Electrocatalytic activity is influenced by the surface charge on the solid catalyst.Conventionally,our attention has been focused on how the surface charge shapes the electric potential and concentration of ionic reac...Electrocatalytic activity is influenced by the surface charge on the solid catalyst.Conventionally,our attention has been focused on how the surface charge shapes the electric potential and concentration of ionic reactant(s)in the local reaction zone.Taking H_(2)O_(2)redox reactions at Pt(111)as a model system,we reveal a peculiar surface charge effect using ab initio molecular dynamics simulations of electrified Pt(111)-water interfaces.In this scenario,the negative surface charge on Pt(111)repels the O-O bond of the reactant(H_(2)O_(2))farther away from the electrode surface.This leads to a higher activation barrier for breaking the O-O bond.Incorporating this microscopic mechanism into a microkinetic-double-layer model,we are able to semi-quantitatively interpret the pH-dependent activity of H_(2)O_(2)redox reactions at Pt(111),especially the anomalously suppressed activity of H_(2)O_(2)reduction with decreasing electrode potential.The relevance of the present surface charge effect is also examined in wider scenarios with different electrolyte cations,solution pHs,crystal facets of the catalyst,and model parameters.In contrast with previous mechanisms focusing on how surface charge influences the local reaction condition at a fixed reaction plane,the present work gives an example in which the location of the reaction plane is adjusted by the surface charge.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
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
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
Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to ...Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to improve sulfur electrochemistry by synergistically enhancing polysulfide fixation and catalytic conversions.Fabricated through mild sequential boronation and sulfurization,this hybrid nanocatalyst integrates the strong polysulfide adsorbability and high conductivity of Ni_(2)B with the high catalytic activity of Ni_(3)S_(2).More importantly,the as-constructed heterointerface inspires new,highly catalytic sites that smooth consecutive sulfur conversions with lower energy barriers,while the built-in electric fields promote directional charge transfer,collectively contributing to fast-kinetic and highly efficient sulfur redox reactions.As a result,Li-S cells incorporating the Ni_(3)S_(2)/Ni_(2)B nanocatalyst exhibit excellent cyclability,with minimal capacity decay of 0.017%per cycle over 900 cycles at 1 C and a superb rate capability of up to 5 C.Even under demanding conditions,such as a high sulfur loading of 5.0 mg cm^(-2)and a low electrolyte-to-sulfur(E/S)ratio of 4.8 mL g^(-1),high capacity and cyclability are maintained,highlighting the great potential of this unique heterointerface engineering in advancing high-performance and practically viable Li-S batteries.展开更多
This review delves into the emerging field of multidimensional catalysis,with a particular focus on the regulation of electrocatalysis by external magnetic fields.It outlines the significance of electrocatalysis in cl...This review delves into the emerging field of multidimensional catalysis,with a particular focus on the regulation of electrocatalysis by external magnetic fields.It outlines the significance of electrocatalysis in clean energy conversion and storage,and how magnetic fields can enhance the efficiency,selectivity,and stability of electrocatalytic reactions through various mechanisms such as Lorentz force,magnetocaloric effects,and spin selectivity.The review also discusses the historical evolution of catalysis research from one-dimensional to multidimensional and highlights the role of magnetic fields in catalyst synthesis,mass transfer,electron transfer,and reaction kinetics.Furthermore,it summarizes key applications of magnetic fields in different electrocatalytic reactions,supported by theoretical calculations that provide insights into the microscopic mechanisms.This comprehensive overview not only offers a theoretical and experimental foundation for the development of new electrocatalysts but also paves the way for more efficient and sustainable electrocatalytic technologies,marking a significant step toward the advancement of clean energy solutions.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
The quest for efficient and durable catalysts using abundant resources has garnered significant interest in the field of bifunctional oxygen electrocatalysis.In this contribution,we have designed a FeN_(4)or CoN_(4)em...The quest for efficient and durable catalysts using abundant resources has garnered significant interest in the field of bifunctional oxygen electrocatalysis.In this contribution,we have designed a FeN_(4)or CoN_(4)embedded graphene-based bilayer as active layer and TMC_(3)or TMN_(3)doped graphene as supporting layer,named as FeN_(4)/TMC_(3)or FeN_(4)/TMN_(3)and CoN_(4)/TMC_(3)or CoN_(4)/TMN_(3),wherein TM strands for transition metal.Based on density functional theory calculations,our results demonstrate that the interaction formed between dual metal atoms in the bilayer interspace leads to the coordination environment altered from flat four-coordination to spatial five-coordination,further stabilizing the bilayer structure and impairing its affinity toward the O-containing intermediates.According to thermodynamic analysis,the bilayers of CoN_(4)/CoN_(3),FeN_(4)/FeC_(3),FeN_(4)/CoC_(3),FeN_(4)/NiC_(3),FeN_(4)/ZnC_(3),FeN_(4)/FeN_(3),FeN_(4)/CrN_(3)and FeN_(4)/ZnN_(3)are attractively promising for bifunctional oxygen electrocatalysis due to the small overpotential differenceΔηbetween oxygen reduction and oxygen evolution that are less than 1 V.Density functional theory calculations combined with machine learning analysis directly identify the key role played by the interbinding formed between bilayers,that boosts catalytic activity,which establishes a predictable framework for a fast screen for graphene-based bilayer vertical heterojunction.This work opens up a new path for designing the efficient electrocatalysts via modification of coordination environment.展开更多
Metallic core–shell nanoparticles(MCSNs)have attracted significant research interest in electrochemical energy conversion owing to their distinctive microstructures and superior catalytic performances.By rationally d...Metallic core–shell nanoparticles(MCSNs)have attracted significant research interest in electrochemical energy conversion owing to their distinctive microstructures and superior catalytic performances.By rationally designing a metallic core with a specific surface(shell),synergistic interactions between the core and the shell,benefiting from the intrinsic strain,ligand,geometric,and ensemble effects,can endow multi-metallic CSNs with highly enhanced activity,selectivity,and stability in electrocatalytic reactions,compared to their monometallic counterparts.In this review,we outline the key breakthroughsDespe cially in the past 5 yearsDof MCSNs,focusing on their precise design/synthesis,intrinsic effects arising from core–shell interactions,state-of-the-art characterization techniques,and exceptional performance in critical electrochemical reactions,including water splitting,oxygen reduction reaction(ORR),CO_(2)reduction reaction(CO_(2)RR),N_(2)/NO_(3)-reduction reaction(N_(2)RR/NO_(3)RR),and small organic molecule electrooxidations.We further discuss the ongoing challenges and opportunities for MCSNs,particularly in achieving computationally guided design/atomic-precision synthesis,enabling scalable production,and advancing in situ or operando characterization methods.We hope that the present review will inspire chemists working in this field to develop new MCSNs for sustainable energy applications.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
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g−1,reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g−1,achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environm...High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.展开更多
Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the...Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.展开更多
文摘Electrocatalytic activity is influenced by the surface charge on the solid catalyst.Conventionally,our attention has been focused on how the surface charge shapes the electric potential and concentration of ionic reactant(s)in the local reaction zone.Taking H_(2)O_(2)redox reactions at Pt(111)as a model system,we reveal a peculiar surface charge effect using ab initio molecular dynamics simulations of electrified Pt(111)-water interfaces.In this scenario,the negative surface charge on Pt(111)repels the O-O bond of the reactant(H_(2)O_(2))farther away from the electrode surface.This leads to a higher activation barrier for breaking the O-O bond.Incorporating this microscopic mechanism into a microkinetic-double-layer model,we are able to semi-quantitatively interpret the pH-dependent activity of H_(2)O_(2)redox reactions at Pt(111),especially the anomalously suppressed activity of H_(2)O_(2)reduction with decreasing electrode potential.The relevance of the present surface charge effect is also examined in wider scenarios with different electrolyte cations,solution pHs,crystal facets of the catalyst,and model parameters.In contrast with previous mechanisms focusing on how surface charge influences the local reaction condition at a fixed reaction plane,the present work gives an example in which the location of the reaction plane is adjusted by the surface charge.
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.
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.
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.
基金supported by the National Natural Science Foundation of China(22379069,22109072)the Fundamental Research Funds for the Central Universities(30922010304)。
文摘Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to improve sulfur electrochemistry by synergistically enhancing polysulfide fixation and catalytic conversions.Fabricated through mild sequential boronation and sulfurization,this hybrid nanocatalyst integrates the strong polysulfide adsorbability and high conductivity of Ni_(2)B with the high catalytic activity of Ni_(3)S_(2).More importantly,the as-constructed heterointerface inspires new,highly catalytic sites that smooth consecutive sulfur conversions with lower energy barriers,while the built-in electric fields promote directional charge transfer,collectively contributing to fast-kinetic and highly efficient sulfur redox reactions.As a result,Li-S cells incorporating the Ni_(3)S_(2)/Ni_(2)B nanocatalyst exhibit excellent cyclability,with minimal capacity decay of 0.017%per cycle over 900 cycles at 1 C and a superb rate capability of up to 5 C.Even under demanding conditions,such as a high sulfur loading of 5.0 mg cm^(-2)and a low electrolyte-to-sulfur(E/S)ratio of 4.8 mL g^(-1),high capacity and cyclability are maintained,highlighting the great potential of this unique heterointerface engineering in advancing high-performance and practically viable Li-S batteries.
基金support from the National Natural Science Foundation of China(No.22405048)the startup funds from Fuzhou University。
文摘This review delves into the emerging field of multidimensional catalysis,with a particular focus on the regulation of electrocatalysis by external magnetic fields.It outlines the significance of electrocatalysis in clean energy conversion and storage,and how magnetic fields can enhance the efficiency,selectivity,and stability of electrocatalytic reactions through various mechanisms such as Lorentz force,magnetocaloric effects,and spin selectivity.The review also discusses the historical evolution of catalysis research from one-dimensional to multidimensional and highlights the role of magnetic fields in catalyst synthesis,mass transfer,electron transfer,and reaction kinetics.Furthermore,it summarizes key applications of magnetic fields in different electrocatalytic reactions,supported by theoretical calculations that provide insights into the microscopic mechanisms.This comprehensive overview not only offers a theoretical and experimental foundation for the development of new electrocatalysts but also paves the way for more efficient and sustainable electrocatalytic technologies,marking a significant step toward the advancement of clean energy solutions.
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.
基金financial support from the National Natural Science Foundation of China(Nos.21503097,52130101,51701152,21806023,and 51702345)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_3905)。
文摘The quest for efficient and durable catalysts using abundant resources has garnered significant interest in the field of bifunctional oxygen electrocatalysis.In this contribution,we have designed a FeN_(4)or CoN_(4)embedded graphene-based bilayer as active layer and TMC_(3)or TMN_(3)doped graphene as supporting layer,named as FeN_(4)/TMC_(3)or FeN_(4)/TMN_(3)and CoN_(4)/TMC_(3)or CoN_(4)/TMN_(3),wherein TM strands for transition metal.Based on density functional theory calculations,our results demonstrate that the interaction formed between dual metal atoms in the bilayer interspace leads to the coordination environment altered from flat four-coordination to spatial five-coordination,further stabilizing the bilayer structure and impairing its affinity toward the O-containing intermediates.According to thermodynamic analysis,the bilayers of CoN_(4)/CoN_(3),FeN_(4)/FeC_(3),FeN_(4)/CoC_(3),FeN_(4)/NiC_(3),FeN_(4)/ZnC_(3),FeN_(4)/FeN_(3),FeN_(4)/CrN_(3)and FeN_(4)/ZnN_(3)are attractively promising for bifunctional oxygen electrocatalysis due to the small overpotential differenceΔηbetween oxygen reduction and oxygen evolution that are less than 1 V.Density functional theory calculations combined with machine learning analysis directly identify the key role played by the interbinding formed between bilayers,that boosts catalytic activity,which establishes a predictable framework for a fast screen for graphene-based bilayer vertical heterojunction.This work opens up a new path for designing the efficient electrocatalysts via modification of coordination environment.
基金supported by funds provided by the National Natural Science Foundation of China(22201294)Guangdong Basic and Applied Basic Research Foundation(2023A1515012370)+4 种基金Guangdong Pearl River Talent Program(2023QN10C361)HighLevel Talents Program of the CAS(E344021001)Clean Energy Joint International Laboratory(E3G1041001)Shenzhen Science and Technology Program(KQTD20221101093647058)SIAT Innovation Fund for Excellent Young Scientists(E3G0071001)。
文摘Metallic core–shell nanoparticles(MCSNs)have attracted significant research interest in electrochemical energy conversion owing to their distinctive microstructures and superior catalytic performances.By rationally designing a metallic core with a specific surface(shell),synergistic interactions between the core and the shell,benefiting from the intrinsic strain,ligand,geometric,and ensemble effects,can endow multi-metallic CSNs with highly enhanced activity,selectivity,and stability in electrocatalytic reactions,compared to their monometallic counterparts.In this review,we outline the key breakthroughsDespe cially in the past 5 yearsDof MCSNs,focusing on their precise design/synthesis,intrinsic effects arising from core–shell interactions,state-of-the-art characterization techniques,and exceptional performance in critical electrochemical reactions,including water splitting,oxygen reduction reaction(ORR),CO_(2)reduction reaction(CO_(2)RR),N_(2)/NO_(3)-reduction reaction(N_(2)RR/NO_(3)RR),and small organic molecule electrooxidations.We further discuss the ongoing challenges and opportunities for MCSNs,particularly in achieving computationally guided design/atomic-precision synthesis,enabling scalable production,and advancing in situ or operando characterization methods.We hope that the present review will inspire chemists working in this field to develop new MCSNs for sustainable energy applications.
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financial support from the National Natural Science Foundation of China(22109127)the Chinese Postdoctoral Science Foundation(2021M702666),+1 种基金he Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(Grant No.2023-TS-02)financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"and the Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)are also sincerely appreciated.
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g−1,reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g−1,achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
基金supported by the Australian Research Council(ARC)Projects(DP220101139,DP220101142,and LP240100542).
文摘High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.
基金supported by the Major Science and Technology Special Plan of Yunnan Province(Nos.202302AB080012 and 202402AB080004)the National Natural Science Foundation of China(No.22264025)+1 种基金the Basic Research Foundation of Yunnan Province(Nos.202401AS070033 and 202501AT070055)the Reserve talents for young and middleaged academic and technical leaders project of Yunnan Province(No.202405AC350071).
文摘Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.
