Electrocatalysis offers efficient and targeted conversion of monomers derived from waste polyester plastics to chemical products under ambient temperature and pressure conditions.This review provides analysis of resea...Electrocatalysis offers efficient and targeted conversion of monomers derived from waste polyester plastics to chemical products under ambient temperature and pressure conditions.This review provides analysis of research on electrochemical upgrading of monomers derived from waste polyester plastics published from2021 to present.Factors for assessing upgrading of waste polyester plastics include alkaline hydrolysis pretreatment,indices of electrochemical reaction process(activity,stability,and techno-economic a nalysis),separation,and product recovery.Types of depolymerization monomers and their value-added products are summarized along with electrocatalytic mechanisms and reaction pathways.Notably,cathode coupled reactions offer significant value for anodic waste plastic oxidation during electrolysis processes.Development of bifunctional electrocatalysts can reduce the cost of coupled systems and complexity of the electrolyzer.Upgrading and recycling of waste plastic monomers using electrocatalytic technology should undergo downstream processing to form high-value products containing C-N and C-S derived functional groups obtained from depolymerized monomers,Electrochemical conversion and upgrading of monomers derived from waste polyester plastics can contribute to industrialization and global economies and help to realize environmental sustainability.展开更多
Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimet...Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimetallic PdCu/TiO_(x)composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOxnanotube arrays.Denitrification experiments demonstrated that the Pd_(1)Cu_(1)/TiO_(x)catalyst exhibited the highest(NO_(3^(–)))removal rate(81.2%)and N_(2)selectivity(67.2%)among all tested catalysts.Leveraging the exceptional light-responsive property of TiO_(x),the introduction of light energy as an assisting factor in electrocatalysis further augmented the(NO_(3^(–)))treatment rate,resulting in a higher(NO_(3^(–)))removal rate of 95.1%and N_(2)selectivity of approximately 90%.Compared to individual electrocatalysis and photocatalysis systems,the overpotential for the catalytic interface active*H formation in the photo-assisted electrocatalysis system was remarkably reduced,thus accelerating electron migration and promoting(NO_(3^(–)))reduction kinetics.Economic analysis revealed an energy consumption of 2.74 k Wh/mol and a corresponding energy consumption per order(EEO)of 0.79 k Wh/m^(3)for the Pd_(1)Cu_(1)/TiOxcatalyst to reduce 25.2 mg/L of(NO_(3^(–)))-N in water to N_(2),showcasing remarkable competitiveness and economic advantages over other water treatment technologies.This study developed the PdCu/TiOxelectrocatalysts with high(NO_(3^(–)))removal rates and N_(2)selectivity,particularly when combined with light energy,the efficiency and selectivity were significantly enhanced,offering a competitive and economically viable solution for wastewater treatment.展开更多
Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications,yet it remains challenging to do so on the surface of multimetallic nanocrystals.Herein,we presen...Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications,yet it remains challenging to do so on the surface of multimetallic nanocrystals.Herein,we present the multifactorial engineering(size,shape,phase,and composition)of the fully ordered PtBi nanoplates at atomic level,achieving a unique catalyst surface where the face-centered cubic(fcc)Pt edges are modified by the isolated Pd atoms and BiO_(x)adatoms.This Pd_(1)/Pt-BiO_(x)electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg^(-1)Pt+Pd toward ethanol oxidation in alkaline electrolyte and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm^(−2).The surrounding BiO_(x)adatoms are critical for mitigating CO-poisoning on the Pt surface,and the Pd_(1)/Pt single-atom alloy further facilitates the electrooxidation of CH_(3)CH_(2)OH.This work offers new insights into the rational design and construction of sophisticated catalyst surface at single-atomic sites for highly efficient electrocatalysis.展开更多
To enhance the efficiency of green energy harvesting and pollutant degradation,significant efforts are focused on identifying highly effective catalysts.Metal-nitrogen-carbon single-atom catalysts(M-N-C SACs)have emer...To enhance the efficiency of green energy harvesting and pollutant degradation,significant efforts are focused on identifying highly effective catalysts.Metal-nitrogen-carbon single-atom catalysts(M-N-C SACs)have emerged as pivotal in catalysis due to their unique geometric structures,electronic states,and catalytic capabilities.Notably,the incorporation of magnetic elements at the active centers of these single-atom catalysts has garnered attention for their role in efficient electrochemical conversions.The orientation of spin states critically influences the adsorption and formation of reactants and intermediates,making the precise control of spin alignment and magnetic moments essential for reducing energy barriers and overcoming spin-related limitations,thereby enhancing catalytic activity.Thus,understanding the catalytic role of spin and modulating spin density at M-N-C single-atom centers holds profound fundamental and technological significance.In this review,we elucidate the fundamental mechanisms governing spin states and its influence in electrocatalysis.We then discuss various strategies for adjusting the spin states of active centers in the M-N-C SACs and the associated characterization techniques.Finally,we outline challenges and future perspectives of spin regulation for high-performance catalysts.This review provides deep insights into the micro-mechanisms of catalytic phenomena and offers a roadmap for designing spin-regulated catalysts for advanced energy applications.展开更多
Multi-metal porous crystalline materials(MPCM),integrating the functions of both multi-metal centres and porous crystalline materials(e.g.,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)),are an ex...Multi-metal porous crystalline materials(MPCM),integrating the functions of both multi-metal centres and porous crystalline materials(e.g.,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)),are an extended class of porous materials that have attracted much attention for a broad range of applications.Owing to the advantages of these materials,they generally display high porosity,multimetal active sites,well-tuned functions,and pre-designable structures,etc.,serving as desired platforms for the study of structure-property relationships.In view of the clean and sustainable target,a series of MPCM have been explored as electrocatalysts for electrocatalytic reactions like hydrogen evolution reaction,oxygen evolution reaction and electrocatalytic CO_(2)reduction reaction.Concerning the progress achieved for MPCM in electrocatalytic field during past years,this review will provide a brief introduction on the recent breakthrough of MPCM based electrocatalysts including their synthesis methods,structure design,component/morphology tuning,electrocatalytic property and structure-property relationship,etc.Besides,it will also conclude the current challenges and present perspectives for the MPCM based electrocatalysts,which might promote the development of porous crystalline materials in electrocatalysis and hope to provide new insights for scientists in related fields.展开更多
In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in whi...In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in which synchronous hypophosphite ion(H_(2)PO_(2)^(-))oxidation to phosphate ion(PO_(4)^(3–))(POR)and nitrate reduction(NO_(3)RR)to ammonia(NH_(3))occur,followed by cascade chemical precipitation to generate struvite.Herein,a bifunctional Cu_(2)O@NiFe_(2)O_(4)Z-scheme heterojunction with a yolk/shell structure and oxygen vacancies(OVs)was designed and developed to optimize the NO_(3)RR/POR.Serving as a key component,the established PA-EC system consisted of a Janus Cu_(2)O@NiFe_(2)O_(4)/NF self-supporting integrated photocathode and a Cu_(2)O@NiFe_(2)O_(4)/NF photocathode with efficient struvite PA-EC synthesis performance under a low cell voltage of 1.6 V vs NHE.Specifically,Janus Cu_(2)O@NiFe_(2)O_(4)/NF photocathode exhibits superior performance with a high NH3 yield of 38.06 mmol L^(-1)and a faradaic efficiency(FE)of 92.31%at 1.6 V vs.NHE and enables ammonia FE over 60%in a broad NO_(3)–concentration window of 0.005–0.5 mol L^(-1).The photoassisted electrochemical catalytic mechanism and reaction pathway for struvite synthesis on Cu_(2)O@NiFe_(2)O_(4)were investigated through a series of experiments and theoretical calculations.The results demonstrated the critical roles of the interfacial electric field,void confinement,and oxygen vacancies in promoting the overall catalytic efficiency.These encouraging results warrant further studies on combined P and N recovery for efficient production of valuable fertilizers.展开更多
Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant c...Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant challenge for practical application.Recently,twodimensional transition metal dichalcogenides(2D-TMDs)have emerged as attractive and cost-effective alternatives for efficient electrocatalysis in the HER.Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs.This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods.Subsequently,recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized.Finally,the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed.We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.展开更多
Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challeng...Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challenges.The precise reaction mechanism for ORR of these catalysts is still unclear on significant aspects involving the rate-determining step and the nature of the ligand effect.Herein,we report a class of solvothermal synthesis of PtRE(RE is Dy or La)nanoalloys.Such PtRE nanoalloys here are active and stable in acidic media,with both high mass activities enhanced by 2-5 times relative to commercial Pt/C catalyst and high stabilities indicative of the little activity decay and negligible structure change after 10,000 cycles.Density functional theory calculations firmly confirm that the ligand effect of RE elements accelerates an O-O bond scission and steers the rate-determining steps from OH^(*)+H^(+)+e-→H_(2)O(on pure Pt surface)to HOOH^(*)+H^(+)+e-→OH^(*)+H_(2)O(on the PtRE nanoalloy surface)for the fast reaction kinetics,which could be fine-tuned by regulating the RE electronic structures and consequently endows the maximal rate of ORR catalysis with PtDy alloy catalysts.展开更多
Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis.However,their electrocatalytic performance were constrained by the limited modula...Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis.However,their electrocatalytic performance were constrained by the limited modulating strategy.Herein,using N-doped commercial coconut shell-derived activated carbon(AC)as catalyst model,the controllably enhanced sp^(2)-C domains,through an flash Joule heating process,effectively improve the edge defect density and overall graphitization degree of AC catalyst,which tunes the electronic structure of N configurations and accelerates electron transfer,leading to excellent oxygen reduction reaction performance(half-wave potential of 0.884 VRHE,equivalent to commercial 20%Pt/C,with a higher kinetic current density of 5.88 mA cm^(−2))and oxygen evolution reaction activity(overpotential of 295 mV at 10 mA cm^(2)).In a Zn-air battery,the catalyst shows outstanding cycle stability(over 1200 h)and a peak power density of 121 mW cm^(−2),surpassing commercial Pt/C and RuO_(2)catalysts.Density functional theory simulation reveals that the enhanced catalytic activity arises from the axial regulation of local sp^(2)-C domains.This work establishes a robust strategy for sp^(2)-C domain modulation,offering broad applicability in natural biomass-based carbon catalysts for electrocatalysis.展开更多
For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable sur...For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.展开更多
Functional carbon-based materials have become a key research direction in the field of advanced electrocatalysis due to their unique structure and properties.Various strategies have been proposed to design and synthes...Functional carbon-based materials have become a key research direction in the field of advanced electrocatalysis due to their unique structure and properties.Various strategies have been proposed to design and synthesize high-performance carbon-based electrocatalysts.In this review,we comprehensively summarize the latest developments in carbon-based materials for advanced electrocatalysis,with particular emphasis on the structure design strategies and the intrinsic relationship between structure,activity,and performance.The functionalization of multi-dimensional carbon-based materials with enhanced electrocatalytic performance is first addressed.Next,the impact of electronic and structural engineering on the performance of carbon-based materials for electrocatalysis is discussed in terms of the advantages of different types of carbon-based materials in electrocatalytic applications.Finally,the prospects in areas such as precise tuning of functional carbon-based materials,the development of renewable carbon materials,the use of advanced characterization techniques and the promotion of smart manufacturing and responsiveness are high-lighted.展开更多
Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reactio...Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.展开更多
With the deep integration of electrochemical research with energy,environment,catalysis,and other fields,more and more new electrochemical catalytic reactions have entered our research field.Alloy catalysts have recen...With the deep integration of electrochemical research with energy,environment,catalysis,and other fields,more and more new electrochemical catalytic reactions have entered our research field.Alloy catalysts have recently emerged as a new type of nanomaterial due to the rapid development of kinetic controlled synthesis technology.These materials offer several advantages over monometallic catalysts,including larger element combinations,complex geometries,bifunctional sites,and reduced use of precious metals.This paper provides a review of alloy electrocatalysts that are designed and prepared specifically for electrocatalytic applications.The use of alloy materials in electrocatalyst design is also discussed,highlighting their widespread application in this field.First,various synthesis methods and synthesis mechanisms are systematically summarized.Following that,by correlating the properties of materials with the structure,relevant strategies toward advanced alloy electrocatalysts including composition regulation,size,morphology,surface engineering,defect engineering,interface engineering and strain engineering are classified.In addition,the important electrocatalytic applications and mechanisms of alloy electrocatalysts are described and summarized.Finally,the current challenges and prospects regarding the development of alloy nanomaterials are proposed.This review serves as a springboard from a fundamental understanding of alloy structural dynamics to design and various applications of electrocatalysts,particularly in energy and environmental sustainability.展开更多
Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis...Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efficiency in pollutants remediation.Although there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory conditions.Realizing industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social demand.In this regard,this review comprehensively summarized several explorations in thefield of photo/electrocatalytic reduction towards potential industrial applications in recent years.Special attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced reactors.The key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.展开更多
Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a chal...Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.展开更多
Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability und...Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability under harsh conditions,nanodiamond has emerged as a promising carbon-based non-metallic material in the field of energy conversion such as electrocatalysis and photocatalysis.Furthermore,nanodiamond,as a new generation of green catalysts,can overcome the poisoning of catalysts by complex pollutants in advanced oxidation processes,thus effectively removing organic matter from water,which is unparalleled in reducing the cost of water purification and avoiding secondary cross-contamination of water by traditional heavy metal-based catalysts.Here,we review the research and development of nanodiamonds as major electrocatalysts and photocatalysts for energy conversion and for air/water treatment for environmental remediation.The relevant properties,trimming strategy,mechanistic understanding,and design principles of nanodiamond as a catalyst are described,as well as the challenges and prospects of this emerging field.展开更多
Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Ov...Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.展开更多
Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attract...Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.展开更多
Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydroge...Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydrogen atoms moving on a catalyst surface was opened up by the setup of the word"hydrogen spillover."However,there is currently a dearth of thorough knowledge regarding the hydrogen spillover effect.Currently,the advancement of sophisticated characterization procedures offers progressively useful information to enhance our grasp of the hydrogen spillover effect.The understanding of material fabrication for hydrogen spillover effect has erupted.Considering these factors,we made an effort to review most of the articles published on the hydrogen spillover effect and carefully analyzed the aspect of material fabrication.All of our attention has been directed toward the molecular pathway that leads to improve hydrogen evolution reactions performance.In addition,we have attempted to elucidate the spillover paths through the utilization of DFT calculations.Furthermore,we provide some preliminary research suggestions and highlight the opportunities and obstacles that are still to be confronted in this study area.展开更多
With characteristics and advantages of functional composite materials,they are commendably adopted in numerous fields especially in oxygen electrocatalysis,which is due to the significant synergies between various com...With characteristics and advantages of functional composite materials,they are commendably adopted in numerous fields especially in oxygen electrocatalysis,which is due to the significant synergies between various components.Herein,a novel bifunctional oxygen electrocatalyst(Co-CNT@COF-Pyr)has been synthesized through in-situ growth of covalent organic frameworks(COFs)layers on the outer surface of highly conductive carbon nanotubes(CNTs)followed by coordination with Co(Ⅱ).For electrocatalytic OER,Co-CNT@COF-Pyr reveals a low overpotential(438 mV)in alkaline electrolyte(1.0 M aqueous solution of KOH)with a current density of 10 mA cm^(-2),which is comparable to most discovered COF-based catalysts.For electrocatalytic ORR,CoCNT@COF-Pyr exhibits a low H_(2)O_(2) yield range(9.0%-10.1%)and a reaction pathway close to 4e^(-)(n=3.82-3.80)in alkaline electrolyte(0.1 M aqueous solution of KOH)within the test potential range of 0.1-0.6 V vs.RHE,which is superior to most reported COF-based catalysts.Hence,this research could not only offer an innovative insight into the construction of composites,but also facilitate the practical application of renewable fuel cells,closed water cycle,and rechargeable metal-air batteries.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22178181)the Natural Science Fund of Tianjin(No.21JCZDJC00180)the Fundamental Research Funds for the Central Universities(Nankai University(No.63243129)).
文摘Electrocatalysis offers efficient and targeted conversion of monomers derived from waste polyester plastics to chemical products under ambient temperature and pressure conditions.This review provides analysis of research on electrochemical upgrading of monomers derived from waste polyester plastics published from2021 to present.Factors for assessing upgrading of waste polyester plastics include alkaline hydrolysis pretreatment,indices of electrochemical reaction process(activity,stability,and techno-economic a nalysis),separation,and product recovery.Types of depolymerization monomers and their value-added products are summarized along with electrocatalytic mechanisms and reaction pathways.Notably,cathode coupled reactions offer significant value for anodic waste plastic oxidation during electrolysis processes.Development of bifunctional electrocatalysts can reduce the cost of coupled systems and complexity of the electrolyzer.Upgrading and recycling of waste plastic monomers using electrocatalytic technology should undergo downstream processing to form high-value products containing C-N and C-S derived functional groups obtained from depolymerized monomers,Electrochemical conversion and upgrading of monomers derived from waste polyester plastics can contribute to industrialization and global economies and help to realize environmental sustainability.
基金the National Natural Science Foundation of China(No.52300084)China Postdoctoral Science Foundation(No.2023M741151)the Fundamental Research Funds for the Central Universities(No.2024MS063)。
文摘Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimetallic PdCu/TiO_(x)composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOxnanotube arrays.Denitrification experiments demonstrated that the Pd_(1)Cu_(1)/TiO_(x)catalyst exhibited the highest(NO_(3^(–)))removal rate(81.2%)and N_(2)selectivity(67.2%)among all tested catalysts.Leveraging the exceptional light-responsive property of TiO_(x),the introduction of light energy as an assisting factor in electrocatalysis further augmented the(NO_(3^(–)))treatment rate,resulting in a higher(NO_(3^(–)))removal rate of 95.1%and N_(2)selectivity of approximately 90%.Compared to individual electrocatalysis and photocatalysis systems,the overpotential for the catalytic interface active*H formation in the photo-assisted electrocatalysis system was remarkably reduced,thus accelerating electron migration and promoting(NO_(3^(–)))reduction kinetics.Economic analysis revealed an energy consumption of 2.74 k Wh/mol and a corresponding energy consumption per order(EEO)of 0.79 k Wh/m^(3)for the Pd_(1)Cu_(1)/TiOxcatalyst to reduce 25.2 mg/L of(NO_(3^(–)))-N in water to N_(2),showcasing remarkable competitiveness and economic advantages over other water treatment technologies.This study developed the PdCu/TiOxelectrocatalysts with high(NO_(3^(–)))removal rates and N_(2)selectivity,particularly when combined with light energy,the efficiency and selectivity were significantly enhanced,offering a competitive and economically viable solution for wastewater treatment.
基金supported by the National Natural Science Foundation of China(NSFC)(Grant Nos.22475132 and 52101259)the Shenzhen Science and Technology Innovation Committee(Grant No.JCYJ20210324105008022)financially supported by the Shenzhen Science and Technology Innovation Program(Nos.KQTD20190929173914967 and ZDSYS20220527171401003).
文摘Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications,yet it remains challenging to do so on the surface of multimetallic nanocrystals.Herein,we present the multifactorial engineering(size,shape,phase,and composition)of the fully ordered PtBi nanoplates at atomic level,achieving a unique catalyst surface where the face-centered cubic(fcc)Pt edges are modified by the isolated Pd atoms and BiO_(x)adatoms.This Pd_(1)/Pt-BiO_(x)electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg^(-1)Pt+Pd toward ethanol oxidation in alkaline electrolyte and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm^(−2).The surrounding BiO_(x)adatoms are critical for mitigating CO-poisoning on the Pt surface,and the Pd_(1)/Pt single-atom alloy further facilitates the electrooxidation of CH_(3)CH_(2)OH.This work offers new insights into the rational design and construction of sophisticated catalyst surface at single-atomic sites for highly efficient electrocatalysis.
文摘To enhance the efficiency of green energy harvesting and pollutant degradation,significant efforts are focused on identifying highly effective catalysts.Metal-nitrogen-carbon single-atom catalysts(M-N-C SACs)have emerged as pivotal in catalysis due to their unique geometric structures,electronic states,and catalytic capabilities.Notably,the incorporation of magnetic elements at the active centers of these single-atom catalysts has garnered attention for their role in efficient electrochemical conversions.The orientation of spin states critically influences the adsorption and formation of reactants and intermediates,making the precise control of spin alignment and magnetic moments essential for reducing energy barriers and overcoming spin-related limitations,thereby enhancing catalytic activity.Thus,understanding the catalytic role of spin and modulating spin density at M-N-C single-atom centers holds profound fundamental and technological significance.In this review,we elucidate the fundamental mechanisms governing spin states and its influence in electrocatalysis.We then discuss various strategies for adjusting the spin states of active centers in the M-N-C SACs and the associated characterization techniques.Finally,we outline challenges and future perspectives of spin regulation for high-performance catalysts.This review provides deep insights into the micro-mechanisms of catalytic phenomena and offers a roadmap for designing spin-regulated catalysts for advanced energy applications.
基金supported by the National Key R&D Program of China(No.2023YFA1507204)the National Natural Science Foundation of China(Nos.22171139,22225109,22309054,22071109,22371080,21775048)+2 种基金Natural Science Foundation of Guangdong Province(No.2023B1515020076)China Postdoctoral Science Foundation(No.2023M731154)China National Postdoctoral Program for Innovative Talents(No.BX20220116)。
文摘Multi-metal porous crystalline materials(MPCM),integrating the functions of both multi-metal centres and porous crystalline materials(e.g.,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)),are an extended class of porous materials that have attracted much attention for a broad range of applications.Owing to the advantages of these materials,they generally display high porosity,multimetal active sites,well-tuned functions,and pre-designable structures,etc.,serving as desired platforms for the study of structure-property relationships.In view of the clean and sustainable target,a series of MPCM have been explored as electrocatalysts for electrocatalytic reactions like hydrogen evolution reaction,oxygen evolution reaction and electrocatalytic CO_(2)reduction reaction.Concerning the progress achieved for MPCM in electrocatalytic field during past years,this review will provide a brief introduction on the recent breakthrough of MPCM based electrocatalysts including their synthesis methods,structure design,component/morphology tuning,electrocatalytic property and structure-property relationship,etc.Besides,it will also conclude the current challenges and present perspectives for the MPCM based electrocatalysts,which might promote the development of porous crystalline materials in electrocatalysis and hope to provide new insights for scientists in related fields.
文摘In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in which synchronous hypophosphite ion(H_(2)PO_(2)^(-))oxidation to phosphate ion(PO_(4)^(3–))(POR)and nitrate reduction(NO_(3)RR)to ammonia(NH_(3))occur,followed by cascade chemical precipitation to generate struvite.Herein,a bifunctional Cu_(2)O@NiFe_(2)O_(4)Z-scheme heterojunction with a yolk/shell structure and oxygen vacancies(OVs)was designed and developed to optimize the NO_(3)RR/POR.Serving as a key component,the established PA-EC system consisted of a Janus Cu_(2)O@NiFe_(2)O_(4)/NF self-supporting integrated photocathode and a Cu_(2)O@NiFe_(2)O_(4)/NF photocathode with efficient struvite PA-EC synthesis performance under a low cell voltage of 1.6 V vs NHE.Specifically,Janus Cu_(2)O@NiFe_(2)O_(4)/NF photocathode exhibits superior performance with a high NH3 yield of 38.06 mmol L^(-1)and a faradaic efficiency(FE)of 92.31%at 1.6 V vs.NHE and enables ammonia FE over 60%in a broad NO_(3)–concentration window of 0.005–0.5 mol L^(-1).The photoassisted electrochemical catalytic mechanism and reaction pathway for struvite synthesis on Cu_(2)O@NiFe_(2)O_(4)were investigated through a series of experiments and theoretical calculations.The results demonstrated the critical roles of the interfacial electric field,void confinement,and oxygen vacancies in promoting the overall catalytic efficiency.These encouraging results warrant further studies on combined P and N recovery for efficient production of valuable fertilizers.
基金supported by the National Key Projects for Fundamental Research and Development of China(2021YFA1500803)the National Natural Science Foundation of China(51825205,52120105002,22088102,22279150,22209186)+1 种基金the Beijing Natural Science Foundation(2222080)the Youth Innovation Promotion Association of the CAS(Y2021011)。
文摘Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant challenge for practical application.Recently,twodimensional transition metal dichalcogenides(2D-TMDs)have emerged as attractive and cost-effective alternatives for efficient electrocatalysis in the HER.Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs.This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods.Subsequently,recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized.Finally,the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed.We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.
基金supported by the National Natural Science Foundation of China(No.21975151)China Postdoctoral Science Foundation(No.2023M733452).
文摘Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challenges.The precise reaction mechanism for ORR of these catalysts is still unclear on significant aspects involving the rate-determining step and the nature of the ligand effect.Herein,we report a class of solvothermal synthesis of PtRE(RE is Dy or La)nanoalloys.Such PtRE nanoalloys here are active and stable in acidic media,with both high mass activities enhanced by 2-5 times relative to commercial Pt/C catalyst and high stabilities indicative of the little activity decay and negligible structure change after 10,000 cycles.Density functional theory calculations firmly confirm that the ligand effect of RE elements accelerates an O-O bond scission and steers the rate-determining steps from OH^(*)+H^(+)+e-→H_(2)O(on pure Pt surface)to HOOH^(*)+H^(+)+e-→OH^(*)+H_(2)O(on the PtRE nanoalloy surface)for the fast reaction kinetics,which could be fine-tuned by regulating the RE electronic structures and consequently endows the maximal rate of ORR catalysis with PtDy alloy catalysts.
基金supported by National Natural Science Foundation of China (No. 32371810)China Postdoctoral Science Foundation (2023M731702)+5 种基金National Key Research and Development Program of China (2023YFB4203702)the Foundation Research Project of Jiangsu Province (BK20221338)Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesInternational Innovation Center for Forest Chemicals and Materials,Nanjing Forestry Universitymerit-based funding for Nanjing innovation and technology projectsthe Foundation of Jiangsu Key Lab of Biomass Energy and Material (JSBEM-S-202101)
文摘Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis.However,their electrocatalytic performance were constrained by the limited modulating strategy.Herein,using N-doped commercial coconut shell-derived activated carbon(AC)as catalyst model,the controllably enhanced sp^(2)-C domains,through an flash Joule heating process,effectively improve the edge defect density and overall graphitization degree of AC catalyst,which tunes the electronic structure of N configurations and accelerates electron transfer,leading to excellent oxygen reduction reaction performance(half-wave potential of 0.884 VRHE,equivalent to commercial 20%Pt/C,with a higher kinetic current density of 5.88 mA cm^(−2))and oxygen evolution reaction activity(overpotential of 295 mV at 10 mA cm^(2)).In a Zn-air battery,the catalyst shows outstanding cycle stability(over 1200 h)and a peak power density of 121 mW cm^(−2),surpassing commercial Pt/C and RuO_(2)catalysts.Density functional theory simulation reveals that the enhanced catalytic activity arises from the axial regulation of local sp^(2)-C domains.This work establishes a robust strategy for sp^(2)-C domain modulation,offering broad applicability in natural biomass-based carbon catalysts for electrocatalysis.
基金supported by National Natural Science Foundation of China(No.52202366)Taishan Scholar Project of Shandong Province(tstp20240515,tsqn202312217)+1 种基金Natural Science Foundation of Shandong Province(China,No.2025HWYQ-050,ZR2021QE011,ZR2022QH072,ZR2021QE284)the King Abdullah University of Science and Technology,the Center of Excellence for Renewable Energy and Storage Technologies.
文摘For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.
文摘Functional carbon-based materials have become a key research direction in the field of advanced electrocatalysis due to their unique structure and properties.Various strategies have been proposed to design and synthesize high-performance carbon-based electrocatalysts.In this review,we comprehensively summarize the latest developments in carbon-based materials for advanced electrocatalysis,with particular emphasis on the structure design strategies and the intrinsic relationship between structure,activity,and performance.The functionalization of multi-dimensional carbon-based materials with enhanced electrocatalytic performance is first addressed.Next,the impact of electronic and structural engineering on the performance of carbon-based materials for electrocatalysis is discussed in terms of the advantages of different types of carbon-based materials in electrocatalytic applications.Finally,the prospects in areas such as precise tuning of functional carbon-based materials,the development of renewable carbon materials,the use of advanced characterization techniques and the promotion of smart manufacturing and responsiveness are high-lighted.
基金support from Horizon 2020 program within the ITN FlowcampDZ acknowledges funding from the Wohl Foundation for research for the promotion of UK-Israel research cooperationDZ acknowledges funding from Israel Ministry of Energy(grant#220-11-047).
文摘Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.
基金supported by the National Natural Science Foundation of China(No.52072153)the Postdoctoral Science Foundation of China(No.2021M690023)+2 种基金the Postdoctoral Science Foundation of Jiangsu Province(No.2021K176B)the Graduate Research Innovation Program of Jiangsu Provincial(Nos.KYCX22_3694 and KYCX23_3649)the Zhenjiang Key R&D Programmes(No.SH2021021)。
文摘With the deep integration of electrochemical research with energy,environment,catalysis,and other fields,more and more new electrochemical catalytic reactions have entered our research field.Alloy catalysts have recently emerged as a new type of nanomaterial due to the rapid development of kinetic controlled synthesis technology.These materials offer several advantages over monometallic catalysts,including larger element combinations,complex geometries,bifunctional sites,and reduced use of precious metals.This paper provides a review of alloy electrocatalysts that are designed and prepared specifically for electrocatalytic applications.The use of alloy materials in electrocatalyst design is also discussed,highlighting their widespread application in this field.First,various synthesis methods and synthesis mechanisms are systematically summarized.Following that,by correlating the properties of materials with the structure,relevant strategies toward advanced alloy electrocatalysts including composition regulation,size,morphology,surface engineering,defect engineering,interface engineering and strain engineering are classified.In addition,the important electrocatalytic applications and mechanisms of alloy electrocatalysts are described and summarized.Finally,the current challenges and prospects regarding the development of alloy nanomaterials are proposed.This review serves as a springboard from a fundamental understanding of alloy structural dynamics to design and various applications of electrocatalysts,particularly in energy and environmental sustainability.
基金supported by the National Natural Science Foundation of China(22278030,22090032,22090030,22288102,22242019)the Fundamental Research Funds for the Central Universities(buctrc202119,2312018RC07)+1 种基金Major Program of Qingyuan Innovation Laboratory(Grant No.001220005)the Experiments for Space Exploration Program and the Qian Xuesen Laboratory,China Academy of Space Technology。
文摘Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efficiency in pollutants remediation.Although there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory conditions.Realizing industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social demand.In this regard,this review comprehensively summarized several explorations in thefield of photo/electrocatalytic reduction towards potential industrial applications in recent years.Special attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced reactors.The key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.
基金This work was supported by the National Natural Science Foundation of China(22279008 and 22109082)the Beijing Institute of Technology Research Fund Program for Young Scholarsthe Tsinghua University Initiative Scientific Research Program。
文摘Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.
基金funded by National Natural Science Foundation of China(Nos.52102162 and 11975205)Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515011794 and 2020B1515120048)+1 种基金the Young Talents in Higher Education of Guangdong(No.2021KQNCX273)the support from Jiangsu Science and Technology Programme-YoungScholar(BK20200251)。
文摘Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability under harsh conditions,nanodiamond has emerged as a promising carbon-based non-metallic material in the field of energy conversion such as electrocatalysis and photocatalysis.Furthermore,nanodiamond,as a new generation of green catalysts,can overcome the poisoning of catalysts by complex pollutants in advanced oxidation processes,thus effectively removing organic matter from water,which is unparalleled in reducing the cost of water purification and avoiding secondary cross-contamination of water by traditional heavy metal-based catalysts.Here,we review the research and development of nanodiamonds as major electrocatalysts and photocatalysts for energy conversion and for air/water treatment for environmental remediation.The relevant properties,trimming strategy,mechanistic understanding,and design principles of nanodiamond as a catalyst are described,as well as the challenges and prospects of this emerging field.
基金We are grateful for financial support from the“Hundred Talents Program”of the Chinese Academy of Sciences and the“Young Talents Training Program”of the Shanghai Branch of the Chinese Academy of Sciences.We acknowledge the financial support from the National Science Youth Foundation of China(22202205)Xiamen City Natural Science Foundation of China(3502Z20227256)Fujian Provincial Natural Science Foundation of China(2022J01502).
文摘Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.
基金financially supported by the National Natural Science Foundation of China(Nos.21677010,51808037)the National Key R&D Program of China(No.2021YFB3500702)the Special Fund of Beijing Key Laboratory of Indoor Air Quality Evaluation and Control(No.BZ0344KF21-04)。
文摘Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.
基金supported by Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(Grant Nos.RS-2023-00284361 and 2021R1A2C2091497)supported by the Nano&Materials Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2024-00436563)
文摘Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydrogen atoms moving on a catalyst surface was opened up by the setup of the word"hydrogen spillover."However,there is currently a dearth of thorough knowledge regarding the hydrogen spillover effect.Currently,the advancement of sophisticated characterization procedures offers progressively useful information to enhance our grasp of the hydrogen spillover effect.The understanding of material fabrication for hydrogen spillover effect has erupted.Considering these factors,we made an effort to review most of the articles published on the hydrogen spillover effect and carefully analyzed the aspect of material fabrication.All of our attention has been directed toward the molecular pathway that leads to improve hydrogen evolution reactions performance.In addition,we have attempted to elucidate the spillover paths through the utilization of DFT calculations.Furthermore,we provide some preliminary research suggestions and highlight the opportunities and obstacles that are still to be confronted in this study area.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2022SHFZ299)the National Natural Science Foundation of China(Nos.52063014 and 51873053)。
文摘With characteristics and advantages of functional composite materials,they are commendably adopted in numerous fields especially in oxygen electrocatalysis,which is due to the significant synergies between various components.Herein,a novel bifunctional oxygen electrocatalyst(Co-CNT@COF-Pyr)has been synthesized through in-situ growth of covalent organic frameworks(COFs)layers on the outer surface of highly conductive carbon nanotubes(CNTs)followed by coordination with Co(Ⅱ).For electrocatalytic OER,Co-CNT@COF-Pyr reveals a low overpotential(438 mV)in alkaline electrolyte(1.0 M aqueous solution of KOH)with a current density of 10 mA cm^(-2),which is comparable to most discovered COF-based catalysts.For electrocatalytic ORR,CoCNT@COF-Pyr exhibits a low H_(2)O_(2) yield range(9.0%-10.1%)and a reaction pathway close to 4e^(-)(n=3.82-3.80)in alkaline electrolyte(0.1 M aqueous solution of KOH)within the test potential range of 0.1-0.6 V vs.RHE,which is superior to most reported COF-based catalysts.Hence,this research could not only offer an innovative insight into the construction of composites,but also facilitate the practical application of renewable fuel cells,closed water cycle,and rechargeable metal-air batteries.
