃ around room temperature can be realized. This fast, recyclable, energy efficient, low cost and green system within a wide range of temperature and pressure is reported here for the first time. The system is believed to open up a new route for the storage and homogeneous utilization of methane.展开更多
Owing to the high viscosity of sodium silicate solution, fly ash geopolymer has the problems of low workability and rapid setting time. Therefore, the effect of chemical admixtures on the properties of fly ash geopoly...Owing to the high viscosity of sodium silicate solution, fly ash geopolymer has the problems of low workability and rapid setting time. Therefore, the effect of chemical admixtures on the properties of fly ash geopolymer was studied to overcome the rapid set of the geo-polymer in this paper. High-calcium fly ash and alkaline solution were used as starting materials to synthesize the geopolymer. Calcium chloride, calcium sulfate, sodium sulfate, and sucrose at dosages of 1wt% and 2wt% of fly ash were selected as admixtures based on concrete knowledge to improve the properties of the geopolymer. The setting time, compressive strength, and degree of reaction were recorded, and the microstructure was examined. The results show that calcium chloride significantly shortens both the initial and final setting times of the geopolymer paste. In addition, sucrose also delays the final setting time significantly. The degrees of reaction of fly ash in the geopolymer paste with the admixtures are all higher than those of the control paste. This contributes to the obvious increases in compressive strength.展开更多
Carbon monoxide(CO) as one of the three important endogenously produced signaling molecules, termed as "gasotransmitter," has emerged as a promising therapeutic agent for treating various inflammation and ce...Carbon monoxide(CO) as one of the three important endogenously produced signaling molecules, termed as "gasotransmitter," has emerged as a promising therapeutic agent for treating various inflammation and cellular-stress related diseases. In this review, we discussed CO’s evolution from a well-recognized toxic gas to a signaling molecule, and the effort to develop different approaches to deliver it for therapeutic application. We also summarize recently reported chemistry towards different CO delivery forms.展开更多
基金supported by the National Natural Science Foundation of China(52373099)Interdisciplinary Research Program of Huazhong University of Science and Technology(5003013161)+1 种基金Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)Hubei Integrative Technology and Innovation Center for Advanced Fiberous Materials(XC202502)。
文摘The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunctional evaporators and elucidating the freshwater-electricity co-generation mechanism remain challenging.In this work,we prepare porous carbon from waste polyester through a metalorganic framework(MOF)-assisted carbonization strategy and subsequently fabricate a bifunctional evaporator for freshwater-hydroelectricity co-generation.The porous carbon contains rich oxygen-containing groups and shows hierarchical micro-and mesopores with a high specific surface area of 904 m^(2)g^(-1).The porous carbon-based evaporator shows broadband and high light absorption,localized thermal management,good hydrophilicity,and high flexibility.Benefiting from these merits,it achieves high-performance freshwater and hydroelectricity co-generation,with the opencircuit voltage of 250 mV,the short-circuit current of 14μA,and the evaporation rate of 2.34 kg m^(-2)h^(-1).Hence,it is ranked among the most efficient freshwater-hydroelectricity co-generator.Additionally,the weakened hydrogen-bonding network reduces water evaporation enthalpy to 1.7 kJ g^(-1).Mechanistic investigations reveal that selective Na+interaction induces differential ion migration rate to generate streaming potential,as evidenced by molecular dynamics simulations.Meanwhile,the photothermal effect enhances voltage output by promoting interfacial ion concentration gradients.During the outdoor freshwater-electricity co-generation,it shows the voltage output of 250 mV and freshwater production of 2.34 kg m-2.This work not only puts forward a new platform to fabricate advanced evaporators from low-cost waste plastics but also unravels the freshwater-electricity co-generation mechanism,offering scalable strategies to tackle freshwater and energy crises.
基金support for this work by Hebei Education Department(No.JZX2024004)Central Guidance on Local Science and Technology Development Fund of Hebei Province(No.236Z1404G)+3 种基金the National Natural Science Foundation of China(Nos.22301060 and 21272053)China Postdoctoral Science Foundation(No.2023M730914)the Natural Science Foundation of Hebei Province(Biopharmaceutical Joint Fund No.B2022206008)Project of Science and Technology Department of Hebei Province(No.22567622H)。
文摘Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporting molybdenum complex on C_(3)N_(4)-K and characterized by FT-IR,XRD,SEM,XPS and ICP-OES.Heterogeneous CN–Mo-Bpy catalyst can be applied to the direct amination of nitroarenes and arylboronic acid,thus constructing various valuable diarylamines in high to excellent yields with a wide substrate scope and good functional group tolerance.It is worth noting that this heterogeneous catalyst has high chemical stability and can be recycled for at least five times without reducing its activity.
基金supported financially by the National Natural Science Foundation of China(No.52172202)Science and Technology Program of Guangzhou,China(No.SL2024A03J00326)+1 种基金Key Research and Development project of High-Level Scientific and Technological Talent Introduction for Luliang City(No.2023RC27)the Basic Research Program(Free Exploration Category)Project for Shanxi Province(No.202303021222251)
文摘Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to address these issues.However,the high interfacial resistance of rigid ceramic electrolytes and the limited ionic conductivity of polymer electrolytes remain significant challenges,further complicated by the substantial volume expansion of Si.In this work,we chemically grafted a flame-retardant,self-healing polyurethane-thiourea polymer onto Li_(7)P_(3)S_(11)(SHPUSB-40%LPS)via nucleophilic addition,creating an electrolyte with exceptional ionic conductivity,high elasticity,and strong compatibility with Si anodes.We observed that FSI^(-)was strongly adsorbed onto the LPS surface through electrostatic interactions with sulfur vacancies,enhancing Li^(+)transport.Furthermore,SHPUSB-40%LPS exhibits dynamic covalent disulfide bonds and hydrogen bonds,enabling self-assembly of the electrolyte at the interface.This dynamic bonding provides a self-healing mechanism that mitigates structural changes during Si expansion and contraction cycles.As a result,the Si anode with SHPUSB-40%LPS presents excellent cycling stability,retaining nearly 53.5%of its capacity after 300 cycles.The practical applicability of this design was validated in a 2 Ah all-solid-state Si‖LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)pouch cell,which maintained a stable Li-ion storage capacity retention of 76.3%after 350cycles at 0.5C.This novel solid-state electrolyte with selfhealing properties offers a promising strategy to address fundamental interfacial and performance challenges associated with Si anodes.
基金supported by National Natural Science Foundation of China(No.52373099)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)。
文摘The dual system capable of solar-driven interfacial steam production and all-weather hydropower generation is emerging as a potential way to alleviate freshwater shortage and energy crisis.However,the intrinsic mechanism of hydroelectricity generation powered by the interaction between seawater and material structure is vague,and it remains challenging to develop dual-functional evaporators with high photothermal conversion efficiency and ionic selectivity.Herein,an all-weather dual-function evaporator based on porous carbon fiber-like(PCF)is acquired through the pyrolysis of barium-based metal-organic framework(Ba-BTEC),which is originated from waste polyimide.The PCF-based evaporator/device exhibits a high steam generation rate of 2.93 kg m^(-2)h^(-1)in seawater under 1 kW m^(-2)irradiation,along with the notable opencircuit voltage of 0.32 V,owing to the good light absorption ability,optimal wettability,and suitable aperture size.Moreover,molecular dynamics simulation result reveals that Na+tends to migrate rapidly within the nanoporous channels of PCF,owing to a strong affinity between oxygen-containing functional group and water molecules.This work not only proposes an eco-friendly strategy for constructing low-cost fulltime freshwater-hydroelectric co-generation device,but also contributes to the understanding of evaporation-driven energy harvesting technology.
文摘Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,this photocatalytic reaction process includes the following steps:First,the semiconductor photocatalyst is photoexcited to generate photoinduced excitons on a femtosecond timescale.Next,the photoinduced excitons are separated into photogenerated electrons and holes,occurring within a femtosecond to picosecond timescale.Subsequently,only a small fraction of the photogenerated electrons and holes can overcome kinetic barriers,such as phonon scattering and bulk defects,to migrate to the surface。
基金the Fundacao de Amparo à Pesquisa do Estado de Sao Paulo(FAPESP,2022/02235-4,2017/11958-1,2017/11986-5,2014/02163-7)Fundacao de Apoio da UFMG(FUNDEP,27192-36,01-P-38465/2023)Conselho Nacional de Desenvolvimento Científico e Tecnológico(CNPq,405675/2022-4,56405643/2022-5,302180/2022-2,306870/2021-5)。
文摘Metal-Supported Solid Oxide Fuel Cells(MS-SOFCs)hold significant potential for driving the energy transition.These electrochemical devices represent the most advanced generation of Solid Oxide Fuel Cell(SOFCs)and can pave the way for mass production and wider adoption than Proton Exchange Membrane Fuel Cells(PEMFCs)due to their fuel flexibility,higher power density and the absence of noble metals in the fabrication processes.This review examines the state-of-the-art of SOFCs and MS-SOFCs,presenting perspectives and research directions for these key technological devices,highlighting novel materials,techniques,architectures,devices,and degradation mechanisms to address current challenges and future opportunities.Techniques such as infiltration/impregnation,ex-solution catalyst synthesis,and the use of a pre-catalytic reformer layer are discussed as their impact on efficiency and prolonged activity.These concepts are also described and connected with well-dispersed nano particles,hindrance of coarsening,and an increased number of Triple Phase Boundaries(TPBs).This review also describes the synergistic use of reformers with MS-SOFCs to compose solutions in energy generation from readily available fuels.Lastly,the End-of-Life(EoL),recycling,and life-cycle assessments(LCAs)of the Fuel Cell Hybrid Electric Vehicles(FCHEVs)were discussed.LCAs comparing Fuel Cell Electric Vehicles(FCEVs)equipped with(PEMFCs)and FCHEVs equipped with MS-SOFCs,both powered with hydrogen(H_(2))generated by different routes were compared.This review aims to provide valuable insights into these key technological devices,emphasizing the importance of robust research and development to enhance performance and lifespan while reducing costs and environmental impact.
基金the National Key R&D Plan of the Ministry of Science and Technology of China(2022YFE0122400)National Natural Science Foundation of China(52002238,22102207)+1 种基金Science and Technology Commission of Shanghai Municipality(22ZR1423800,21ZR1465200,23ZR1423600)Shanghai Municipal Education Commission and the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.
基金support was provided by the European Regional Development Fund(ERDF),through the Centro 2020 Regional Operational Programme,Portugal(Project No.:CENTRO-01-0145-FEDER-000012(HealthyAging2020))through the COMPETE 2020-Operational Programme for Competitiveness and Internationalisation and Portuguese National Funds via Fundaçao para a Ciencia e a Tecnologia,Portugal(Project Nos.:POCI-01-0145-FEDER-029369 UIDB/04539/2020,iBiMED UIDB/04501/2020,DOI identifier https://doi.org/10.54499/UIDB/04501/2020 and project reference UIDP/04501/2020,DOI identifier https://doi.org/10.54499/UIDP/04501/2020,and LA/P/0058/2020)supported by Fundaçao para a Ciencia e a Tecnologia through the individual PhD fellowships,Portugal(Grant Nos.:PD/BDE/142926/2018 and SFRH/BD/110717/2015)。
文摘Skin sensitization is a common adverse effect of a wide range of small reactive chemicals,leading to allergic contact dermatitis(ACD),the most frequent manifestation of immunotoxicity in humans.The prevalence of ACD is increasing,affecting up to 20%of the Western European population.This trend was particularly pronounced in high-risk occupational sectors,including healthcare,food services,metal and construction workers,and hairdressers[1].The skin sensitization adverse outcome pathway(AOP)comprises 11 elements,with four designated key events(KEs):formation of proteinhapten complexes(KE-1),inflammatory keratinocyte response(KE-2),dendritic cell(DC)activation(KE-3),and T-cell proliferation(KE-4)[2].As there is no cure for ACD,preventive strategies are of great relevance.In addition to avoiding exposure,preventive measures,such as the use of latex gloves,barrier creams,emollients,and moisturizers,often have limited effectiveness[3].
基金supported by the National Natural Science Foundation of China(No.22273103)the National Natural Science Foundation of China(NSFC Center for Chemical Dynamics)(No.22288201)+1 种基金Dalian Institute of Chemical Physics(DICP I202230)the Scientific Instrument Developing Project of the Chinese Academy of Sciences(grant GJJSTD20220001)。
文摘Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were generat-ed with internal excitation by multiphoton photolysis of CHBr_(3)at 248 nm,and its rotational temperature was found to relax to the flow temperature in a few microseconds by colliding with bath gas.The relaxation rate coefficients for CH(X^(2)Π,v=0)radical in He,Ar,and N_(2)flow were obtained by time-resolved laser-induced fluorescence measurements,ranging from 10^(-12)cm^(3)·molecule^(-1)·s^(-1)to 10^(-11)cm^(3)·molecule^(-1)·s^(-1).The N_(2)flow exhibits the highest relax-ation rate for CH(X^(2)Π)radical due to its additional rovibrational levels,which allow for more efficient energy dissipation during collisions compared to monoatomic gases.The Ar flow shows a larger relaxation rate than He flow due to its greater polarizability and stronger long-range interaction with the CH(X^(2)Π)radical.
基金financial support from the National Natural Science Foundation of China(Nos.22276159,J2224005)the Key research project plan for higher education institutions of Henan province(No.24ZX009)+1 种基金the Development Program for Key Young Teachers in Colleges and Universities of Henan Province(No.2020GGJS146)the Starting Research Fund of Xinxiang Medical University(No.XYBSKYZZ201911)。
文摘In this work,atomic Co catalysts are anchored on a three-dimensional(3D)interconnected g-C_(3)N_(4)(SACo-CN)through Co-N coordination,which exhibit efficient charge carrier transition and low activation energy barriers for peroxymonosulfate(PMS).The incorporation of Co atoms extends the absorption spectrum and enhances the photoelectron-hole separation efficiency of the SACo-CN samples.The 3D interconnected structure,combined with the synergistic interplay between Co-N coordination and visible light irradiation,results in SACo-CN catalysts demonstrating excellent catalytic activity and stability for PMS activation.This leads to a degradation rate of 98.8%for oxytetracycline(OTC)within 30 min under visible light.The research proposes three potential mineralization pathways with eight intermediates,leading to a significant decrease in the toxicity of the intermediates.This work provides a facile and promising approach for the preparation of metal single atom catalysts with highly efficient PMS activation performance.
基金supported by Mahidol University(Fundamental Fund:fiscal year 2024 by the National Science Research and Innovation Fund(NSRF),FF-078/2567)Academy of Tropical Agricultural Sciences for Science and Technology Innovation Team of National Tropical Agricultural Science Center(No.CATASCXTD202401)the National Research Council of Thailand(NRCT)via the Royal Golden Jubilee Ph.D.Program(No.PHD/0150/2560)。
文摘This study delves into the pivotal role of sulfur vulcanization in defining the mechanical characteristics of natural rubber(NR)latex-dipped products.Utilizing sulfur vulcanization,known for its operational simplicity and cost-effectiveness,we examine its ability to enhance product elasticity and mechanical strength through various sulfidic bond formations such as mono-,di-,and polysulfidic bonds.Different vulcanization systems and sulfur contents were evaluated for their influence on the mechanical attributes of latex films,employing three types of NR latex,namely concentrated NR(CNR),deproteinized NR(DPNR),and small rubber particle NR(SRP),each representing distinct non-rubber components(NRCs).The study utilized advanced atomic force microscopy(AFM)equipped with PeakForce Quantitative Nanomechanical Mapping(QNM)to visualize and measure Young’s modulus distribution across the film of pre-vulcanized latex.Our findings reveal that films by CNR processed using the conventional vulcanization(CV)system exhibited enhanced tensile strength and elongation at break.It even showed a lower crosslink density than those processed using the efficient vulcanization(EV)system.Interestingly,DPNR films showed a more uniform distribution of Young’s modulus,correlating well with their superior mechanical strength.In contrast,SRP films showed excessive network structure formation in the particles due to accelerated vulcanization rates,hampering subsequent post-vulcanization interparticle crosslinking in film formation and remaining more rigid.The overall results Illustrate clearly that the ultimate mechanical properties of the latex films are strongly dependent on the type of sulfidic bonds formed.This research reveals further the very intricate relationship between the vulcanization methods,sulfur content,and latex type in optimizing the mechanical performance of NR latex products.It provides valuable insights for industry practices aimed at improving the quality and performance of latex-dipped goods.
基金financially supported by the National Natural Science Foundation of China (No.52071146)Guangdong Provincial Natural Science Foundation (No.2023A1515010989)the Science and Technology Projects in Guangzhou (No.202201000008)。
文摘Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of photogenerated charge carriers.Simultaneously increasing the number of active sites and improving charge separation efficiency has proven difficult.In this study,we present a novel approach combining molybdenum(Mo) monoatomic doping and size engineering to produce a series of Mo-ReS_(2) quantum dots(MR QDs) with controllable dimensions.High-resolution structural characterization,first-principle calculations,and piezo force microscopy reveal that Mo monoatomic doping enhances the lattice asymmetry,thereby improving the piezoelectric properties.The resulting piezoelectric polarization and the generated built-in electric field significantly improve charge separation efficiency,leading to optimized photocatalytic performance.Additionally,the doping strategy increases the number of active sites and improves the adsorption of intermediate radicals,substantially boosting photo-sterilization efficiency.Our results demonstrate the elimination of 99.95% of Escherichia coli and 100.00% of Staphylococcus aureus within 30 min.Furthermore,we developed a self-purification system simulating water drainage,utilizing low-frequency water streams to trigger the piezoelectric behavior of MR QDs,achieving piezoelectric synergistic photodegradation.This innovative approach provides a more environmentally friendly and economical method for water self-purification,paving the way for advanced water treatment technologies.
基金supported by the National Natural Science Foundation of China(Nos.22241304,22225303,22403091,22173100)the Major Program of the National Natural Science Foundation of China(Nos.42494850 and 42494853)+5 种基金the National Natural Science Foundation of China(NSFC Center for Chemical Dynamics(No.22288201))the Strategic Priority Research Program of the Chinese Academy of Sciences(Nos.XDB0970000 and XDB0970200)the Innovation Program for Quantum Science and Technology(No.2021ZD0303304)the Liaoning Revitalization Talents Program(No.XLYC2402046)the Shenzhen Science and Technology Program(No.ZDSYS20200421111001787)Zhenxing Li thanks the Guangdong Science and Technology Program(No.2025A1515012671)。
文摘We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond fission is the dominant fragmentation pathway at these wavelengths,yielding SD fragments in both the ground(X)and excited(A)electronic states.Most S(^(1)D)atoms arising via 21A′21A′the rival S atom elimination channel when exciting at~139.1 nm are formed with D_(2)partners,in a wide range of rovibrational levels.The partially resolved structure in the total translational energy distributions,P(ET),derived from the S(^(1)D)atom images,implies two dynamical routes into S(^(1)D)+D_(2)products following non-adiabatic coupling from the photo-excited Rydberg state to the dissociative potential energy surface(PES).Similar D_(2)products are evident in the P(ET)spectra derived from analysis of S(^(1)D)images from D_(2)S photolysis at~129.1 nm,but their contribution is overshadowed by a feature attributable to three-body dissociation to S(^(1)D)+2D fragments.These atomic products are deemed to arise via a natural extension of the dynamics responsible for the previously observed highly rotationally excited SD(A)fragments arising via the rival S–D bond fission pathway:asymmetric bond extension together with a dramatic opening of the interbond angle driven by torques generated after coupling to the highly anisotropic 2^(1)A′PES,leading to a centripetally-driven break-up.
基金supported by the National Key Research and Development Program of China(No.2022YFC2804800 to W.J.)the National Natural Science Foundation of China(No.22494704.,22137002 to Y.D.,92253305 to W.J.and 31971111 to C.L.)+6 种基金the Science and Technology Commission of Shanghai Municipality(Grant 20JC1410900 to Y.D.)the University Innovation Research Group in Chongqing(No.CXQT21016 to Y.D.)the Chongqing Talent Program Project(No.CQYC20200302119 to Y.D.)High-Level Innovation Platform Cultivation Plan of Chongqing(to Y.D.)Joint Fund of the Natural Science Innovation and Development Foundation of Chongqing(to Y.D.)Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning(to W.J.)Chongqing Doctoral Express Entry Project(No.CSTB2022BSXM-JCX0044 to J.H.).
文摘Natural products play a crucial role in new drug development,but their druggability is often limited by uncertain molecular targets and insufficient research on mechanisms of action.In this study,we developed a new RPL19-TRAP^(KI)-seq method,combining CRISPR/Cas9 and TRAP technologies,to investigate these mechanisms.We identified and validated seven ribosomal large subunit surface proteins suitable for TRAP,selecting RPL19 for its high enrichment.We successfully established a stable cell line expressing EGFP-RPL19 using CRISPR knock-in and verified its efficiency and specificity in enriching ribosomes and translating mRNA.Integrated with next-generation sequencing,this method allows precise detection of translating mRNA.We validated RPL19-TRAP^(KI)-seq by investigating rapamycin,an mTOR inhibitor,yielding results consistent with previous reports.This optimized TRAP technology provides an accurate representation of translating mRNA,closely reflecting protein expression levels.Furthermore,we investigated SBF-1,a 23-oxa-analog of natural saponin OSW-1 with significant anti-tumor activity but an unclear mechanism.Using RPL19-TRAP^(KI)-seq,we found that SBF-1 exerts its cytotoxic effects on tumor cells by disturbing cellular oxidative phosphorylation.In conclusion,our method has been proven to be a promising tool that can reveal the mechanisms of small molecules with greater accuracy,setting the stage for future exploration of small molecules and advancing the fields of pharmacology and therapeutic development.
基金The National Basic Research Program (973) of China (No. 2006CB403300, 2002CB42308) and the Key Project of KnowledgeInnovation Programme of CAS (No. KZCX1-SW-12)
文摘Understanding phosphorus sorption phenomena in different wetland sediments is important in controlling the P output in headstream watersheds. The pond chain structure （PCS） is widespread in the headstream agricultural watersheds in the southeast of China. Phosphorus sorption characteristics were determined for pond surface sediments （0-12 cm） along a pond chain structure in Liuchahe watershed of Chaohu Lake. Results showed that P sorption capacities （expressed by P sorption index （PSI）） varied both with the landscape position of the ponds and sediment depth. From foothill ponds to riverside ponds the P sorption capacities indicated a significant gradient variability. The higher elevation ponds showed greater sorption capacities, and with the pond elevation decline, P sorption capacities gradually decreased. Some physico-chemical properties, such as pH, oxalate-extractable Fe （Feox）, organic matter （TOC） and Mehlich l-extractable Ca, Mg of pond sediments also indicated significant gradient variability from high elevation ponds to low elevation ponds. Feox was the sediment parameters most highly positively correlated with PSI and was the key factor in controlling P sorption capacity in the pond chain structure （r=0.92, p〈0.001）. Long-term hydrologic and sediment inputs can affect the distribution of sediment constituents and further affect the P sorption capacity. Making the best of the spatial difference of sorption capacities of ponds in watersheds to control nonpoint source P pollutant is necessary.
基金This work was financially supported by the National Science Foundation of China (Project No.20533010).
文摘A reversible storage-release process switched by a temperature difference of 10 ℃ around room temperature can be realized. This fast, recyclable, energy efficient, low cost and green system within a wide range of temperature and pressure is reported here for the first time. The system is believed to open up a new route for the storage and homogeneous utilization of methane.
文摘Owing to the high viscosity of sodium silicate solution, fly ash geopolymer has the problems of low workability and rapid setting time. Therefore, the effect of chemical admixtures on the properties of fly ash geopolymer was studied to overcome the rapid set of the geo-polymer in this paper. High-calcium fly ash and alkaline solution were used as starting materials to synthesize the geopolymer. Calcium chloride, calcium sulfate, sodium sulfate, and sucrose at dosages of 1wt% and 2wt% of fly ash were selected as admixtures based on concrete knowledge to improve the properties of the geopolymer. The setting time, compressive strength, and degree of reaction were recorded, and the microstructure was examined. The results show that calcium chloride significantly shortens both the initial and final setting times of the geopolymer paste. In addition, sucrose also delays the final setting time significantly. The degrees of reaction of fly ash in the geopolymer paste with the admixtures are all higher than those of the control paste. This contributes to the obvious increases in compressive strength.
基金the National Institutes of Health (No.R01DK119202)the Georgia Research Alliance Eminent Scholar endowmentinternal sources at Georgia State University。
文摘Carbon monoxide(CO) as one of the three important endogenously produced signaling molecules, termed as "gasotransmitter," has emerged as a promising therapeutic agent for treating various inflammation and cellular-stress related diseases. In this review, we discussed CO’s evolution from a well-recognized toxic gas to a signaling molecule, and the effort to develop different approaches to deliver it for therapeutic application. We also summarize recently reported chemistry towards different CO delivery forms.
