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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 technologies.However,the relationship between the intrinsic properties of materials such as lattice thermal conductivity and catalysis remains to be explored.In this work,the lattice thermal conductivity of BN and graphene was calculated by Sheng BTE.In 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 TMs.The molecular dynamics(MD)simulation and migration barrier of Ni loaded on BN and graphene were calculated.Our 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

Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction

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Nano Research 2022年第7期15卷 5792-5815页

作者： Peng Zhu Xiang Xiong Dingsheng Wang Department of Chemistry Tsinghua UniversityBeijing 100084China Powder Metallurgy Research Institute and State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China

Hydrogen production from water splitting using renewable electric energy is an interesting topic towards the carbon neutral future.single atom catalysts(SACs)have emerged as a new frontier in the field of catalysis such as hydrogen evolution reaction(HER),owing to their intriguing properties like high activity and excellent chemical selectivity.The catalytic active moiety is often comprised of a single metal atom and its neighboring environment from the supports.Recent published reviews about electricdriven HER tend to classify these SACs by the species of active center atom,nevertheless the influence of their neighboring coordinated atoms from the supports is somehow neglected.Thus we classify the SACs for HER through the type of supports,highlighting the electronic metal–support interaction and their coordination environment from support.Then,we put forward some structural designing strategies including regulating of the central atoms,coordination environments,and metal-support interactions.Finally,the current challenges and future research perspectives of SACs for HER are briefly proposed.

关键词： single atom catalysts coordination environment electrocatalytic hydrogen evolution reaction

Ultrafast synthetic strategies under extreme heating conditions toward single-atom catalysts

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International Journal of Extreme Manufacturing 2022年第3期4卷 49-63页

作者： Guanchao He Minmin Yan Haisheng Gong Huilong Fei Shuangyin Wang State Key Laboratory for Chemo/Biosensing and Chemometrics Advanced Catalytic Engineering Research Centre of the Ministry of Educationand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082People’s Republic of China

Dispersing atomic metals on substrates provides an ideal method to maximize metal utilization efficiency, which is important for the production of cost-effective catalysts and the atomic-level control of the electronic structure. However, due to the high surface energy, individual single atoms tend to migrate and aggregate into nanoparticles during preparation and catalytic operation. In the past few years, various synthetic strategies based on ultrafast thermal activation toward the effective preparation of single-atom catalysts(SACs) have emerged, which could effectively solve the aggregation issue. Here, we highlight and summarize the latest developments in various ultrafast synthetic strategy with rapid energy input by heating shockwave and instant quenching for the synthesis of SACs, including Joule heating, microwave heating, solid-phase laser irradiation, flame-assisted method, arc-discharge method and so on,with special emphasis on how to achieve the uniform dispersion of single metal atoms at high metal loadings as well as the suitability for scalable production. Finally, we point out the advantages and disadvantages of the ultrafast heating strategies as well as the trends and challenges of future developments.

关键词： ultrafast synthesis single atom catalysts extreme conditions Joule heating microwave heating laser irradiation

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 field.Great advance has been obtained in constructing diverse active sites of SACs for improving the performance and understanding the fundamental principles of regulating acid ORR performance.However,the ORR performance of SACs is still unsatisfactory.Importantly,microenvironment adjustment of SACs offers chance to promote the performance of acid ORR.In this review,acid ORR mechanism,attenuation mechanism and performance improvement strategies of SACs are presented.The strategies for promoting ORR activity of SACs include the adjustment of center metal and its microenvironment.The 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 far.We 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 donor.Given the unique ge-ometric and electronic properties of the Co single atoms,the excellent catalytic activity,selectivity and stability were observed.Benefiting 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 ef-fect.Highly 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

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

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中国化学快报:英文版 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 catalysis.The 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 selectivity.In 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 support.Then,characterization technologies for identifying single metal atoms are presented.Besides,the environmental applications including management of harmful gases,water purification are discussed.Finally,future opportunities and challenges for preparation strategies,mechanisms and applications are concluded.We 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

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 materials.However,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 identification.Herein,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 temperature.Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-Nxspecies.Our catalyst shows superior ORR performance with positive half-wave potential(E1/2=0.85 V vs.RHE)in alkaline condition and moderate activity(E1/2=0.68 V vs.RHE)under the acidic condition,excellent methanol tolerance and good long-term stability.All 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

Fe–N–C single atom catalysts for the electrochemical conversion of carbon,nitrogen and oxygen elements

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Materials Reports(Energy) 2022年第3期2卷 22-37页

作者： Jian Huang Qiao Zhang Jie Ding Yueming Zhai The Institute for Advanced Studies Wuhan UniversityWuhan430072China School of Chemical and Biomedical Engineering Nanyang Technological University62 Nanyang DriveSingapore637459Singapore

single atom catalysts(SACs)are constituted by isolated active metal centers,which are heterogenized on inert supports such as graphene,porous carbon,and amorphous carbon.The thermal stability,electronic properties,and catalytic activities of the metal center can be controlled via manipulating the neighboring heteroatoms such as nitrogen,oxygen,and sulfur.Due to the atomical dispersion of the active catalytic centers,the amount of metal required for catalysis can be decreased.Furthermore,new possibilities are offered to easily control the selectivity of a given transformation process as well as to improve turnover frequencies and turnover numbers of target reactions.Among them,Fe–N–C single atom catalysts own special electronic structure,and have been widely used in many fields of electrocatalysis.This review aims to summarize the synthesis of Fe–N–C based on anchoring individual iron atoms on carbon/graphene.The spin-related properties of Fe–N–C catalysts are described,including the relation between spin and electron structure of Fe–N x as well as the coupling between electronic structure of Fe–N x and electronic(orbit)of CO_(2),N_(2)and O_(2).Next,mechanistic investigations conducted to un-derstand the specific behavior of Fe–N–C catalysts are highlighted,including C,N,O electro-reduction.Finally,some issues related to the future developments of Fe–N–C are put forward and corresponding feasible solutions are offered.

关键词： single atom catalysts Fe-N-C synthesis Spin Electrochemical conversion CO_(2)reduction reaction Nitrogen reduction reaction Oxygen reduction reaction

Recent progress of electrochemical reduction of CO_(2)by single atom catalysts

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Materials Reports(Energy) 2022年第3期2卷 3-21页

作者： Tian Wang Jincheng Zhang Fuhua Li Bin Liu Sibudjing Kawi Department of Chemical&Biomolecular Engineering National University of Singapore117585Singapore School of Chemical and Biomedical Engineering Nanyang Technological University637459Singapore

Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic performances.Additionally,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active sites.In this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly summarized.Then,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal sites.As the most popular and efficient coordination modulation strategy,introducing heteroatom was then reviewed.Moreover,as an extension of SACs,the development of dual atom catalysts was also briefly discussed.At last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.

关键词： single atom catalysts CO_(2)reduction reaction Reaction pathways Coordination modulation Dual atom catalysts