Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host-guest strategy.,Nature Chemistry

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Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host-guest strategy.
Nature Chemistry ( IF 21.8 ) Pub Date : 2020-06-15 , DOI: 10.1038/s41557-020-0473-9
Zhi Li ₁ , Yuanjun Chen ₁ , Shufang Ji ₁ , Yan Tang ₁ , Wenxing Chen ₁ , Ang Li ₂ , Jie Zhao ₃ , Yu Xiong ₁ , Yuen Wu ₄ , Yue Gong ₅ , Tao Yao ₆ , Wei Liu ₆ , Lirong Zheng ₇ , Juncai Dong ₇ , Yu Wang ₈ , Zhongbin Zhuang ₉ , Wei Xing _{10,

11} , Chun-Ting He ₁₂ , Chao Peng _{13,

14} , Weng-Chon Cheong ₁ , Qiheng Li ₁ , Maolin Zhang ₁ , Zheng Chen ₁ , Ninghua Fu ₁ , Xin Gao ₁ , Wei Zhu ₁ , Jiawei Wan ₁ , Jian Zhang ₁ , Lin Gu ₅ , Shiqiang Wei ₆ , Peijun Hu _{13,

14} , Jun Luo ₁₅ , Jun Li ₁ , Chen Chen ₁ , Qing Peng ₁ , Xiangfeng Duan _{16,

17} , Yu Huang _{17,

18} , Xiao-Ming Chen ₁₂ , Dingsheng Wang ₁ , Yadong Li _{1,

4}

Affiliation

Department of Chemistry, Tsinghua University, Beijing, China.
Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, China.
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, Shanghai, China.
Department of Chemistry, University of Science and Technology of China, Hefei, China.
Institute of Physics, Chinese Academy of Sciences, Beijing, China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China.
State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
Laboratory of Advanced Chemical Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China.
Jilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun, China.
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen Unversity, Guangzhou, China.
Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai, China.
School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast, UK.
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, Tianjin, China.
Department of Chemistry and Biochemistry, University of California, Los Angeles, CA, USA.
California NanoSystems Institute, University of California, Los Angeles, CA, USA.
Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA.

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 \({{{\rm{A}}\,{\rm{mg}}^{-1}_{{\rm{Ir}}}}}\) whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10⁻³ \({{{\rm{A}}\,{\rm{mg}}^{-1}_{{\rm{Ir}}}}}\)). 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.

中文翻译：

氮掺杂碳上铱单原子催化剂，用于甲酸的氧化，采用一般的主客体策略合成。

单原子催化剂不仅可以最大程度地提高金属原子效率，而且还具有与常规纳米粒子相当的特性，这使其成为一种有前途的研究材料。在这里，我们开发了一种通用的主客体策略，可以在掺氮碳（M ₁ / CN，M = Pt，Ir，Pd，Ru，Mo，Ga，Cu，Ni，Mn）上制造各种金属单原子催化剂。铱变体Ir ₁ / CN电催化甲酸氧化反应，质量活性为12.9 \（{{{\ rm {A}} \，{\ rm {mg}} ^ {-1} _ {{\ rm { Ir}}}}} \），而Ir / C纳米粒子催化剂几乎是惰性的（〜4.8×10 ^-3 \（{{{\ rm {A}} \，{\ rm {mg}} ^ {-1} _ {{\ rm {Ir}}}} \））。Ir ₁的活性/ CN分别比Pd / C和Pt / C大16倍和19倍。此外，Ir ₁ / CN显示出对CO中毒的高耐受性。第一原理密度泛函理论表明，Ir ₁ / CN的性质源于铱位点的空间隔离以及相对于常规纳米粒子催化剂而言铱的修饰电子结构。

更新日期：2020-06-15

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