摘要：The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen-containing ***,we developed an electron catalyzed method to directly fix N_(2)into azos,by pushing and pulling the electron into and from the aromatic halide with the cyclic voltammetry *** round-trip journey of electron can successfully weaken the triple bond in N_(2)through the electron pushing-induced aryl radical via a“brick trowel”transition state,and then produce the diazonium ions by pulling the electron out from the diazo radical *** azos can be synthesized with this developed electron catalyzed *** approach provides a novel concept and practical route for the fixation of N_(2)at atmospheric pressure into chemical products valuable for industrial and commercial applications.

摘要：Electrocatalytic materials with different morphologies,sizes,and components show different catalytic behavior in various heterogeneous catalytic *** has been proved that the catalytic properties of these materials are strongly influenced by several factors at different levels,including the electrode morphology,reaction channels,three-phase interface,and surface active *** developments of mesoscience allow one to study the relationship between the apparent catalytic performance of electro-catalytic materials with these factors from different *** this review,following a brief introduction of new mesoscience,we summarize the effect of mesoscience on electrocatalytic material design,including modulating the geometric and electronic structures of materials focusing on morphology(particulate,fiber,film,array,monolith,and superlattice),pore structure(microporous,mesoporous,and hierarchical),size(single atoms,nanoclusters,and nanoparticles),multiple components(alloys,heterostructures,and multiple ligands),and crystal structures(crystalline,amorphous,and multiple crystal phases).By evaluating the electrocatalytic performance of catalytic materials tuned at the mesoscale,we paint a picture of how these factors at different levels affect the final system performance and then provide a new direction to better understand and design catalytic materials from the viewpoint of mesoscience.

摘要：In the context of the current serious problems related to energy demand and climate change,substantial progress has been made in developing a sustainable energy *** hydrogen-water conversion is an ideal energy system that can produce fuels via sustainable,fossil-free ***,the energy conversion efficiency of two functioning technologies in this energy system—namely,water electrolysis and the fuel cell—still has great scope for *** review analyzes the energy dissipation of water electrolysis and the fuel cell in the hydrogen-water energy system and discusses the key barriers in the hydrogen-and oxygen-involving reactions that occur on the catalyst *** means of the scaling relations between reactive intermediates and their apparent catalytic performance,this article summarizes the frameworks of the catalytic activity trends,providing insights into the design of highly active electrocatalysts for the involved reactions.A series of structural engineering methodologies(including nano architecture,facet engineering,polymorph engineering,amorphization,defect engineering,element doping,interface engineering,and alloying)and their applications based on catalytic performance are then introduced,w让h an emphasis on the rational guidance from previous theoretical and experimental *** key scientific problems in the electrochemical hydrogen-water conversion system are outlined,and future directions are proposed for developing advanced catalysts for technologies with high energy-conversion efficiency.

摘要：Electrochemical water splitting is regarded as the most promising approach to produce ***,the sluggish electrochemical reactions occurring at the anode and cathode,namely,the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),respectively,consume a tremendous amount of energy,seriously hampering its wide ***,single-atom catalysts(SACs)have been proposed to effectively enhance the kinetics of these two *** this minireview,we focus on the recent progress in SACs for OER and HER *** classes of SACs have been reviewed,i.e.,alloy-based SACs,carbon-based SACs and SACs supported on other *** factors affecting the activities of SACs are also highlighted,including the inherent element property,the coordination environment,the geometric structure and the loading amount of metal ***,we summarize the current problems and directions for future development in SACs.

摘要：随着市场竞争的加剧,以产品需求为导向精确定制符合需求的化学品成为化学工程研究发展的探索新方向。电解水制氢是生产高纯氢气并转换储存大规模可再生能源的一种有效方法。为实现高效的电-氢气转换效率,高性能的电解水析氢析氧电极是必不可少的。电解水电极材料具有复杂的化学组成及多层次的结构,其中电极表面催化材料的物理化学性质和形貌结构是决定电解水性能的最主要因素。本文结合本课题组在电解水催化方面的研究工作,综述了近几年国内外电解水电极催化材料的最新研究进展,阐述了电解水电极催化材料以反应机理为导向的催化剂设计理论、以产品性能为导向的催化剂设计方法学(包括纳米结构构筑、晶面调控、载体复合、晶相调节、杂原子掺杂、合金化和聚合物表面修饰)及应用,针对化学产品工程的发展与需要,介绍了电解水电极催化材料跨越分子尺度、微纳结构及合成应用的产品设计和产品工程研究的关键科学问题和发展方向。

摘要：由于快速增长的能源需求和日益紧迫的环境问题,清洁和可再生能源的开发受到全球范围的高度关注.质子交换膜燃料电池(PEMFC)可以直接把燃料所具有的化学能转换为电能,具有转化效率高、环境污染小和比能量高等优点,广泛应用于汽车、飞机等交通工具以及固定电站等领域.PEMFC中阴极侧的氧还原反应(ORR),由于多重质子-电子转移和固有的缓慢动力学,是影响燃料电池整体效率的重要因素.Pt基催化剂由于能够提供较好的催化性能而被认为是较好的阴极材料.然而,广泛使用的Pt基催化剂因成本较高和资源短缺等问题严重阻碍了PEMFC的大规模应用.因此,设计开发非贵金属阴极催化剂对于降低催化剂的成本十分必要.其中,碳基催化剂因具有较好的导电性和化学稳定性,已经成为ORR领域中贵金属催化剂强有力的替代品之一.本文从碳基催化剂的活性位点和孔道结构出发,系统总结和讨论了提高催化剂活性、稳定性和抗中毒性能等方面的研究进展.首先,简单介绍了ORR反应的机理以及碳基催化剂在反应过程中存在的主要问题,即本征活性低,活性位密度低,体积密度小以及稳定性差等.然后,针对以上问题,提出了构筑高活性和高稳定性碳基催化剂的策略.在碳载体中掺杂适量的杂原子和金属原子有助于构建具有高本征活性的催化位点,将金属纳米颗粒设计成原子级和超小纳米团簇有助于增加活性位点的数目.对于目前使用最广泛的Fe-N-C催化剂,从理论上解释了其在酸性介质中活性位点极易失活的主要原因,提出制备具有优异稳定性ORR催化剂的解决方案.孔道结构作为催化剂微观结构的重要组成部分,对活性位点的分布和传质具有十分重要的影响.从合成策略和不同孔径大小对ORR性能影响的两个角度出发,具体论述了现有文献中所报道的制备微孔、介孔和大孔三种孔道结构的方法,同时详细讨论了三种孔结构在ORR中的作用.最后,基于活性位点的设计和多孔结构的构建,对设计和制备高效碳基电催化剂进行了总结,展望了碳基催化剂未来的发展和研究思路.

摘要：Two-dimensional(2D)MXene and single-atom(SA)catalysts are two frontier research fields in catalysis.2D materials with unique geometric and electronic structures can modulate the catalytic performance of supported SAs,which,in turn,affect the intrinsic activity of 2D *** functional theory calculations were used to systematically explore the potential of O-terminated V2C MXene(V_(2)CO_(2))-supported transition metal(TM)SAs,including a series of 3d,4d,and 5d metals,as oxygen reduction reaction(ORR)and hydrogen oxidation reaction(HOR)*** combination of TM SAs and V_(2)CO_(2)changes their electronic structure and enriches the active sites,and consequently regulates the intermediate adsorption energy and catalytic activity for ORR and *** the investigated TM-V_(2)CO_(2)models,Sc-,Mn-,Rh-,and PtMCCh showed high ORR activity,while Sc-,Ti-,V-,Cr-,and Mn-V_(2)CO_(2)exhibited high HOR ***,Mn-and Sc-V_(2)CO_(2)are expected to serve as highly efficient and cost-effective bifunctional catalysts for fuel cells because of their high catalytic activity and *** work provides theoretical guidance for the rational design of efficient ORR and HOR bifunctional catalysts.

摘要：以单质硫为正极的锂硫电池表现出极高的放电比容量(1672 mAh·g^(-1)),是极具潜力的下一代二次动力电池。然而,充放电过程中溶解的高阶多硫化锂(Li_(2)S_(n),4≤n≤8)的穿梭效应,以及硫物种缓慢的氧化还原动力学过程是锂硫电池商业应用前需要解决的关键问题。而电化学催化的引入是解决上述问题行之有效的策略。本文从电化学催化角度出发,重新讨论认识多硫化物的存在形式,并从吸附-催化、活性中间体两个方面,根据不同的反应机理、路径分析多硫化物转化机制,总结定量评价催化性能方法,以期为锂硫电池高效电催化剂的设计提供思路。

摘要：电化学反应器中隔膜材料是将正极和负极在电子通路上隔开但在离子传输通路上保持畅通的特殊材料。作为电化学反应器三个关键材料之一,隔膜材料还需耐强酸/强碱和高电压等环境。围绕电化学反应器中隔膜材料,从分子设计的角度针对材料电化学性能与化学稳定性的调控、电化学装置的介观传质性能的促进和改善等研究思路与进展进行了综述,为相关研究提供性能导向的分子设计参考。

摘要：燃料电池是将化学能转化成电能的装置,其空气电极催化层的设计,既要包含丰富的、易于接近的反应活性位,也要具备高度连通的电子、质子以及反应物、产物传质通道,因此电极必须具有特定三维几何结构形貌和有序分布的各功能化孔道,确保催化活性位得以充分利用以及反应可以连续进行。针对催化剂孔道的几何结构调控,本文调研了最近报道的一系列研究工作,从模板法、高温相变法、模板/相变复合方法以及基于金属有机框架材料进行孔道设计等四种主要方法出发,综述了该领域的最新研究进展。