摘要：Metal-based electrocatalysts with different sizes(single atoms,nanoclusters,and nanoparticles)show different catalytic behaviors for various electrocatalytic *** the coordination environment of active sites with precision to rationally design an efficient electrocatalyst is of great significance for boosting electrocatalytic *** review summarizes the recent process of heterogeneous supported single atoms,nanoclusters,and nanoparticles catalysts in electrocatalytic reactions,respectively,and figures out the construct strategies and design concepts based on their strengths and ***,four key factors for enhancing electrocatalytic performance,including electronic structure,coordination environment,support property,and interfacial interactions are proposed to provide an overall comprehension to readers in this ***,some insights into the current challenges and future opportunities of the heterogeneous supported electrocatalysts are provided.

摘要：Water electrolysis technology holds the perfect promise of the hydrogen production,yet control of efficiency and rate of water electrolysis greatly relies on the availability of high-performance electrode materials for kinetic-sluggish oxygen evolution reaction(OER).Accordingly,substantial endeavors have been made to explore advanced electrode materials over the past ***,RuO_(2) and RuO_(2)-based materials have been demonstrated to be promising for OER due to their remarkable electrocatalytic activity and pH-universal ***,the great achievements and progresses of this flourishing spot are comprehensively reviewed,which are started by a general description of OER to understand the reaction mechanism in ***,the key advantages and issues of RuO_(2) towards OER are also introduced,followed by proposing many advanced strategies for further promoting the electrocatalytic OER performance of RuO_(2).Finally,the daunting challenges and future progresses of RuO_(2) electrocatalysts toward practical water oxidation are highlighted,aiming to provide guidance for the fabrication of desirable RuO_(2)-based electrocatalysts toward OER.

摘要：The recent development of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide（CO） has attracted much attention due to their unique activity and selectivity compared to other metal catalysts. Particularly, Cu is the unique electrocatalyst for COelectrochemical reduction with high selectivity to generate a variety of hydrocarbons. In this review, we mainly summarize the recent advances on the rational design of Cu nanostructures, the composition regulation of Cu-based alloys, and the exploitation of advanced supports for improving the catalytic activity and selectivity toward electrochemical reduction of CO. The special focus is to demonstrate how to enhance the activity and selectivity of Cubased electrocatalyst for COreduction. The perspectives and challenges for the development of Cu-based electrocatalysts are also addressed. We hope this review can provide timely and valuable insights into the design of advanced electrocatalytic materials for COelectrochemical reduction.

摘要：The rational design and construction of hierarchically porous nanostructure for oxygen reduction reaction (ORR) electrocatalysts is crucial to facilitate the exposure of accessible active sites and promote the mass/electron transfer under the gas-solid-liquid triple-phase condition. Herein, an ingenious method through the pyrolysis of creative polyvinylimidazole coordination with Zn/Fe salt precursors is developed to fabricate hierarchically porous Fe-N-doped carbon framework as efficient ORR electrocatalyst. The volatilization of Zn species combined with the nanoscale Kirkendall effect of Fe dopants during the pyrolysis build the hierarchical micro-, meso-, and macroporous nanostructure with a high specific surface area (1,586 m^(2)·g^(−1)), which provide sufficient exposed active sites and multiscale mass/charge transport channels. The optimized electrocatalyst exhibits superior ORR activity and robust stability in both alkaline and acidic electrolytes. The Zn-air battery fabricated by such attractive electrocatalyst as air cathode displays a higher peak power density than that of Pt/C-based Zn-air battery, suggesting the great potential of this electrocatalyst for Zn-air batteries.

摘要：Designing highly selective and efficient singleatom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance trends of transition metal complexes with P-based ligands in nitrogen reduction reaction(NRR) and further develops a design principle for high-performance single-atom catalysts(SACs)of NRR. Among the explored catalysts, W@BP(0.40 eV),Ta@BP(0.47 eV), and Nb@BP(0.53 eV) are identified as remarkable candidates with low free energy change in the potential-limiting step, high stability and high electrical conductivity for NRR. It is worth noting that almost all SACs with P-based ligands exhibit high NRR selectivity, due to the fact that they adsorb *N_(2) more strongly than *H. The adsorption free energy of *N_(2) H can be considered as a descriptor for the intrinsic activity trends in NRR. Furthermore, by constructing a volcano plot of the activity against the electronic charge on metal centers, it is demonstrated that the metal center with a moderate amount of positive charge can promote the catalytic performance of NRR.

摘要：Sluggish kinetics of anodic hydrogen oxidation reaction(HOR)in alkaline media,which arises from the two orders of magnitude lower HOR activity in alkali than that in acid media for platinum group metals,hinders the commercial implementation of anion exchange membrane fuel cells(AEMFCs).Consequently,the development of platinum-based catalysts combined with high efficiency and durability is urgently ***,we report a facile route for the synthesis of ternary PtRuTe alloy nanofibers with Pt atomic ratio of only 11%via a simple galvanic replacement *** optimize the adsorption strength of platinum and ruthenium towards hydrogen and hydroxyl species by regulating the electron donation from tellurium to platinum and ***,the obtained trimetallic alloy catalyst exhibits an impressive kinetic current density of 30.6 mA cm^(−2)_(geo) at 50 mV and an exchange current density of 0.426 mA cm^(−2)_(metal),which shows 3.0-and 2.5-fold enhancement compared with the commercial Pt/C in alkaline electrolyte,***,the catalyst also demonstrates excellent stability with merely 5%activity attenuation after 2000 potential *** work offers new pathways to boost alkaline HOR by rationally designing multicomponent alloys.

摘要：Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water ***,production of inexpensive and high-efficiency bifunctional electrocatalysts remains a ***,we demonstrate a simple method to synthesize a paper-mulberry(Broussonetia papyrifera)-inspired Co_(9)S_(8)@CoNi_(2)S_(4)/nickel foam(Co_(9)S_(8)@CoNi_(2)S_(4)/NF)heterojunction with high catalytic activity and *** process involves in situ growth of NiCo layered double hydroxide and in situ derivatization of ZIF-67,followed by the S heteroatom *** Co_(9)S_(8)@CoNi_(2)S_(4)/NF benefits from the heterostructure and functional advantages of multidimensional building blocks including one-dimensional(1D)nanowires,2D nanosheets and *** optimized Co_(9)S_(8)@CoNi_(2)S_(4)/NF heterojunction with 10% sulphur content reveals excellent electrocatalytic activity with the lower overpotentials of 68 mV for hydrogen evolution reaction(HER)and 170 mV for oxygen evolution reaction(OER)at 10 mA cm^(-2) in the 1.0 mol L^(-1) KOH solution,which is superior to the recently reported transition metal based *** outstanding performance is attributed to the strong interface coupling between CoNi_(2)S_(4) and Co_(9)S_(8),the advantage of multidimensional structure and the customized electronic *** density functional theory suggests that the interface between Co_(9)S_(8) and CoNi_(2)S_(4) optimizes the adsorption of the multiple intermediates and further facilitates water splitting *** work offers a generic approach for heterostructure engineering design of highperformance catalytic system applications.

摘要：The polysulfide shuttling and sluggish redox kinetics,due to the notorious adsorption-catalysis underperformance,are the ultimate obstacles of the practical application of lithium-sulfur(Li-S)*** carbon-based and transition metal compound-based material solutions generally suffer from poor catalysis and adsorption,respectively,despite the performance gain in terms of the ***,we have enhanced polysulfide adsorptioncatalytic capability and protected the Li anode using a complementary bimetallic carbide electrocatalyst,Co3 Mo3 C,modified commercial *** this demonstration,the potentials of bimetal compounds,which have been well recognized in other environmental catalysis,are also extended to Li-S *** with this modified separator,a simple cathode(S/Super P composite)can deliver high sulfur utilization,high rate performance,and excellent cycle stability with a low capacity decay rate of^0.034%per cycle at 1 C up to1000 *** at a high S-loading of 8.0 mg cm^-2 with electrolyte/sulfur ratio=6 m L g^-1,the cathode still exhibits high areal capacity of^6.8 m A h cm^-*** experimental analysis and the first-principles calculations proved that the bimetallic carbide Co3 Mo3 C provides more binding sites for adsorbing polysulfides and catalyzing the multiphase conversion of sulfur/polysulfide/sulfide than monometallic carbide Mo2 ***,the modified separator can be reutilized with comparable electrochemical *** also showed other bimetallic carbides with similar catalytic effects on Li-S batteries and this material family has great promise indifferent energy electrocatalytic systems.

摘要：In this work,we report a novel one-dimensional metal-organic framework(MOF)templated for the synthesis of transition metal sulfides with excellent oxygen evolution reaction(OER)performance via a self-sulfidation process,eliminating the need for additional sulfur *** pyrolysis,MOFs containing Co ions as the metal nodes and 1-phenyl-5-mercaptotetrazole(PMTA)as the ligand were transformed to Co_(9)S_(8)nanoparticles,which were encapsulated in a nitrogen and sulfur dual-doped carbon(Co_(9)S_(8)@NSC)***,PMTA,as a ligand,possesses the unique advantage of forming porous coordination polymers with a wide range of metals(e.g.,Fe,Ni,and Cu),enabling the versatile synthesis of transition metal sulfide ***,when served as the electrocatalyst for OER,the N,S co-doped Co_(9)S_(8)@NSC porous nanotubes exhibited excellent OER performance with the overpotential of only 248 mV at 10 mA cm^(−2)and long-term *** works provide new insights and inspiration for the rational design and development of non-precious metal-based sulfides with practical potential applications.