Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host–guest strategy
Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host–guest strategy to fabricate...
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| Published in | Nature chemistry Vol. 12; no. 8; pp. 764 - 772 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
01.08.2020
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host–guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M
1
/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir
1
/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9
A
mg
Ir
−
1
whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10
−3
A
mg
Ir
−
1
). The activity of Ir
1
/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir
1
/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir
1
/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst.
Single-atom catalysts maximize metal atom efficiency and exhibit properties that can be considerably different to their nanoparticle equivalent. Now a general host–guest strategy to make various single-atom catalysts on nitrogen-doped carbon has been developed; the iridium variant electrocatalyses the formic acid oxidation reaction with high mass activity and displays high tolerance to CO poisoning. |
|---|---|
| AbstractList | Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host-guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M1/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir1/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 [Formula: see text] whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10-3 [Formula: see text]). The activity of Ir1/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir1/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir1/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst.Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host-guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M1/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir1/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 [Formula: see text] whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10-3 [Formula: see text]). The activity of Ir1/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir1/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir1/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst. Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host–guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M1/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir1/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 AmgIr−1 whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10−3 AmgIr−1). The activity of Ir1/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir1/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir1/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst.Single-atom catalysts maximize metal atom efficiency and exhibit properties that can be considerably different to their nanoparticle equivalent. Now a general host–guest strategy to make various single-atom catalysts on nitrogen-doped carbon has been developed; the iridium variant electrocatalyses the formic acid oxidation reaction with high mass activity and displays high tolerance to CO poisoning. Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host-guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M /CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir /CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 [Formula: see text] whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10 [Formula: see text]). The activity of Ir /CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir /CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir /CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst. Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host–guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M 1 /CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir 1 /CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 A mg Ir − 1 whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10 −3 A mg Ir − 1 ). The activity of Ir 1 /CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir 1 /CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir 1 /CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst. Single-atom catalysts maximize metal atom efficiency and exhibit properties that can be considerably different to their nanoparticle equivalent. Now a general host–guest strategy to make various single-atom catalysts on nitrogen-doped carbon has been developed; the iridium variant electrocatalyses the formic acid oxidation reaction with high mass activity and displays high tolerance to CO poisoning. |
| Author | Ji, Shufang Li, Yadong Duan, Xiangfeng Zhang, Jian Wang, Dingsheng Li, Ang He, Chun-Ting Chen, Wenxing Xiong, Yu Yao, Tao Fu, Ninghua Chen, Xiao-Ming Gu, Lin Chen, Chen Zhang, Maolin Zhu, Wei Wu, Yuen Wan, Jiawei Zhao, Jie Gong, Yue Hu, Peijun Gao, Xin Zheng, Lirong Wang, Yu Liu, Wei Wei, Shiqiang Peng, Qing Huang, Yu Li, Zhi Chen, Zheng Li, Jun Luo, Jun Xing, Wei Li, Qiheng Dong, Juncai Cheong, Weng-Chon Zhuang, Zhongbin Chen, Yuanjun Peng, Chao Tang, Yan |
| Author_xml | – sequence: 1 givenname: Zhi surname: Li fullname: Li, Zhi organization: Department of Chemistry, Tsinghua University – sequence: 2 givenname: Yuanjun surname: Chen fullname: Chen, Yuanjun organization: Department of Chemistry, Tsinghua University – sequence: 3 givenname: Shufang surname: Ji fullname: Ji, Shufang organization: Department of Chemistry, Tsinghua University – sequence: 4 givenname: Yan surname: Tang fullname: Tang, Yan organization: Department of Chemistry, Tsinghua University – sequence: 5 givenname: Wenxing orcidid: 0000-0001-9669-4358 surname: Chen fullname: Chen, Wenxing organization: Department of Chemistry, Tsinghua University – sequence: 6 givenname: Ang surname: Li fullname: Li, Ang organization: Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology – sequence: 7 givenname: Jie orcidid: 0000-0002-0451-0919 surname: Zhao fullname: Zhao, Jie organization: Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Chemistry Department, School of Chemistry and Molecular Engineering, East China University of Science and Technology – sequence: 8 givenname: Yu orcidid: 0000-0002-9156-0438 surname: Xiong fullname: Xiong, Yu organization: Department of Chemistry, Tsinghua University – sequence: 9 givenname: Yuen orcidid: 0000-0001-9524-2843 surname: Wu fullname: Wu, Yuen organization: Department of Chemistry, University of Science and Technology of China – sequence: 10 givenname: Yue orcidid: 0000-0002-5764-3117 surname: Gong fullname: Gong, Yue organization: Institute of Physics, Chinese Academy of Sciences – sequence: 11 givenname: Tao orcidid: 0000-0001-8699-8294 surname: Yao fullname: Yao, Tao organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 12 givenname: Wei orcidid: 0000-0002-6665-220X surname: Liu fullname: Liu, Wei organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 13 givenname: Lirong surname: Zheng fullname: Zheng, Lirong organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 14 givenname: Juncai orcidid: 0000-0001-8860-093X surname: Dong fullname: Dong, Juncai organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 15 givenname: Yu orcidid: 0000-0002-9071-0238 surname: Wang fullname: Wang, Yu organization: Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences – sequence: 16 givenname: Zhongbin orcidid: 0000-0001-7187-1266 surname: Zhuang fullname: Zhuang, Zhongbin organization: State Key Lab of Organic–Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology – sequence: 17 givenname: Wei surname: Xing fullname: Xing, Wei organization: Laboratory of Advanced Chemical Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Jilin Province Key Laboratory of Low Carbon Chemical Power Sources – sequence: 18 givenname: Chun-Ting surname: He fullname: He, Chun-Ting organization: MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen Unversity – sequence: 19 givenname: Chao orcidid: 0000-0003-3099-2808 surname: Peng fullname: Peng, Chao organization: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, School of Chemistry and Chemical Engineering, Queen’s University Belfast – sequence: 20 givenname: Weng-Chon orcidid: 0000-0002-7684-2808 surname: Cheong fullname: Cheong, Weng-Chon organization: Department of Chemistry, Tsinghua University – sequence: 21 givenname: Qiheng surname: Li fullname: Li, Qiheng organization: Department of Chemistry, Tsinghua University – sequence: 22 givenname: Maolin surname: Zhang fullname: Zhang, Maolin organization: Department of Chemistry, Tsinghua University – sequence: 23 givenname: Zheng surname: Chen fullname: Chen, Zheng organization: Department of Chemistry, Tsinghua University – sequence: 24 givenname: Ninghua surname: Fu fullname: Fu, Ninghua organization: Department of Chemistry, Tsinghua University – sequence: 25 givenname: Xin surname: Gao fullname: Gao, Xin organization: Department of Chemistry, Tsinghua University – sequence: 26 givenname: Wei orcidid: 0000-0002-0317-7229 surname: Zhu fullname: Zhu, Wei organization: Department of Chemistry, Tsinghua University – sequence: 27 givenname: Jiawei surname: Wan fullname: Wan, Jiawei organization: Department of Chemistry, Tsinghua University – sequence: 28 givenname: Jian orcidid: 0000-0001-9275-5790 surname: Zhang fullname: Zhang, Jian organization: Department of Chemistry, Tsinghua University – sequence: 29 givenname: Lin orcidid: 0000-0002-7504-031X surname: Gu fullname: Gu, Lin organization: Institute of Physics, Chinese Academy of Sciences – sequence: 30 givenname: Shiqiang orcidid: 0000-0002-2052-1132 surname: Wei fullname: Wei, Shiqiang organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 31 givenname: Peijun orcidid: 0000-0002-6318-1051 surname: Hu fullname: Hu, Peijun organization: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, School of Chemistry and Chemical Engineering, Queen’s University Belfast – sequence: 32 givenname: Jun orcidid: 0000-0001-5084-2087 surname: Luo fullname: Luo, Jun organization: Center for Electron Microscopy, TUT-FEI Joint Laboratory, Tianjin Key Laboratory of Advanced Functional Porous Materials, Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology – sequence: 33 givenname: Jun orcidid: 0000-0002-8456-3980 surname: Li fullname: Li, Jun organization: Department of Chemistry, Tsinghua University – sequence: 34 givenname: Chen orcidid: 0000-0001-5902-3037 surname: Chen fullname: Chen, Chen organization: Department of Chemistry, Tsinghua University – sequence: 35 givenname: Qing surname: Peng fullname: Peng, Qing organization: Department of Chemistry, Tsinghua University – sequence: 36 givenname: Xiangfeng orcidid: 0000-0002-4321-6288 surname: Duan fullname: Duan, Xiangfeng organization: Department of Chemistry and Biochemistry, University of California, California NanoSystems Institute, University of California – sequence: 37 givenname: Yu orcidid: 0000-0003-1793-0741 surname: Huang fullname: Huang, Yu organization: California NanoSystems Institute, University of California, Department of Materials Science and Engineering, University of California – sequence: 38 givenname: Xiao-Ming orcidid: 0000-0002-3353-7918 surname: Chen fullname: Chen, Xiao-Ming organization: MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen Unversity – sequence: 39 givenname: Dingsheng orcidid: 0000-0003-0074-7633 surname: Wang fullname: Wang, Dingsheng email: wangdingsheng@mail.tsinghua.edu.cn organization: Department of Chemistry, Tsinghua University – sequence: 40 givenname: Yadong orcidid: 0000-0003-1544-1127 surname: Li fullname: Li, Yadong email: ydli@mail.tsinghua.edu.cn organization: Department of Chemistry, Tsinghua University, Department of Chemistry, University of Science and Technology of China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/32541950$$D View this record in MEDLINE/PubMed |
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| ContentType | Journal Article |
| Copyright | The Author(s), under exclusive licence to Springer Nature Limited 2020 The Author(s), under exclusive licence to Springer Nature Limited 2020. |
| Copyright_xml | – notice: The Author(s), under exclusive licence to Springer Nature Limited 2020 – notice: The Author(s), under exclusive licence to Springer Nature Limited 2020. |
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| Snippet | Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional... |
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| SubjectTerms | 639/638/161/886 639/638/298 639/638/77/886 Analytical Chemistry Atom economy Biochemistry Carbon Carbon monoxide Carbon monoxide poisoning Catalysts Chemistry Chemistry and Materials Science Chemistry/Food Science Copper Density functional theory Displays Electronic structure Equivalence First principles Formic acid Inorganic Chemistry Iridium Manganese Molybdenum Nanoparticles Nickel Nitrogen Organic Chemistry Oxidation Palladium Physical Chemistry Platinum Poisoning Properties (attributes) Single atom catalysts Strategy |
| Title | Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host–guest strategy |
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