1 Introduction Magnesium salts are very important by-product of salt lake industry in West China.Nearly 200 million cubic meters of waste brine are released to the environment
Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These cata...Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction(ORR)due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be achieved.This agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these catalysts.However,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ORR.Therefore,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin states.Additionally,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR activity.We have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.展开更多
Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient cat...Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.展开更多
The Ru-based catalysts with different preparation methods or supports were achieved and applied in efficientlycatalytic elimination of 1,2-dichloroethane(1,2-DCE).It wasfirstly found that the redox ability and chlorine...The Ru-based catalysts with different preparation methods or supports were achieved and applied in efficientlycatalytic elimination of 1,2-dichloroethane(1,2-DCE).It wasfirstly found that the redox ability and chlorine re-sistance of the catalyst could be improved by regulating the interaction between Ru and supports.Compared withother supports and conventionally impregnated methods,the Ru@ZSM-5 catalyst synthesized by the in-situ en-capsulation strategy exhibited an excellent low-temperature catalytic performance(T50=262°C,T90=327℃),superior stability in long-term test as well as ideal target products.The acidity,specific surface area,and in-teraction with precious metals of the supports have significant influences on the catalytic activity,and the Ruclusters inside the pore structures are more closely bound to the framework Al species,which promotes theoxidation behavior.The encapsulation strategy also significantly improves the Ru dispersion thereby facilitatesoxygen activation as well as Cl-containing volatile organic compounds(CVOCs)deep oxidation,and preserveslarge amounts of Brønsted acid sites to optimize the hydrolysis mechanism for purification of CVOCs.Subse-quently,the synergistic effect between metal redox and acidity is greatly optimized,thus extremely promotingthe catalytic efficiency of 1,2-DCE oxidation.展开更多
Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capabi...Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay.Herein,a three-dimensional polyaniline is wrapped by carboxylcarbon nanotubes(denoted as C-PANI)which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling,thereby improving Zn-I_(2) batteries.Specifically,carboxyl-carbon nanotubes serve as a proton reservoir for more protonated-NH+=sites in PANI chains,achieving a direct I0/I−reaction for suppressed polyiodide generation and Zn corrosion.Attributing to this“proton-iodine”regulation,catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible-N=/-NH^(+)-reaction.Therefore,the electrolytic Zn-I_(2) battery with C-PANI cathode exhibits an impressive capacity of 420 mAh g^(−1) and ultra-long lifespan over 40,000 cycles.Additionally,a 60 mAh pouch cell was assembled with excellent cycling stability after 100 cycles,providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.展开更多
Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br...Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br-) was investigated with a spontaneous adsorption process,which realized a great improvement of supercapacitor performances by adjusting the coordination geometry.Experiments coupled with theoretical calculations demonstrated that the change of Fe-O bond length and structural distortion of β-FeOOH,which is rooted in halogen ions embedment,led to the relatively narrow band gap.Because of the strong electronegativity of X-,the Fe element in β-FeOOH(X)s presented the unexpected high valence state(3+δ),which is facilitating to adsorb S032-species.Consequently,the designed β-FeOOH(X)s exhibited the good electric conductivity and enhanced the contact between electrode and electrolyte.When used as a negative electrode,the β-FeOOH(F) showed the excellent specific capacity of 391.9 F g-1 at 1 A g-1 current density,almost tenfold improvement compared with initial β-FeOOH,with the superior rate capacity and cyclic stability.This combinational design principle of electronic structure and electrochemical performances provides a promising way to develop advanced electrode materials for supercapacitor.展开更多
Defect engineering,especially oxygen vacancies(O-vacancies) introduction into metal oxide materials has been proved to be an effective strategy to manipulate their surface electron exchange processes.However,quantitat...Defect engineering,especially oxygen vacancies(O-vacancies) introduction into metal oxide materials has been proved to be an effective strategy to manipulate their surface electron exchange processes.However,quantitative investigation of O-vacancies on CO2 electroreduction still remains rather ambiguous.Herein,a series of nanoporous tin oxide(SnOx) materials have been prepared by thermal treatment at various temperatures and reaction conditions.The annealing temperature dependent Ovacancies property of the SnOx was revealed and attributed to the balance tunning of the desorption of oxygen species and the continous oxidation of SnOx.The as-prepared nanoporous SnOx with 300℃treatment was found to be highest O-vacant material and showed an impressive CO2 RR activity and selectivity towards the conversion of CO2 into formic acid(up to 88.6%),and superior HCOOH incomplete current density to other samples.The ideal performance of the O-vacancies rich SnOx-300 material can be ascribed to the high delocalized electron density inducing much enhanced adsorption of CO2 with O binding and benefiting the subsequent reduction with high selectively forming of formic acid.展开更多
This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates...This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates was experimentally optimized,and the corresponding emission behaviors were systematically investigated.The substrates were successfully used to enhance the ultraviolet B(UVB) emission of a low-power light source(e.g.,an 8 W lamp),whose UVB emission intensity was increased by approximately 11 times.By virtue of the novel light source,the productivity of a single set of photochemical microreactor with a 12-meter-long channel(0.6 mm i.d.) was increased to 1.83 kg·a^(-1),which was 42% higher than that of a 100 W lamp,and no cooling devices were used.The method is simple and has great potential to replace traditional medium-pressure mercury lamps for UVB-irradiated photochemical reactions.展开更多
With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy stor...With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy storage device.However,the limitations suffered by AZIBs,including volume expansion and active materials dissolution of the cathode,electrochemical corrosion,irreversible side reactions,zinc dendrites of the anode,have seriously decelerated the civilianization process of AZIBs.Currently,polymers have tremendous superiority for application in AZIBs attributed to their exceptional chemical stability,tunable structure,high energy density and outstanding mechanical properties.Considering the expanding applications of AZIBs and the superiority of polymers,this comprehensive paper meticulously reviews the benefits of utilizing polymeric applied to cathodes and anodes,respectively.To begin with,with adjustable structure as an entry point,the correlation between polymer structure and the function of energy storage as well as optimization is deeply investigated in respect to the mechanism.Then,depending on the diversity of properties and structures,the development of polymers in AZIBs is summarized,including conductive polymers,redox polymers as well as carbon composite polymers for cathode and polyvinylidene fluoride-,carbonyl-,amino-,nitrile-based polymers for anode,and a comprehensive evaluation of the shortcomings of these strategies is provided.Finally,an outlook highlights some of the challenges posed by the application of polymers and offers insights into the potential future direction of polymers in AZIBs.It is designed to provide a thorough reference for researchers and developers working on polymer for AZIBs.展开更多
Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utiliza...Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.展开更多
Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical...Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical reaction of CaC_(2) and a carbonate(CaCO_(3),Na2CO_(3),or NaHCO_(3))at ambient temperature.The resultant OACMs are micro mesoporous carbon nanomaterials with high specific area(>648 m2 g^(-1)),highly crosslinked texture,and rich alkynyl and oxygenated groups.The OACMs exhibit excellent Hg(Ⅱ)adsorption due to the soft acid-soft base interaction between alkynyl and Hg(Ⅱ),and OACM-3 derived from CaC_(2) and NaHCO_(3) has the saturated Hg(Ⅱ)adsorbance of 483.9 mg g^(-1)along with good selectivity and recyclability.The adsorption is mainly chemisorption following the Langmuir mode.OACM-3 also shows high adsorbance for other heavy metal ions,e.g.256.6 mg g^(-1)for Pb(II),232.4 mg g^(-1)for Zn(II),and 198.7 mg g^(-1)for Cu(II).This work expands the mechnochemical reaction of CaC_(2)with carbonates and possibly other oxyanionic salts,provides a new synthesis approach for functional alkynyl carbon materials with excellent adsorption performance for heavy metal ions,as well as a feasible approach for CO2 resource utilization.展开更多
Latex wastewater is a kind of refractory organic wastewater containing high concentrations of organics and ammonia nitrogen.In this work,the combined process of forward osmosis(FO)and reverse osmosis(RO)was designed t...Latex wastewater is a kind of refractory organic wastewater containing high concentrations of organics and ammonia nitrogen.In this work,the combined process of forward osmosis(FO)and reverse osmosis(RO)was designed to treat the latex wastewater in the whole process,achieving the water recovery rate of 99%and basically no waste discharge after the catalytic oxidation process.The turbidity of the latex wastewater was decreased to below 1 NTU by microfiltration pretreatment,and then using MgCl_2 worked as the draw solution for FO process to treat the latex wastewater.Different operation conditions including adding acid or scale inhibitor as the pretreatment methods were conducted to improve the treatment performance of the combined process.After the treatment of the whole process,the concentration of COD was less than 20 mg·L^(-1),the concentration of NH_3-N was less than 10 mg·L^(-1),and the concentration of TP was less than 0.5 mg·L^(-1)for the treated latex wastewater.The water quality met standards of industrial water reuse after the complete analysis of the treated latex wastewater,meanwhile,useful substances of L-Quebrachitol(L-Q)were successfully extracted from the concentrated solution.Therefore,the combined process of FO and RO could realize the efficient treatment and reuse of latex wastewater,which provided with some important guidance on the industrial application.展开更多
Pressure-related sensing materials in mechanochromic luminescent materials have received wide attention.However,at present,most piezochromic luminescence(PCL)materials have problems such as aggregation-caused quenchin...Pressure-related sensing materials in mechanochromic luminescent materials have received wide attention.However,at present,most piezochromic luminescence(PCL)materials have problems such as aggregation-caused quenching(ACQ)effect due to the presence of powder form,complicated preparation methods and fluorescence quenching effect under high pressure.To solve these problems,we employ three components containing carbon dots(CDs),layered double hydroxides(LDHs)and polyvinyl alcohol(PVA)to construct the CDs-LDHs/PVA film.The LDHs can provide a rigid environment for CDs and improve the luminescent efficiency of CDs.The film shows high sensitivity,stability and reversibility.Moreover,the compressed film can recover to its original state by heating.Therefore,the PCL film with dual emission(fluorescence and phosphorescence)characteristic is constructed,which boosts the sensitivity of pressure-sensing.展开更多
Objective： Scandix pecten-veneris L. is a less studied wild edible herb and is considered an extinct plant species in many parts of the world. This study was designed to evaluate its phytochemical composition and bio...Objective： Scandix pecten-veneris L. is a less studied wild edible herb and is considered an extinct plant species in many parts of the world. This study was designed to evaluate its phytochemical composition and biological potential of S. pecten-veneris L. Methods： Phytochemicals including alkaloids, fiavonoids, polyphenols, and tannins were determined in extracts of S. pecten-veneris. Antioxidant activity was determined using 2,2-diphenyl-1- picrylhydrazyl （DPPH）, while reducing power was tested by ferric reducing/antioxidant power （FRAP） assay. Antimi- crobial activity against seven bacterial and four fungal strains was evaluated using agar well diffusion assay. Enzymes inhibition study was performed for urease, phosphodiesterase-I, and catalase-II. Results： S. pecten-veneris showed moderate antiradical activity and reducing potential of hydroxyl radicals to about 20% of the initial value. The antiox- idant activity of various extracts of S. pecten-veneris showed a linear correlation with total phenolic contents in the order of water〉n-butanol〉chloroform〉ethyl acetate〉methanol extracts. S. pecten-veneris leaves showed the highest inhibitory activity against Staphylococcus aureus while the highest antifungal activity was observed against Candida albicans. The plant extract was most potent against urease enzymes but showed moderate activity against phosphodiestrase-I and carbonic anhydrase-II. Conclusions： Our data demonstrate that in addition to its culinary uses, S. pecten-veneris has good medicinal potential and hence could be used for treating some specific health ailments.展开更多
Biomass-derived hard carbon is becoming promising anodes for potassium-ion batteries(PIBs)thanks to their resource abundance.Yet,it is a big challenge to improve the charge carrier kinetics of the disordered carbon la...Biomass-derived hard carbon is becoming promising anodes for potassium-ion batteries(PIBs)thanks to their resource abundance.Yet,it is a big challenge to improve the charge carrier kinetics of the disordered carbon lattice in hard carbon.Herein,confined pitch-based soft carbon in pollen-derived hard carbon(PSC/PHC)is synthesized by vapor deposition strategy as anodes for PIBs.The ordered pitch-based soft carbon compensates for the short-range electron conduction in hard carbon to enhance the charge transfer kinetics,and the externally disordered pollen-derived hard carbon alleviates the volume change of soft carbon during cycling.Benefiting from the synergistic effect of soft and hard carbon,as well as the reinforced structure of order-in-disordered carbon,the PSC/PHC obtained with deposition time of 0.5 h(PSC/PHC-0.5)displays an excellent rate capability(148.7 mAh g^(-1)at 10 A g^(-1))and superb cycling stability(70%retention over 2000 cycles at 1 A g^(-1)).This work offers a unique insight in tuning the microcrystalline structure of soft-hard carbon anode for advanced PIBs.展开更多
Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films wi...Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr_(3) /poly[bis(phenoxy phosphazene)](PBPP) delivered better air and light stability, and CsPbBr_(3) /poly[bis(4-esterphenoxy)phosphazene](PBEPP) exhibited superior water and heat resistance. CsPbBr_(3) /PBEPP showed a greater increase in fiuorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature(150℃). These findings thus provide new insight into fiexible luminescent CsPbBr_(3) films with high stability in optoelectronic applications.展开更多
The demand for high-energy-density sodium-ion batteries has driven research to increase the hard carbon(HC)plateau capacity(<0.1 V),but the plateau capacity-rate capability trade-off limits performance.We report a ...The demand for high-energy-density sodium-ion batteries has driven research to increase the hard carbon(HC)plateau capacity(<0.1 V),but the plateau capacity-rate capability trade-off limits performance.We report a way to regulate the closed pore structure and improve the rate capability of HC by the addition of graphene oxide using an emulsification process.In a non-emulsion system,graphene oxide not only shortens ion diffusion paths by inducing the formation of flakelike HC but also significantly improves the rate performance by serving as conductive bridges within the carbon matrix.The prepared graphene/phenolic resin carbon composite has reversible capacities of 362,340,319,274,119,86,69 and 48 mAh g^(−1)at current densities of 0.02,0.05,0.1,0.2,0.5,1,2 and 5 A g^(−1),respectively.When emulsification is introduced,the graphene oxide acts as a nano-confinement template,guiding the cross-linking of phenolic resin to form uniformly sized closed pores.This composite electrode material has the highest plateau capacity of 268 mAh g^(−1)at 20 mA g^(−1).展开更多
In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and...In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and exceptional properties.Graphene oxide(GO),a two-dimensional material with an extremely high specific surface area and excellent conductivity,offers new possibilities for enhancing the electrochemical performance of metal oxides.In this work,we synthesized met-al-organic framework(MOF)and GO composites by regulating the amount of GO,and successfully prepared composites of metal oxides supported by nitrogen-doped carbon frameworks and GO through a simple one-step calcination process.Based on the electrochemical tests,the optimal amount of GO was determined.This research will provide new insights into and directions for designing and synthesizing metal oxide and graphene oxide composite materials with an ideal electro-chemical performance.展开更多
Nervonic acid(NA) is a long-chain monounsaturated fatty acid with significant potential for neural fiber repair.In this study,a mixed fatty acid methyl ester was synthesized as the raw material through saponification ...Nervonic acid(NA) is a long-chain monounsaturated fatty acid with significant potential for neural fiber repair.In this study,a mixed fatty acid methyl ester was synthesized as the raw material through saponification of Acer truncatum Bunge seed oil.Based on the differences in boiling points and relative volatilities of various components,a four-stage vacuum batch distillation process was employed to enrich the nervonic acid methyl ester(NAME).The effect of distillation process parameters on enrichment efficiency was investigated,including distillation temperature,operating pressure,and reflux ratio.The purity of NAME achieved as 91.20% under optimal conditions and the corresponding yield was 48.91%.To further increase the purity,a low-temperature crystallization process was adopted and a final purity of NAME was obtained as 97.56%.Simulation of the above four-stage batch distillation was conducted using Aspen Plus software,and a continuous distillation processes was further simulated to establish a theoretical basis for future industrial-scale production.The results of experiments and simulation demonstrate that the integrated process of vacuum distillation and low-temperature crystallization exhibits remarkable separation performances,providing robust guidance for the production of high-purity NA.展开更多
基金supported by the National Natural Science Foundationthe National Key Technologies R&D Program (2011BAE28B01)the 863 Program (2013AA032501)
文摘1 Introduction Magnesium salts are very important by-product of salt lake industry in West China.Nearly 200 million cubic meters of waste brine are released to the environment
基金supported by the Research Fund for International Scientists(RFIS-Grant numbers:52150410410)National Natural Science Foundation of Chinathe Deanship of Scientific Research and Graduate Studies at King Khalid University for funding this research work through Large Research Project under the grant number RGP2/121/1445.
文摘Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction(ORR)due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be achieved.This agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these catalysts.However,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ORR.Therefore,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin states.Additionally,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR activity.We have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.
基金National Natural Science Foundation of China,Grant/Award Number:22179029Fundamental Research Funds for the Central Universities,Grant/Award Number:buctrc202324+2 种基金Young Elite Scientists Sponsorship Program by BAST,Grant/Award Number:BYESS2023093Ministero dell'Istruzione,dell'Universitàe della Ricerca,Grant/Award Number:2022FNL89YKempestiftelserna。
文摘Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.
基金supported by the National Key Research and Development Program of China(No.2023YFC3905400)the National Natural Science Foundation of China(No.22176010).
文摘The Ru-based catalysts with different preparation methods or supports were achieved and applied in efficientlycatalytic elimination of 1,2-dichloroethane(1,2-DCE).It wasfirstly found that the redox ability and chlorine re-sistance of the catalyst could be improved by regulating the interaction between Ru and supports.Compared withother supports and conventionally impregnated methods,the Ru@ZSM-5 catalyst synthesized by the in-situ en-capsulation strategy exhibited an excellent low-temperature catalytic performance(T50=262°C,T90=327℃),superior stability in long-term test as well as ideal target products.The acidity,specific surface area,and in-teraction with precious metals of the supports have significant influences on the catalytic activity,and the Ruclusters inside the pore structures are more closely bound to the framework Al species,which promotes theoxidation behavior.The encapsulation strategy also significantly improves the Ru dispersion thereby facilitatesoxygen activation as well as Cl-containing volatile organic compounds(CVOCs)deep oxidation,and preserveslarge amounts of Brønsted acid sites to optimize the hydrolysis mechanism for purification of CVOCs.Subse-quently,the synergistic effect between metal redox and acidity is greatly optimized,thus extremely promotingthe catalytic efficiency of 1,2-DCE oxidation.
基金supported by the National Natural Science Foundation of China(22209006,21935001)the Natural Science Foundation of Shandong Province(ZR2022QE009)+1 种基金Fundamental Research Funds for the Central Universities(buctrc202307)the Beijing Natural Science Foundation(Z210016).
文摘Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay.Herein,a three-dimensional polyaniline is wrapped by carboxylcarbon nanotubes(denoted as C-PANI)which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling,thereby improving Zn-I_(2) batteries.Specifically,carboxyl-carbon nanotubes serve as a proton reservoir for more protonated-NH+=sites in PANI chains,achieving a direct I0/I−reaction for suppressed polyiodide generation and Zn corrosion.Attributing to this“proton-iodine”regulation,catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible-N=/-NH^(+)-reaction.Therefore,the electrolytic Zn-I_(2) battery with C-PANI cathode exhibits an impressive capacity of 420 mAh g^(−1) and ultra-long lifespan over 40,000 cycles.Additionally,a 60 mAh pouch cell was assembled with excellent cycling stability after 100 cycles,providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.
基金supported by the National Natural Science Foundation of China(Nos.2177060378,21627813,and 21521005)the Program for Changjiang Scholars,Innovative Research Teams in Universities(No.IRT1205)the Fundamental Research Funds for the Central Universities(Nos.12060093063 and XK1803-05).
文摘Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br-) was investigated with a spontaneous adsorption process,which realized a great improvement of supercapacitor performances by adjusting the coordination geometry.Experiments coupled with theoretical calculations demonstrated that the change of Fe-O bond length and structural distortion of β-FeOOH,which is rooted in halogen ions embedment,led to the relatively narrow band gap.Because of the strong electronegativity of X-,the Fe element in β-FeOOH(X)s presented the unexpected high valence state(3+δ),which is facilitating to adsorb S032-species.Consequently,the designed β-FeOOH(X)s exhibited the good electric conductivity and enhanced the contact between electrode and electrolyte.When used as a negative electrode,the β-FeOOH(F) showed the excellent specific capacity of 391.9 F g-1 at 1 A g-1 current density,almost tenfold improvement compared with initial β-FeOOH,with the superior rate capacity and cyclic stability.This combinational design principle of electronic structure and electrochemical performances provides a promising way to develop advanced electrode materials for supercapacitor.
基金supported by the National Natural Science Foundation of China,National Key Research and Development Project (No.2016YFF0204402)the Program for Changjiang Scholars and Innovative Research Team in the University+1 种基金the Fundamental Research Funds for the Central Universitiesthe longterm subsidy mechanism from the Ministry of Finance and the Ministry of Education of PRC
文摘Defect engineering,especially oxygen vacancies(O-vacancies) introduction into metal oxide materials has been proved to be an effective strategy to manipulate their surface electron exchange processes.However,quantitative investigation of O-vacancies on CO2 electroreduction still remains rather ambiguous.Herein,a series of nanoporous tin oxide(SnOx) materials have been prepared by thermal treatment at various temperatures and reaction conditions.The annealing temperature dependent Ovacancies property of the SnOx was revealed and attributed to the balance tunning of the desorption of oxygen species and the continous oxidation of SnOx.The as-prepared nanoporous SnOx with 300℃treatment was found to be highest O-vacant material and showed an impressive CO2 RR activity and selectivity towards the conversion of CO2 into formic acid(up to 88.6%),and superior HCOOH incomplete current density to other samples.The ideal performance of the O-vacancies rich SnOx-300 material can be ascribed to the high delocalized electron density inducing much enhanced adsorption of CO2 with O binding and benefiting the subsequent reduction with high selectively forming of formic acid.
基金the National Natural Science Foundation of China (21978008, 21606008)the State Key Laboratory of Chemical Engineering (SKL-ChE-17A02)the Fundamental Research Funds for the Central Universities (JD2017)。
文摘This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates was experimentally optimized,and the corresponding emission behaviors were systematically investigated.The substrates were successfully used to enhance the ultraviolet B(UVB) emission of a low-power light source(e.g.,an 8 W lamp),whose UVB emission intensity was increased by approximately 11 times.By virtue of the novel light source,the productivity of a single set of photochemical microreactor with a 12-meter-long channel(0.6 mm i.d.) was increased to 1.83 kg·a^(-1),which was 42% higher than that of a 100 W lamp,and no cooling devices were used.The method is simple and has great potential to replace traditional medium-pressure mercury lamps for UVB-irradiated photochemical reactions.
基金financially supported by the National Natural Science Foundation of China(51872090,51772097,22304055)the Hebei Natural Science Fund for Distinguished Young Scholar(E2019209433)+4 种基金the Youth Talent Program of Hebei Provincial Education Department(BJ2018020)the Natural Science Foundation of Hebei Province(E2020209151,E2022209158,B2022209026,D2023209012)the Central Guiding Local Science and Technology Development Fund Project(236Z4409G)the Science and Technology Project of Hebei Education Department(SLRC2019028)the Science and Technology Planning Project of Tangshan City(22130227H)。
文摘With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy storage device.However,the limitations suffered by AZIBs,including volume expansion and active materials dissolution of the cathode,electrochemical corrosion,irreversible side reactions,zinc dendrites of the anode,have seriously decelerated the civilianization process of AZIBs.Currently,polymers have tremendous superiority for application in AZIBs attributed to their exceptional chemical stability,tunable structure,high energy density and outstanding mechanical properties.Considering the expanding applications of AZIBs and the superiority of polymers,this comprehensive paper meticulously reviews the benefits of utilizing polymeric applied to cathodes and anodes,respectively.To begin with,with adjustable structure as an entry point,the correlation between polymer structure and the function of energy storage as well as optimization is deeply investigated in respect to the mechanism.Then,depending on the diversity of properties and structures,the development of polymers in AZIBs is summarized,including conductive polymers,redox polymers as well as carbon composite polymers for cathode and polyvinylidene fluoride-,carbonyl-,amino-,nitrile-based polymers for anode,and a comprehensive evaluation of the shortcomings of these strategies is provided.Finally,an outlook highlights some of the challenges posed by the application of polymers and offers insights into the potential future direction of polymers in AZIBs.It is designed to provide a thorough reference for researchers and developers working on polymer for AZIBs.
基金financially supported by the National Key Research and Development Program of China (2018YFA0702002)the Beijing Natural Science Foundation (Z210016)the National Natural Science Foundation of China (21935001)。
文摘Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.
基金supports from the National Natural Science Foundation of China(No.21776015)the University Scientific Research Project of Anhui Province(No.KJ2018A0065&KJ2020A0245).
文摘Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical reaction of CaC_(2) and a carbonate(CaCO_(3),Na2CO_(3),or NaHCO_(3))at ambient temperature.The resultant OACMs are micro mesoporous carbon nanomaterials with high specific area(>648 m2 g^(-1)),highly crosslinked texture,and rich alkynyl and oxygenated groups.The OACMs exhibit excellent Hg(Ⅱ)adsorption due to the soft acid-soft base interaction between alkynyl and Hg(Ⅱ),and OACM-3 derived from CaC_(2) and NaHCO_(3) has the saturated Hg(Ⅱ)adsorbance of 483.9 mg g^(-1)along with good selectivity and recyclability.The adsorption is mainly chemisorption following the Langmuir mode.OACM-3 also shows high adsorbance for other heavy metal ions,e.g.256.6 mg g^(-1)for Pb(II),232.4 mg g^(-1)for Zn(II),and 198.7 mg g^(-1)for Cu(II).This work expands the mechnochemical reaction of CaC_(2)with carbonates and possibly other oxyanionic salts,provides a new synthesis approach for functional alkynyl carbon materials with excellent adsorption performance for heavy metal ions,as well as a feasible approach for CO2 resource utilization.
基金supported by the National Natural Science Foundation of China (22125802 and 22108012)Natural Science Foundation of Beijing Municipality (2222017)Fundamental Research Funds for the Central Universities (BUCTRC-202109)。
文摘Latex wastewater is a kind of refractory organic wastewater containing high concentrations of organics and ammonia nitrogen.In this work,the combined process of forward osmosis(FO)and reverse osmosis(RO)was designed to treat the latex wastewater in the whole process,achieving the water recovery rate of 99%and basically no waste discharge after the catalytic oxidation process.The turbidity of the latex wastewater was decreased to below 1 NTU by microfiltration pretreatment,and then using MgCl_2 worked as the draw solution for FO process to treat the latex wastewater.Different operation conditions including adding acid or scale inhibitor as the pretreatment methods were conducted to improve the treatment performance of the combined process.After the treatment of the whole process,the concentration of COD was less than 20 mg·L^(-1),the concentration of NH_3-N was less than 10 mg·L^(-1),and the concentration of TP was less than 0.5 mg·L^(-1)for the treated latex wastewater.The water quality met standards of industrial water reuse after the complete analysis of the treated latex wastewater,meanwhile,useful substances of L-Quebrachitol(L-Q)were successfully extracted from the concentrated solution.Therefore,the combined process of FO and RO could realize the efficient treatment and reuse of latex wastewater,which provided with some important guidance on the industrial application.
基金supported by the National Key R&D Program of China(No.2019YFC1906100)the National Natural Science Foundation of China(Nos.21571014 and 21521005)+2 种基金the Beijing Municipal Natural Science Foundation(No.2172044)the Open Research Fund Program of Key Laboratory of Cosmetic,China National Light Industry,Beijing Technology and Business University(No.KLC-2019-ZD1)the Fundamental Research Funds for the Central Universities(No.12060093063)。
文摘Pressure-related sensing materials in mechanochromic luminescent materials have received wide attention.However,at present,most piezochromic luminescence(PCL)materials have problems such as aggregation-caused quenching(ACQ)effect due to the presence of powder form,complicated preparation methods and fluorescence quenching effect under high pressure.To solve these problems,we employ three components containing carbon dots(CDs),layered double hydroxides(LDHs)and polyvinyl alcohol(PVA)to construct the CDs-LDHs/PVA film.The LDHs can provide a rigid environment for CDs and improve the luminescent efficiency of CDs.The film shows high sensitivity,stability and reversibility.Moreover,the compressed film can recover to its original state by heating.Therefore,the PCL film with dual emission(fluorescence and phosphorescence)characteristic is constructed,which boosts the sensitivity of pressure-sensing.
基金Project supported by the Directorate of Science and Technology(DoST),Khyber Pakhtunkhwa,Pakistan,under Research Project Developmental Scheme(Bio-Tech Sector,Phase-1,A03959 Bio-Tech)
文摘Objective： Scandix pecten-veneris L. is a less studied wild edible herb and is considered an extinct plant species in many parts of the world. This study was designed to evaluate its phytochemical composition and biological potential of S. pecten-veneris L. Methods： Phytochemicals including alkaloids, fiavonoids, polyphenols, and tannins were determined in extracts of S. pecten-veneris. Antioxidant activity was determined using 2,2-diphenyl-1- picrylhydrazyl （DPPH）, while reducing power was tested by ferric reducing/antioxidant power （FRAP） assay. Antimi- crobial activity against seven bacterial and four fungal strains was evaluated using agar well diffusion assay. Enzymes inhibition study was performed for urease, phosphodiesterase-I, and catalase-II. Results： S. pecten-veneris showed moderate antiradical activity and reducing potential of hydroxyl radicals to about 20% of the initial value. The antiox- idant activity of various extracts of S. pecten-veneris showed a linear correlation with total phenolic contents in the order of water〉n-butanol〉chloroform〉ethyl acetate〉methanol extracts. S. pecten-veneris leaves showed the highest inhibitory activity against Staphylococcus aureus while the highest antifungal activity was observed against Candida albicans. The plant extract was most potent against urease enzymes but showed moderate activity against phosphodiestrase-I and carbonic anhydrase-II. Conclusions： Our data demonstrate that in addition to its culinary uses, S. pecten-veneris has good medicinal potential and hence could be used for treating some specific health ailments.
基金partly supported by the National Natural Science Foundation of China(52072002,52372037,and 22108003)the Postdoctoral Fellowship Program of CPSF(GZC20230015)+2 种基金the Outstanding Scientific Research and Innovation Team Program of Higher Education Institutions of Anhui Province(2023AH010015)the Excellent Young Talents Fund Program of Higher Education Institutions of Anhui Province(2023AH030026)financial support from the Anhui International Research Center of Energy Materials Green Manufacturing and Biotechnology。
文摘Biomass-derived hard carbon is becoming promising anodes for potassium-ion batteries(PIBs)thanks to their resource abundance.Yet,it is a big challenge to improve the charge carrier kinetics of the disordered carbon lattice in hard carbon.Herein,confined pitch-based soft carbon in pollen-derived hard carbon(PSC/PHC)is synthesized by vapor deposition strategy as anodes for PIBs.The ordered pitch-based soft carbon compensates for the short-range electron conduction in hard carbon to enhance the charge transfer kinetics,and the externally disordered pollen-derived hard carbon alleviates the volume change of soft carbon during cycling.Benefiting from the synergistic effect of soft and hard carbon,as well as the reinforced structure of order-in-disordered carbon,the PSC/PHC obtained with deposition time of 0.5 h(PSC/PHC-0.5)displays an excellent rate capability(148.7 mAh g^(-1)at 10 A g^(-1))and superb cycling stability(70%retention over 2000 cycles at 1 A g^(-1)).This work offers a unique insight in tuning the microcrystalline structure of soft-hard carbon anode for advanced PIBs.
基金supported by the National Science Foundation (NSF) of China (No. 51773010)the Weifang Science and Technology Development Plan Program (No. 2023GX005)。
文摘Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr_(3) /poly[bis(phenoxy phosphazene)](PBPP) delivered better air and light stability, and CsPbBr_(3) /poly[bis(4-esterphenoxy)phosphazene](PBEPP) exhibited superior water and heat resistance. CsPbBr_(3) /PBEPP showed a greater increase in fiuorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature(150℃). These findings thus provide new insight into fiexible luminescent CsPbBr_(3) films with high stability in optoelectronic applications.
文摘The demand for high-energy-density sodium-ion batteries has driven research to increase the hard carbon(HC)plateau capacity(<0.1 V),but the plateau capacity-rate capability trade-off limits performance.We report a way to regulate the closed pore structure and improve the rate capability of HC by the addition of graphene oxide using an emulsification process.In a non-emulsion system,graphene oxide not only shortens ion diffusion paths by inducing the formation of flakelike HC but also significantly improves the rate performance by serving as conductive bridges within the carbon matrix.The prepared graphene/phenolic resin carbon composite has reversible capacities of 362,340,319,274,119,86,69 and 48 mAh g^(−1)at current densities of 0.02,0.05,0.1,0.2,0.5,1,2 and 5 A g^(−1),respectively.When emulsification is introduced,the graphene oxide acts as a nano-confinement template,guiding the cross-linking of phenolic resin to form uniformly sized closed pores.This composite electrode material has the highest plateau capacity of 268 mAh g^(−1)at 20 mA g^(−1).
基金supported by the National Natural Science Foundation of China(51971157)Shenzhen Science and Technology Program(JCYJ20210324115412035,JCYJ202103-24123202008,JCYJ20210324122803009 and ZDS-YS20210813095534001)Guangdong Foundation for Basic and Applied Basic Research Program(2021A1515110880).
文摘In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and exceptional properties.Graphene oxide(GO),a two-dimensional material with an extremely high specific surface area and excellent conductivity,offers new possibilities for enhancing the electrochemical performance of metal oxides.In this work,we synthesized met-al-organic framework(MOF)and GO composites by regulating the amount of GO,and successfully prepared composites of metal oxides supported by nitrogen-doped carbon frameworks and GO through a simple one-step calcination process.Based on the electrochemical tests,the optimal amount of GO was determined.This research will provide new insights into and directions for designing and synthesizing metal oxide and graphene oxide composite materials with an ideal electro-chemical performance.
基金supported by the National Natural Science Foundation of China(22125802,22108150,22338001)。
文摘Nervonic acid(NA) is a long-chain monounsaturated fatty acid with significant potential for neural fiber repair.In this study,a mixed fatty acid methyl ester was synthesized as the raw material through saponification of Acer truncatum Bunge seed oil.Based on the differences in boiling points and relative volatilities of various components,a four-stage vacuum batch distillation process was employed to enrich the nervonic acid methyl ester(NAME).The effect of distillation process parameters on enrichment efficiency was investigated,including distillation temperature,operating pressure,and reflux ratio.The purity of NAME achieved as 91.20% under optimal conditions and the corresponding yield was 48.91%.To further increase the purity,a low-temperature crystallization process was adopted and a final purity of NAME was obtained as 97.56%.Simulation of the above four-stage batch distillation was conducted using Aspen Plus software,and a continuous distillation processes was further simulated to establish a theoretical basis for future industrial-scale production.The results of experiments and simulation demonstrate that the integrated process of vacuum distillation and low-temperature crystallization exhibits remarkable separation performances,providing robust guidance for the production of high-purity NA.
