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Electrocatalytic organic transformation reactions in green chemistry: Exploring nanocrystals and single atom catalysts

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Nano Research 2024年第11期17卷 9326-9344页

作者： Ziwei Deng Yuexin Guo Zhiyi Sun Jie Lin Huazhang Zhai Wenxing Chen School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 China School of pharmacy North China University of Science and Technology Tangshan 063210 China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Beijing Institute of Technology Beijing 100081 China Ningbo Institute of Materials Technology and Engineering Chinese Academy of Science Ningbo 315201 China

Organic synthesis chemistry plays a crucial role in supporting social sustainable development and finds widespread applications across various fields. Electrocatalysis, with its benefits of high efficiency, mild reaction conditions, controllability, and environmental friendliness, stands out as one of the most effective strategies for driving the transformation of organic substrates. In recent years, nanocrystals (NCs) and single atom catalysts (SACs) have garnered significant attention in the realm of electrocatalytic organic transformation. This article presents a comprehensive overview of the applications of NCs and SACs in electrocatalytic organic transformation. It delves into advanced catalysts for electrocatalysis of representative substrates, covering both anodic oxidation and cathodic reduction aspects, and addresses their synthesis, characterization, catalytic mechanism, and performance. The ultimate goal of this review is to serve as a valuable reference and a source of inspiration for further exploration into the development of more effective catalysts for electrocatalytic organic transformation.

关键词： single atom catalysts nanocrystals electrocatalysis organic transformation

Preparation of single atom catalysts for high sensitive gas sensing

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International Journal of Extreme Manufacturing 2024年第3期6卷 216-248页

作者： Xinxin He Ping Guo Xuyang An Yuyang Li Jiatai Chen Xingyu Zhang Lifeng Wang Mingjin Dai Chaoliang Tan Jia Zhang Key Laboratory of Microsystems and Microstructure Manufacturing Ministry of EducationHarbin Institute of TechnologyHarbin 150080People’s Republic of China Institute for Frontier Materials Deakin UniversityWaurn Ponds CampusLocked Bag 20000Victoria 3220Australia School of Electrical and Electronic Engineering Nanyang Technological UniversitySingapore 639798Singapore Department of Electrical and Electronic Engineering The University of Hong KongPokfulam RoadHong Kong Special Administrative Region of China 999077People’s Republic of China Chongqing Research Institute Harbin Institute of TechnologyChongqing 401120People’s Republic of China

single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical *** the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive *** this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the *** facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low *** research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing ***,the challenges and future perspectives on the SACs based gas sensing are presented.

关键词： single atom catalysts preparation sensing mechanism gas sensing

Progresses and Prospects of Asymmetrically Coordinated single atom catalysts for Lithium-Sulfur Batteries

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Energy & Environmental Materials 2024年第4期7卷 48-63页

作者： Rong Zhou Shaonan Gu Meng Guo Shuzheng Xu Guowei Zhou Key Laboratory of Fine Chemicals in Universities of Shandong Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China

Lithium-sulfur batteries(LSBs)are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material ***,the practical applications of LSBs are limited by the shuttle effect of lithium polysulfides(LiPSs),electronic insulation of charge and discharge products,and slow LiPSs conversion reaction ***,the introduction of catalysts into LSBs is one of the effective strategy to solve the issues of the sluggished LiPS *** of their nearly 100%atom utilization and high electrocatalytic activity,single-atom catalysts(SACs)have been widely used as reaction mediators for LSBs’***,the SACs with asymmetric coordination structures have exhibited intriguing electronic structures and superior catalytic activities when compared to the traditional M-N_(4)active *** this review,we systematically describe the recent advancements in the installation of asymmetrically coordinated single-atom structure as reactions catalysts in LSBs,including asymmetrically nitrogen coordinated SACs,heteroatom coordinated SACs,support effective asymmetrically coordinated SACs,and bimetallic coordinated *** noteworthy is the discussion of the catalytic conversion mechanism of LiPSs spanning asymmetrically coordinated ***,a perspective on the future developments of asymmetrically coordinated SACs in LSB applications is provided.

关键词： asymmetrical coordination conversion catalysis Li-S batteries shuttle effect single atom catalysts

Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

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Science China Chemistry 2020年第6期63卷 810-817页

作者： Qian He Yuying Meng Hao Zhang Ying Zhang Qingdi Sun Tao Gan Huajian Xiao Xiaohui He Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Institute of Advanced Wear&Corrosion Resistant and Functional Materials Jinan UniversityGuangzhou 510632China Fine Chemical Industry Research Institute School of Chemical Engineering and TechnologySun Yat-sen UniversityZhuhai 519082China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Recently,nitrogen-doped porous carbon supported single atom catalysts(SACs)have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction(ORR)due to their outstanding performance,especially those derived from porphyrin-based ***,most of them involve other metal residuals,which would cause the tedious pre-and/or post-treatment,even mislead the mechanistic investigations and active-site ***,we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin,followed by pyrolysis at high *** characterization results provide the compelling evidence of the dominant presence of atomically dispersed *** catalyst shows superior ORR performance with positive half-wave potential(E1/2=0.85 V ***)in alkaline condition and moderate activity(E1/2=0.68 V ***)under the acidic condition,excellent methanol tolerance and good long-term *** the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.

关键词： single atom catalysts porphyrin precursor-dilution oxygen reduction reaction active site

Structure design and electrochemical properties of carbon-based single atom catalysts in energy catalysis:A review

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Journal of Energy Chemistry 2024年第11期98卷 196-236页

作者： Shuqi Li Xincheng Lu Shuling Liu Jingjing Zhou Yanyan Liu Huanhuan Zhang Ruofan Shen Kang Sun Jianchun Jiang Yongfeng Wang Baojun Li College of Science Henan Agricultural UniversityZhengzhou 450002HenanChina College of Chemistry Zhengzhou UniversityZhengzhou 450001HenanChina Institute of Chemical Industry of Forest Products CAFNational Engineering Lab for Biomass Chemical UtilizationKey and Open Lab on Forest Chemical EngineeringState Forestry AdministrationNanjing 210042JiangsuChina Center for Carbon-based Electronics and Key Laboratory for the Physics and Chemistry of Nanodevices Peking UniversityBeijing 100871China

single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply ***, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of

关键词： Carbon materials Coordination chemistry Defective structure Energy catalysis single atom catalysts

Recent advances in regulating the performance of acid oxygen reduction reaction on carbon-supported non-precious metal single atom catalysts

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Journal of Energy Chemistry 2023年第1期76卷 601-616,I0015页

作者： Yanqiu Wang Jiayu Hao Yang Liu Min Liu Kuang Sheng Yue Wang Jun Yang Jie Li Wenzhang Li School of Chemistry and Chemical Engineering Central South UniversityChangsha 410083HunanChina School of Physics and Electronics Central South UniversityChangsha 410083HunanChina

Developing high performance and low-cost catalysts for oxygen reduction reaction(ORR)in challenging acid condition is vital for proton-exchange-membrane fuel cells(PEMFCs).Carbon-supported nonprecious metal single atom catalysts(SACs)have been identified as potential catalysts in the *** advance has been obtained in constructing diverse active sites of SACs for improving the performance and understanding the fundamental principles of regulating acid ORR ***,the ORR performance of SACs is still ***,microenvironment adjustment of SACs offers chance to promote the performance of acid *** this review,acid ORR mechanism,attenuation mechanism and performance improvement strategies of SACs are *** strategies for promoting ORR activity of SACs include the adjustment of center metal and its *** relationship of ORR performance and structure is discussed with the help of advanced experimental investigations and theoretical calculations,which will offer helpful direction for designing advanced SACs for ORR.

关键词： Oxygen reduction reaction single atom catalysts Microenvironment of center metal Regulation of center metal atoms Electron structure Proton-exchange-membrane fuel cells

Quasi-continuous synthesis of cobalt single atom catalysts for transfer hydrogenation of quinoline

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Chinese Chemical Letters 2022年第5期33卷 2569-2572页

作者： Liyun Huang Hao Zhang Yujie Cheng Qingdi Sun Tao Gan Qian He Xiaohui He Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute of Sun Yat-sen University Huizhou 516216China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China School of Environmental and Chemical Engineering Foshan UniversityFoshan 528000China

Improving the transfer hydrogenation of N-heteroarenes is of key importance for various industrial pro-cesses and remains a challenge so *** reported here a microcapsule-pyrolysis strategy to quasi-continuous synthesis S,N co-doped carbon supported Co single atom catalysts(Co/SNC),which was used for transfer hydrogenation of quinoline with formic acid as the hydrogen *** the unique ge-ometric and electronic properties of the Co single atoms,the excellent catalytic activity,selectivity and stability were *** from the quasi-continuous synthesis method,the as-obtained cata-lysts provide a reference for the large-scale preparation of single atom catalysts without amplification *** catalytic performances and quasi-continuous preparation process,demonstrating a new and promising approach to rational design of atomically dispersed catalysts with maximum atomic efficiency in industrial.

关键词： Quasi-continuous synthesis single atom catalysts Microcapsule Transfer hydrogenation Quinoline

First-principles study of the relationship between the formation of single atom catalysts and lattice thermal conductivity

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Chinese Chemical Letters 2024年第6期35卷 502-506页

作者： Chaozheng He Pei Shi Donglin Pang Zhanying Zhang Long Lin Yingchun Ding Department of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252059China Henan Key Laboratory of Materials on Deep-Earth Engineering School of Materials Science and EngineeringHenan Polytechnic UniversityJiaozuo 454000China School of Materials Science and Engineering Henan Polytechnic UniversityJiaozuo 454000China Department of Basic Medicine North Sichuan Medical CollegeNanchong 637000China

single atom catalysts(SACs)have been in the forefront of catalysts research because of their high efficiency and low cost and provide new ideas for development of renewable energy conversion and storage ***,the relationship between the intrinsic properties of materials such as lattice thermal conductivity and catalysis remains to be *** this work,the lattice thermal conductivity of BN and graphene was calculated by Sheng *** addition,the adsorption properties of 3d-TM(TM=V,Cr,Mn,Fe,Co,Ni)on BN and graphene were investigated using first-principles methods,and it was found that Ni atom can form relatively stable SACs compared to other *** molecular dynamics(MD)simulation and migration barrier of Ni loaded on BN and graphene were *** study found that graphene has higher thermal conductivity and is easier to form SACs than BN,but the SACs formed on BN surface have higher thermodynamic stability.

关键词： First-principles calculation Thermal conductivity single atom catalysts Graphene BN

Preparation and characterization of M_(1)-N_(x)-C_(y)based single atom catalysts for environmental applications

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Chinese Chemical Letters 2023年第8期34卷 130-141页

作者： Xinjiang Hu Daixi Zhou Hui Wang Wenlong Zhang Haoxiang Zhong Yongsheng Chen College of Environmental Science and Engineering Central South University of Forestry and TechnologyChangsha 410004China School of Civil and Environmental Engineering Georgia Institute of TechnologyAtlantaGA 30332United States Georgia Tech Shenzhen Institute Tianjin UniversityShenzhen 518067China

single atom catalysts(SACs)have become the frontier research fields in *** M_(1)-N_(x)-C_(y)based SACs,wherein single metal atoms(M1)are stabilized by N-doped carbonaceous materials,have provided new opportunities for catalysis due to their high reactivity,maximized atomic utilization,and high *** this review,the fabrication methods of M_(1)-N_(x)-C_(y)based SACs via support anchoring strategy and coordination design strategy are summarized to help the readers understand the interaction mechanism of single atoms and ***,characterization technologies for identifying single metal atoms are ***,the environmental applications including management of harmful gases,water purification are ***,future opportunities and challenges for preparation strategies,mechanisms and applications are *** conclude this review by emphasizing the fact that M_(1)-N_(x)-C_(y)based SACs has the potential to become an important candidate for solving current and future environmental pollution problems.

关键词： single atom catalysts Photocatalysis Electrocatalysis Environmental applications