摘要：Electrocatalytic nitrate reduction reaction is considered as a promising and sustainable method for ammonia ***,the selectivity and yield rate of ammonia are limited by the competitive hydrogen evolution reaction and the complex eight-electron transfer ***,we developed a(FeCoNiCu)Ox/CeO_(2)polymetallic oxide electrocatalyst for effective nitrate reduction to *** synergistic effects among the multiple elements in the electrocatalyst were clearly elucidated by comprehensive ***,Cu acted as the active site for reducing nitrate to nitrite,and Co facilitated the subsequent reduction of nitrite to ammonia,while Fe and Ni promoted water dissociation to provide ***,the incorporation of CeO_(2)increased the active surface area of(FeCoNiCu)Ox,resulting in an improved ammonia yield rate to meet industrial ***,the(FeCoNiCu)Ox/CeO_(2)electrocatalyst achieved an ammonia current density of 382 mA cm^(-2)and a high ammonia yield rate of 30.3 mg h^(-1)cm^(-2)with a long-term *** work offers valuable insights for the future design of highly efficient multi-element electrocatalysts.

摘要：Fuel cells have attracted extensive attention due to their high conversion efficiency and environmental ***,their wider application is limited by the poor activity and high cost of platinum(Pt),which is widely used as the cathode catalyst to overcome the slow kinetics associated with oxygen reduction reaction(ORR).Pt‐based composites with one‐dimensional(1D)nanoarchitectures demonstrate great advantages towards efficient ORR *** review focuses on the recent advancements in the design and synthesis of 1D Pt‐based ORR *** introducing the fundamental ORR mechanism and the advanced 1D architectures,their synthesis strategies(template‐based and template‐free methods)are ***,their morphology and structure optimization are highlighted,followed by the superstructure assembly using 1D Pt‐based ***,the challenges and perspectives on the synthesis innovation,structure design,physical characterization,and theoretical investigations are proposed for 1D Pt‐based ORR *** anticipate this study will inspire more research endeavors on efficient ORR nanocatalysts in fuel cell application.

摘要：The practical application of high-energy lithium–sulfur battery is plagued with two deadly *** is the“shuttle effect”originated from the sulfur cathode,and the other is the low Coulombic efficiency and security issues arising from the lithium metal *** addressing these issues,we propose a novel silicon-sulfurized poly(acrylonitrile)full *** this lithium metal-free system,the Li source is pre-loaded in the cathode,using a nitrogen evolution reaction(NER)to implant Li+into the silicon/carbon *** poly(acrylonitrile)based on a solid–solid conversion mechanism can fundamentally circumvent the“shuttle effect”.Meanwhile,the silicon/carbon anode can achieve more efficient utiliza-tion and higher security when compared with the Li metal *** full cell used in this technology can deliver a capacity of 1169.3 mAh g^(-1),and it can be stabilized over 100 cycles,implying its excellent elec-trochemical ***,the practical pouch cell with a high sulfur loading of 4.2 mg cm^(-2)can achieve a high specific energy of 513.2 Wh *** mechanism of the NER in cathode has also been investigated and analyzed by in situ ***,this battery design completely conforms to the current battery production technology because of the degassing of gasbag,resulting in a low manufactur-ing *** work will open the avenue to develop a lithium metal-free battery using the NER.

摘要：The development of high‐performance nonprecious metal catalysts(NPMCs)to supersede Pt‐based catalysts for the oxygen reduction reaction(ORR)in polymer electrolyte membrane fuel cells is highly desirable but remains *** this paper,we present a pyrolysis strategy for spatial confinement and active‐site fixation using iron phthalocyanine(FePc),phthalocyanine(Pc)and Zn salts as *** the obtained carbon‐based NPMC with a hierarchically porous nanostructure of thin‐layered carbon nanosheets,nearly 100%of the total Fe species are Fe^(Ⅱ)‐N_(4) active *** contrast,pyrolyzing FePc alone forms Fe‐based nanoparticles embedded in amorphous carbon with only 5.9%Fe^(Ⅱ)‐N_(4) active *** experimental characterization and density functional theory calculations reveal that spatial confinement through the staggeredπ–πstacking of Pc macrocycles effectively prevents the demetallation of Fe atoms and the formation of Fe‐based nanoparticles via ***,Zn‐induced microporous defects allow the fixation of Fe^(Ⅱ)‐N_(4) active *** synergistic effect of staggered stacking confinement and microporous defect fixation results in a high density of atomic Fe^(Ⅱ)‐N_(4) active sites that can enhance the *** optimal Fe^(Ⅱ)‐N_(4)‐C electro‐catalyst outperforms a commercial Pt/C catalyst in terms of half‐wave potential,methanol toler‐ance,and long‐term stability in alkaline *** modulation strategy can greatly advance efforts to develop high‐performance NPMCs.

摘要：Though touted as a potential way to realize clean ammonia synthesis,electrochemical ammonia synthesis is currently limited by its catalytic *** effort has been made to find catalysts with improved activity toward electrochemical nitrogen reduction reaction(eNRR).Rational screening of catalysts can be facilitated using the volcano relationship between catalytic activity and adsorption energy of an intermediate,namely,the activity *** this work,we proposeΔG^(*)_(NH_(2))+ΔG^(*)_(NNH)as a combinatorial descriptor,which shows better predictive power than traditional descriptors using the adsorption free energies of single *** volcano plots based on the combinatorial descriptor exhibits peak activity fixedly at the descriptor value corresponding to the formation free energy of NH3,regardless of the catalyst types;while the descriptor values correspond to the top activities for eNRR on volcano plots based on single descriptors usually vary with the types of catalysts.

摘要：High interfacial energy Li^(0)-electrolyte interface contributes to larger Li^(0) nucleation embryos and a more stable interface,so the interfacial energy is essential for highly reversible Li^(0) deposition/***,a high interfacial-energy artificial solid electrolyte interphase(SEI)with rich LiF embedded in lithiated poly-2-acrylamido-2-methylpropane sulfonic acid(PAMPS-Li)network is designed to realize favorable Li^(0) nucleation and rapid desolvation of Li+*** Li-F bonds in LiF(001)exhibit stronger ion-dipole interactions with Li atoms,offering higher interfacial *** the growth surface energy and total interfacial energy of Li^(0) are balanced,the high interfacial energy SEI with abundant LiF can promote the formation of larger Li^(0) nucleation *** addition,the PAMPS-Li with immobilized anions presents weaker interaction with Li^(0) and possesses higher polymer-Li interfacial energy,and its amide and sulfonic acid groups exhibit higher binding energies with Li^(+).Therefore,PAMPS-Li can easily promote the Li+to escape from the solvent sheath and weaken the desolvation energy *** highly reversible Li^(0) deposition behavior with restricted side reactions is achieved based on the synergistic modification of high interfacial energy SEI with *** importantly,lifespan of multi-layered Li^(0) pouch cell(330 Wh kg-1)with a low N/P ratio(1.67)is over 100 cycles,verifying its potential practical application.

摘要：高熵合金近年来在电催化领域广受关注.由于其四大“核心效应”,即高熵效应、晶格畸变效应、迟滞扩散效应和鸡尾酒效应,高熵合金在诸多电催化反应中展现出了优异的活性和选择性.然而在已报道的文献综述中,有关其优异性能的理解以及合理设计的系统性总结仍然具有局限性.本文不仅综述了高熵合金电催化剂的特点和设计准则,还对其应用的最新进展进行了系统性的归纳整理,对高熵合金未来的发展具有指导意义.首先我们从多个角度阐明了高熵合金作为一种优异电催化剂的原因,包括其出色的机械性能、可优化的结构和组成、大量具有高本征活性的活性位点,以及出色的稳定性.为了进一步深入对高熵合金电催化剂的理解,我们还从设计准则、元素选择,以及理论计算预测材料性质等角度,详细介绍了高熵合金的合理设计.随后,我们介绍了高熵合金电催化剂在电解水、有机小分子氧化、燃料电池和碳/氮基转化反应的最新研究进展,其中还包括了一系列理论计算和原位表征在理解催化反应机理方面的应用.最后,我们展望了高熵合金电催化剂在未来发展中面临的挑战和机遇.

摘要：Alloying and nanostructuring are two strategies used to facilitate the efficient electrocatalysis of the oxygen reduction reaction(ORR)by Pt,where the high index surfaces(HISs)of Pt exhibit superior activity for ***,we report the fabrication of PtCu3 nanodendrites possessing rich spiny branches exposing n(111)×(110)*** dendrites were formed through an etching‐modulated seeding and growing ***,an oxidative atmosphere was initially applied to form the concaved nanocubes of the Pt‐Cu seeds,which was then switched to an inert atmosphere to promote an explosive growth of ***,the oxidative or inert atmosphere failed to produce this hyperbranched *** dealloying of the PtCu3 nanodendrites produced Pt3Cu shells with Pt‐rich surfaces where HIS‐exposed dendrite structures were *** resulting PtCu_(3)@Pt_(3)Cu@Pt nanodendrites in 0.1 M HClO4 exhibited excellent mass and area specific activities for ORR,which were 14 and 24 times higher than that of commercial Pt/C,*** calculations revealed that Cu alloying and HISs both contributed to the significantly enhanced activity of Pt,and that the oxygen binding energy on the step sites of HISs on the PtCu_(3)@Pt_(3)Cu@Pt nanodendrites approached the optimal value to achieve a near peak‐top ORR activity.

摘要：The demanding all-in-one electrocatalyst system for oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in zinc-air batteries or water splitting requires elaborate material manufacturing, which is usually complicated and *** interface engineering between MXene and highly active electrocatalytic species(CoS_(2)) is, herein, achieved by an in situ hydrothermal growth and facile sulfurization *** CoS_(2)@MXene electrocatalyst is composed by one-dimensional CoS_(2) nanowires and two-dimensional MXene nanosheets, which lead to a hierarchical structure(large specific surface area and abundant active sites), a spatial electron redistribution(high intrinsic activity), and high anchoring strength(superior performance stability). Therefore, the electrocatalyst achieves enhanced catalytic activity and longtime stability for ORR(a half-wave potential of 0.80 V), OER(an overpotential of 270 mV at 10 mA cm^(-2), i.e., η10= 270 mV)and HER(η10= 175 mV). Furthermore, the asymmetry water splitting system based on the CoS_(2)@MXene composites delivers a low overall voltage of 1.63 V at 10 mA cm^(-2). The solidstate zinc-air batteries using CoS_(2)@MXene as the air cathode display a small charge-discharge voltage gap(0.53 V at1 mA cm^(-2)) and superior stability(60 circles and 20-h continuous test). The energy interconversion between the chemical energy and electricity can be achieved by a self-powered system via integrating the water splitting system and quasisolid-state zinc-air batteries. Supported by in situ Raman analyses, the formation of cobalt oxyhydroxide species provides the active sites for water oxidation. This study paves apromising avenue for the design and application of multifunctional nanocatalysts.

摘要：Although organic electrode materials have merits of abundant resources,diverse structures and environmental friendliness,their performance for electrochemical energy storage is far *** this work,a thiourea-based polyimide/reduced graphene oxide(PNTCSA/RGO)composite was synthesized via a condensation polymerization *** a cathode material in lithium-ion batteries,excellent performance is demonstrated with high reversible capacity(144.2 mA h g^−1),high discharge voltage(∼2.5 V),and long cycling life(over 2000 cycles at 500 mA g^−1),which are comparable to those of other well documented in organic *** electrochemical performance is also demonstrated for sodium ion batteries(a cycling life of 800 cycles at 500 mA g^−1),while poor performance is delivered in potassium ion *** studies reveal that the active sites are carbonyl groups for all alkali ions but one inserted alkali metal ion is shared by two carbonyl groups from the two neighbor *** importantly,K ions have stronger interaction with S atoms than Li/Na ions,which may lead to poor structure reversibility and account for the poor cycling *** findings provide a fundamental understanding of polyimide based polymer electrodes and help to design and develop high performance organic electrode materials for alkali metal ion batteries.