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| 1 | Single-atom site catalysts for environmental catalysis显示文摘In recent decades,the environmental protection and long-term sustainability have become the focus of attention due to the increasing pollution generated by the intense industrialization.To overcome these issues,environmental catalysis has increasingly been used to solve the negative impact of pollutants emission on the global environment and human health.Supported platinum-metal-group(PGM)materials are commonly utilized as the state-of-the-art catalysts to eliminate gaseous pollutants but large quantities of PGMs are required.By comparison,single-atom site catalysts(SACs)have attracted much attention in catalysis owing to their 100%atom efficiency and unique catalytic performances towards various reactions.Over the past decade,we have witnessed burgeoning interests of SACs in heterogeneous catalysis.However,to the best of our knowledge,the systematic summary and analysis of SACs in catalytic elimination of environmental pollutants has not yet been reported.In this paper,we summarize and discuss the environmental catalysis applications of SACs.Particular focus was paid to automotive and stationary emission control,including model reaction(CO oxidation,NO reduction and hydrocarbon oxidation),overall reaction(three-way catalytic and diesel oxidation reaction),elimination of volatile organic compounds(formaldehyde,benzene,and toluene),and removal/decomposition of other pollutants(Hg0 and SO3).Perspectives related to further challenges,directions and design strategies of single-atom site catalysts in environmental catalysis were also provided. | Ningqiang Zhang Chenliang Ye Han Yan Lingcong Li Hong He Dingsheng Wang Yadong Li | 2020 | Nano Research2020，13，12： | 38 |
| 2 | Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline显示文摘Single-atom site(SA)catalysts on N-doped carbon(CN)materials exhibit prominent performance for their active sites being M-Nx.Due to the commonly random doping behaviors of N species in these CN,it is a tough issue to finely regulate their doping types and clarify their effect on the catalytic property of such catalysts.Herein,we report that the N-doping type in CN can be dominated as pyrrolic-N and pyridinic-N respectively through compounding with different metal oxides.It is found that the proportion of distinct doped N species in CN depends on the acidity and basicity of compounded metal oxide host.Owing to the coordination by pyrrolic-N,the SA Cu catalyst displays an enhanced activity(two-fold)for transfer hydrogenation of quinoline to access the valuable molecule tetrahydroquinoline with a good selectivity(99%)under mild conditions.The higher electron density of SA Cu species induced by the predominate pyrrolic-N coordination benefits the hydrogen transfer process and reduces the energy barrier of the hydrogenation pathway,which accounts for the improved catalytic effeciency. | Jian Zhang Caiyan Zheng Maolin Zhang Yajun Qiu Qi Xu Weng-Chon Cheong Wenxing Chen Lirong Zheng Lin Gu Zhengpeng Hu Dingsheng Wang Yadong Li | 2020 | Nano Research2020，13，11： | 29 |
| 3 | Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene显示文摘The oxidation of hydrocarbons to produce high value-added compounds(ketones or alcohols)using oxygen in air as the only oxidant is an efficient synthetic strategy from both environmental and economic views.Herein,we successfully synthesized cobalt single atom site catalysts(Co SACs)with high metal loading of 23.58 wt.%supported on carbon nitride(CN),which showed excellent catalytic properties for oxidation of ethylbenzene in air.Moreover,Co SACs show a much higher turn-over frequency(19.6 h^(−1))than other reported non-noble catalysts under the same condition.Comparatively,the as-obtained nanosized or homogenous Co catalysts are inert to this reaction.Co SACs also exhibit high selectivity(97%)and stability(unchanged after five runs)in this reaction.DFT calculations reveal that Co SACs show a low energy barrier in the first elementary step and a high resistance to water,which result in the robust catalytic performance for this reaction. | Yu Xiong Wenming Sun Yunhu Han Pingyu Xin Xusheng Zheng Wensheng Yan Juncai Dong Jian Zhang Dingsheng Wang Yadong Li | 2021 | Nano Research2021，14，7： | 20 |
| 4 | Understanding the structure–performance relationship of active sites at atomic scale显示文摘Metal-based atomically dispersed catalysts have attracted more attention because of their excellent catalytic performance and nearly 100%atom utilization.Therefore,it is very important to comprehensively and systematically understand the relationship between catalytic active sites and catalytic performance at atomic scale.Here,we discuss and summarize in detail the key and fundamental factors affecting the active site,and relate them to the catalytic performance.First,we describe the effectiveness of active site design by coordination effects.Then,the role of chemical bonds in the active sites in changing the reaction performance is discussed.In addition,for intermetallic compounds,we explore how the spacing of active atoms affects the catalytic behavior.Moreover,the importance of synergistic effect in catalyst design is further discussed.Finally,the key parameters affecting the catalytic performance at atomic scale are summarized,and the main challenges and development prospects of atomic catalysts in the future are put forward. | Runze Li Dingsheng Wang | 2022 | Nano Research2022，15，8： | 13 |
| 5 | Fe_(1)N_(3)结构单原子Fe催化剂在硝基苯加氢和转移加氢中的优异性能显示文摘设计性能优异的硝基化合物选择性加氢或转移加氢生成胺类的非贵金属多相催化剂具有重要的意义,但又具有很大的挑战性.本文报道了氮掺杂碳负载的单原子Fe催化剂(Fe_(1)/N-C).通过调控温度,Fe_(1)/N-C催化剂对硝基苯的选择性加氢和转移加氢均具有良好的催化性能.DFT计算表明,Fe_(1)/N-C在较低温度下能够很好地活化反应物和中间体,因此具有较高的选择性加氢活性.此外,Fe_(1)/N-C在较高温度下可以克服异丙醇脱氢反应的能量障碍,因此具有很好的转移加氢性能. | 田书博 胡敏 徐琪 龚万兵 陈文星 杨嘉睿 朱有奇 陈春 何佳 刘强 赵惠军 王定胜 李亚栋 | 2021 | Science China Materials2021，64，3： | 9 |
| 6 | Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis显示文摘Supported atomically dispersed metal catalysts(ADMCs)have received enormous attention due to their high atom utilization efficiency,mass activity and excellent selectivity.Single-atom site catalysts(SACs)with monometal-center as the quintessential ADMCs have been extensively studied in the catalysis-related fields.Beyond SACs,novel atomically dispersed metal catalysts(NADMCs)with flexible active sites featuring two or more catalytically centers including dual-atom and triple-atom catalysts have drawn ever-increasing attention recently.Owing to the presence of multiple neighboring active sites,NADMCs could exhibit much higher activity and selectivity compared with SACs,especially in those complicated reactions with multi-step intermediates.This review comprehensively outlines the recent exciting advances on the NADMCs with emphasis on the deeper understanding of the synergistic interactions among multiple metal atoms and underlying structure-performance relationships.It starts with the systematical introduction of principal synthetic approaches for NADMCs highlighting the key issues of each fabrication method including the atomically precise control in the design of metal nuclearity,and then the state-of-the-art characterizations for identifying and monitoring the atomic structure of NADMCs are explored.Thereafter,the recent development of NADMCs in energy-related applications is systematically discussed.Finally,we provide some new insights into the remaining challenges and opportunities for the development of NADMCs. | Xiaobo Zheng Beibei Li Qishun Wang Dingsheng Wang Yadong Li | 2022 | Nano Research2022，15，9： | 9 |
| 7 | Electrochemical conversion of CO2 to syngas with a wide range of CO/H2 ratio over Ni/Fe binary single-atom catalysts显示文摘A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method.Depending on the Ni/Fe content,they exhibit a wide-range of controllable CO/H2 ratio from 0.14 to 10.86,which is meaningful to specific chemical processes.The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity.The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO2 reduction reactions. | Meng Zhang Zheng Hu Lin Gu Qinghua Zhang Linghui Zhang Qian Song Wei Zhou Shi Hu | 2020 | Nano Research2020，13，12： | 8 |
| 8 | Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium-sulfur batteries显示文摘Lithium-sulfur(Li-S)batteries are considered as a highly promising energy storage system due to their ultrahigh theoretical energy density.However,the sluggish kinetics of the complex multi-electron sulfur redox reactions seriously hinders the actual battery performance especially under practical working conditions.Homogeneous redox mediation,through elaborately designing the additive molecules,is an effective approach to promote the sulfur redox kinetics.Herein a promoter of mixed organodiselenides(mixed-Se)is proposed to comprehensively improve the sulfur redox kinetics following the redox comediation principles.Concretely,diphenyl diselenide promotes the liquid-liquid conversion between polysulfides and the solid-liquid conversion regarding lithium sulfide oxidation to polysulfides,while dimethyl diselenide enhances the liquid-solid conversion regarding lithium sulfide deposition.Consequently,the mixed-Se promoter endows a high discharge capacity of 1002 mAh g^(−1)with high sulfur loading of 4.0 mg cm^(−2),a high capacity retention of 81.6%after 200 cycles at 0.5 C,and a high actual energy density of 384 Wh kg^(−1)at 0.025 C in 1.5 Ah-level Li-S pouch cells.This work affords an effective kinetic promoter to construct high-energy-density Li-S batteries and inspires molecular design of kinetic promoters toward targeted energy-related redox reactions. | Meng Zhao Xi-Yao Li Xiang Chen Bo-Quan Li Stefan Kaskel Qiang Zhang Jia-Qi Huang | 2021 | eScience2021，1，1： | 8 |
| 9 | Rapid, high-efficient and scalable exfoliation of high-quality boron nitride nanosheets and their application in lithium-sulfur batteries显示文摘Boron nitride nanosheets(BNNSs)have gained significant attraction in energy and environment fields because of their two-dimensional(2D)nature,large band gap and high thermal/mechanical performance.However,the current low production efficiency of high-quality BNNSs is still a bottleneck limiting their applications.Herein,based on sonication-assisted liquid-phase exfoliation,we demonstrated a rapid,high-efficient and scalable production strategy of BNNSs and documented the effects of a spectrum of exfoliation factors(e.g.,ultrasonic condition,solvent and bulk material feeding)on the yield of BNNSs.A record of yield of 72.5%was achieved while the exfoliated BNNSs have few-layer and defect-free feature.Thanks to the Lewis acid sites of the boron atoms,the BNNSs can interact with the polysulfide anions in liquid electrolyte and also can facilitate the uniform lithium deposition,which finally endow a lithium-sulfur(Li-S)battery with long life.This work provides a facile and rapid strategy for large scale preparation of high-quality BNNSs,also contributes a long-life strategy for dendrite-free Li-S battery,opens new avenues of BNNSs in energy application. | Yu Chen Qi Kang Pingkai Jiang Xingyi Huang | 2021 | Nano Research2021，14，7： | 7 |
| 10 | 石墨烯及其复合材料在锂硫电池中抑制穿梭效应的应用进展显示文摘硫锂电池具有比能高达1675 mAh g^(−1)、价格低廉、环保等优点,是一种具有良好应用前景的二次电池。但由于放电过程中多硫化物溶解产生的穿梭效应、硫的绝缘和硫电极的体积膨胀等原因导致锂硫电池的循环稳定性还不能满足工业化要求。石墨烯具有优异的导电性、超大的比表面积、良好的机械柔韧性和热化学稳定性,因此石墨烯及其衍生物成为全固态锂硫电池电极和改性隔膜的重要材料。本文综述了在全固态锂硫电池中,石墨烯的网络结构对电子转移非常有利,可以限制硫电极体积膨胀并促进离子迁移;同时作为改性隔膜的首选材料之一,石墨烯及其衍生物的六边形层状结构形成的锂离子输运通道能够捕获硫。总结了石墨烯及其衍生物抑制穿梭效应的机制,提出了石墨烯在锂硫电池中的发展策略和前景。 | 李丽波 单宇航 | 2021 | 新型炭材料2021，36，2： | 6 |
| 11 | Atomic Fe-Zn dual-metal sites for high-efficiency pH-universal oxygen reduction catalysis显示文摘An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction(ORR)is crucial for energy conversion and storage devices.However,most of the high-efficiency ORR catalysis was reported in alkaline conditions.Herein,we demonstrated the preparation of atomically dispersed Fe-Zn pairs anchored on porous N-doped carbon frameworks(Fe-Zn-SA/NC),which works efficiently as ORR catalyst in the whole pH range.It achieves high half-wave potentials of 0.78,0.85 and 0.72 V in 0.1 M HClO4,0.1 M KOH and 0.1 M phosphate buffer saline(PBS)solutions,respectively,as well as respectable stability.The performances are even comparable to Pt/C.Furthermore,when assembled into a Zn-air battery,the high power density of 167.2 mWcm−2 and 120 h durability reveal the feasibility of Fe-Zn-SA/NC in real energy-related devices.Theoretical calculations demonstrate that the superior catalytic activity of Fe-Zn-SA/NC can be contributed to the lower energy barriers of ORR at the Fe-Zn-N6 centers.This work demonstrates the potential of Fe-Zn pairs as alternatives to the Pt catalysts for efficient catalytic ORR and provides new insights of dual-atom catalysts for other energy conversion related catalytic reactions. | Jie Xu Shuhua Lai Defeng Qi Min Hu Xianyun Peng Yifan Liu Wei Liu Guangzhi Hu Heng Xu Fan Li Chao Li Jia He Longchao Zhuo Jiaqiang Sun Yuan Qiu Shusheng Zhang Jun Luo Xijun Liu | 2021 | Nano Research2021，14，5： | 6 |
| 12 | Recent advances in anode materials for potassium-ion batteries:A review显示文摘Potassium-ion batteries(PIBs)are appealing alternatives to conventional lithium-ion batteries(LIBs)because of their wide potential window,fast ionic conductivity in the electrolyte,and reduced cost.However,PIBs suffer from sluggish K+reaction kinetics in electrode materials,large volume expansion of electroactive materials,and the unstable solid electrolyte interphase.Various strategies,especially in terms of electrode design,have been proposed to address these issues.In this review,the recent progress on advanced anode materials of PIBs is systematically discussed,ranging from the design principles,and nanoscale fabrication and engineering to the structure-performance relationship.Finally,the remaining limitations,potential solutions,and possible research directions for the development of PIBs towards practical applications are presented.This review will provide new insights into the lab development and real-world applications of PIBs. | Lianbo Ma Yaohui Lv Junxiong Wu Chuan Xia Qi Kang Yizhou Zhang Hanfeng Liang Zhong Jin | 2021 | Nano Research2021，14，12： | 6 |
| 13 | Porous γ-Fe_(2)O_(3) nanoparticle decorated with atomically dispersed platinum: Study on atomic site structural change and gas sensor activity evolution显示文摘Decorating semi-conducting metal oxide with noble metal has been recognized as a viable approach to improve the sensitivity of gas sensor. However, conventional method which relys on noble metal nanoparticles is confronted with drawback of significantly increased cost. To maximize the atom efficiency and reduce the cost for practical industrial application, designing sensor material with noble metal isolated single atom sites (ISAS) doping is a desired option. Here, we report an atomically dispersed platinum on one-dimensional arranged porous γ-Fe2O3 nanoparticle composites as highly efficient ethanol gas sensor. The optimized sample (Pt1-Fe2O3-ox) exhibited a high response (Ra/Rg = 102.4) and good selectivity to ethanol gas. It is demonstrated only the Pt single atom sites with high valance can effectively promote the adsorption capacity to ethanol and consequently enhance the sensitivity of sensing process by changing the electrical structure of Fe2O3 support. This work indicates the single atom sites could play a vital role in improving the performance of conventional metal oxides gas sensors and pave way for the exploration of ISAS-enhanced gas sensor for other volatile organic compounds (VOCs). | Qiheng Li Zhi Li Qinghua Zhang Lirong Zheng Wensheng Yan Xiao Liang Lin Gu Chen Chen Dingsheng Wang Qing Peng Yadong Li | 2021 | Nano Research2021，14，5： | 5 |
| 14 | Pd单原子整体催化剂:功能化的三维结构和优异的化学加氢选择性显示文摘原子级别调控催化剂在选择性加氢反应中的选择性是一个巨大的挑战.在本文中,我们报告了一种简单实用的策略,用于合成Pd单原子负载在氮掺杂碳纳米泡沫(Pd-SAs/CNF)上的整体型单原子催化剂.此外,我们证明独特电子结构的单原子Pd位点使得PdSAs/CNF产生孤立位点效应,进而导致在4-硝基苯基乙炔半氢化反应中具有出色的活性和选择性.此外,得益于较高的完整性和良好的机械强度,整体型Pd-SAs/CNF催化剂易与反应体系分离,进一步有利于回收循环利用.循环测试表明,整体型Pd-SAs/CNF催化剂具有优异的可重复使用性和稳定性.孤立位点效应的发现为设计高选择性催化剂提供了一种新方法.整体式单原子催化剂的研究为推进单原子催化剂的实际应用提供了新的机会. | 张泽栋 周敏 陈远均 柳守杰 王海丰 张剑 冀淑方 王定胜 李亚栋 | 2021 | Science China Materials2021，64，8： | 5 |
| 15 | Use of rare earth elements in single-atom site catalysis:A critical review——Commemorating the 100th anniversary of the birth of Academician Guangxian Xu显示文摘Rare earth metals are strategic resources with potential applications in optics,metallurgy and catalysis.In recent years,single-atom site catalysts(SASCs) have attracted increasing attention owing to their 100%atom efficiency and unique catalytic performances.Over the past decade,rare earth elements,including rare earth metals and their oxides,have shown great potential in SASCs.However,systematic analyses of data are still handful.In this mini-review,the use of rare earth metals and their oxides in SASCs was summarized and the results are discussed.A particular focus was paid to the synthetic strategies,characterization of rare earth-containing SASCs,and applications as catalysis supports,promoters and active sites.Current issues faced by rare-earth metals and their oxides in SASCs,as well as future prospects were also provided. | Ningqiang Zhang Han Yan Lingcong Li Rui Wu Liyun Song Guizhen Zhang Wenjun Liang Hong He | 2021 | Journal of Rare Earths2021，39，3： | 4 |
| 16 | Low‐dimensional material supported single‐atom catalysts for electrochemical CO_(2) reduction显示文摘Converting CO_(2) emissions to valuable carbonaceous chemicals/fuels under mild conditions provides a sustainable way to maintain carbon balance and alleviate the energy shortage.Low‐dimensional material(LDM)supported single‐atom catalysts(SACs)have been attracted significant attention for electrochemical CO_(2) reduction reaction(ECR)in recent years.This is mainly because integrating the single‐atoms and LDMs can inherit the advantages of themselves and the synergy effects between them are potential to enhance the ECR performance.In this review,we summarized the strategies for synthesizing LDM supported SACs for ECR,and different LDM supported SACs for ECR have been briefly introduced.Moreover,some optimization strategies for LDM supported SACs towards CO_(2) electroreduction are highlighted.At the end of this review,the perspectives and challenges of LDM supported SACs for ECR are provided. | Bingqing Wang Shenghua Chen Zedong Zhang Dingsheng Wang | 2022 | SmartMat2022，3，1： | 4 |
| 17 | Effect of Zn atom in Fe-N-C catalysts for electro-catalytic reactions: theoretical considerations显示文摘Due to the high specific surface area,abundant nitrogen and micropores,ZIF-8 is a commonly used precursor for preparing high performance Fe-N-C catalysts.However,the Zn element is inevitably remained in the prepared Fe-N-C catalyst.Whether the residual Zn element affects the catalytic activity and active site center of the Fe-N-C catalyst caused widespread curiosity,but has not been studied yet.Herein,we built several Fe,Zn,and N co-doped graphene models to investigate the effect of Zn atoms on the electrocatalytic performance of Fe-N-C catalysts by using density functional theory method.The calculation results show that all the calculated Fe-Zn-N_(x) structures are thermodynamically stable due to the negative formation energies and relative stabilities.The active sites around Fe and Zn atoms in the structure of Fe-Zn-N_(6)(III)show the lowest oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)overpotentials of 0.38 and 0.43 V,respectively.The bridge site of Fe-Zn in Fe-Zn-N_(5) shows the lowest η^(HER) of−0.26 V.A few structures with a better activity than that of FeN_(4) or ZnN_(4) are attributed to the synergistic effects between Fe and Zn atoms.The calculated ORR reaction pathways on Fe-Zn-N6(III)show that H_(2)O is the final product and the ORR mechanism on the catalyst would be a four-electron process,and the existence of Zn element in the Fe-N-C catalysts plays a key role in reducing the ORR activation energy barrier.The results are helpful for the deep understand of high-performance Fe-N-C catalysts. | Yongcheng Li Riming Hu Zhibin Chen Xin Wan Jia-Xiang Shang Fu-He Wang Jianglan Shui | 2021 | Nano Research2021，14，3： | 3 |
| 18 | Rational design of palladium single-atoms and clusters supported on silicoaluminophosphate-31 by a photochemical route for chemoselective hydrodeoxygenation of vanillin显示文摘Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals.Herein,we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31(SAPO-31)as a highly active,chemoselective,and reusable catalyst for hydrodeoxygenation of vanillin.Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy,extended X-ray absorption fine structure measurement,and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed,without forming strong palladium-palladium metallic bonding,over the SAPO-31 support.This catalyst,with a full metal availability to the reactants,exhibits exceptional catalytic activity(TOF:3,000 h^(−1),Yield:>99%)in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol(MMP)under mild conditions(1 atm,80°C,30 min),along with excellent stability,scalability(up to 100-fold),and wide substrate scope.The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters,as well as the strong metal-support interactions.This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities. | Xiaowen Lu Chunmu Guo Mingyang Zhang Leipeng Leng J.Hugh Horton Wei Wu Zhijun Li | 2021 | Nano Research2021，14，11： | 3 |
| 19 | High-throughput screening of carbon-supported single metal atom catalysts for oxygen reduction reaction显示文摘Carbon-supported transition metal single atoms are promising oxygen reduction reaction(ORR)electrocatalyst.Since there are many types of carbon supports and transition metals,the accurate prediction of the components with high activity through theoretical calculations can greatly save experimental time and costs.In this work,the ORR catalytic properties of 180 types single-atom catalysts(SACs)composed of the eight representative carbon-based substrates(graphdiyne,C_(2)N,C_(3)N_(4),phthalocyanine,C-coordination graphene,N-coordination graphene,covalent organic frameworks and metal-organic frameworks)and 3d,4d,and 5d transition metal elements are investigated by density functional theory(DFT).The adsorption free energy of OH^(*) is proved a universal descriptor capable of accurately prediction of the ORR catalytic activity.It is found that the oxygen reduction reaction overpotentials of all the researched SACs follow one volcano shape very well with the adsorption free energy of OH^(*).Phthalocyanine,N-coordination graphene and metal-organic frameworks stand out as the promising supports for single metal atom due to the relatively lower overpotentials.Notably,the Co-doped metal-organic frameworks,Ir-doped phthalocyanine,Co-doped N-coordination graphene,Co-doped graphdiyne and Rh-doped phthalocyanine show extremely low overpotentials comparable to that of Pt(111).The study provides a guideline for design and selection of carbon-supported SACs toward oxygen reduction reaction. | Yiran Wang Riming Hu Yongcheng Li Fuhe Wang Jiaxiang Shang Jianglan Shui | 2022 | Nano Research2022，15，2： | 2 |
| 20 | Simultaneous diffusion of cation and anion to access N,S cocoordinated Bi-sites for enhanced CO_(2) electroreduction显示文摘Developing highly active single-atom sites catalysts for electrochemical reduction of CO_(2) is an effective and environmental-friendly strategy to promote carbon-neutral energy cycle and ameliorate global climate issues.Herein,we develop an atomically dispersed N,S co-coordinated bismuth atom sites catalyst(Bi-SAs-NS/C)via a cation and anion simultaneous diffusion strategy for electrocatalytic CO_(2) reduction.In this strategy,the bonded Bi cation and S anion are simultaneously diffused into the nitrogen-doped carbon layer in the form of Bi2S3.Then Bi is captured by the abundant N-rich vacancies and S is bonded with carbons.support at high temperature,formed the N,S co-coordinated Bi sites.Benefiting from the simultaneous diffusion of Bi and S,different electronegative N and S can be effectively co-coordinated with Bi,forming the uniform Bi-N_(3)S/C sites.The synthesized.Bi-SAs-NS/C exhibits a high selectivity towards CO with over 88%Faradaic efficiency in a wide potential range,and achieves a maximum FE_(CO)of 98.3%at-0.8 V vs.RHE with a current density of 10.24 mA·cm^(-2),which can keep constant with negligible degradation in 24 h continuous electrolysis.Experimental results and theoretical calculations reveal that the significantly improved catalytic performance of Bi-SAs-NS/C than Bi-SAs-N/C is ascribed to the replacement of one coordinated-N with low electronegative S in Bi-N_(4)C center,which can greatly reduce the energy barrier of the intermediate formation in rate-limiting step and increase the reaction kinetics.This work provides an effective strategy for rationally designing highly active single-atom sites;catalysts for efficient electrocatalysis with optimized electronic structure. | Zhiyuan Wang Chun Wang Yidong Hu Shuai Yang Jia Yang Wenxing Chen Huang Zhou Fangyao Zhou Lingxiao Wang Junyi Du Yafei Li Yuen Wu | 2021 | Nano Research2021，14，8： | 2 |
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