A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution
Dual-atom catalysts, which exhibit high activity and atom utilization, show promise for sustainable energy conversion and storage technologies. However, the rational design and synthesis of a dual-atom catalyst with structurally homogeneous and flexible active sites remains challenging. In this work...
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| Veröffentlicht in: | Nature Synthesis Jg. 3; H. 7; S. 878 - 890 |
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| Format: | Journal Article |
| Sprache: | Englisch |
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01.07.2024
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| Abstract | Dual-atom catalysts, which exhibit high activity and atom utilization, show promise for sustainable energy conversion and storage technologies. However, the rational design and synthesis of a dual-atom catalyst with structurally homogeneous and flexible active sites remains challenging. In this work, we developed a strategy for the synthesis of a carbon-based catalyst with diatomic Fe–Co sites in which the Fe and Co atoms are coordinated to N and O atoms, respectively, and linked through bridging N and O atoms (FeCo–N3O3@C). The Janus FeCo–N3O3@C quaternary dimer is a stable and efficient bifunctional catalyst in the electrocatalytic oxygen reduction reaction (half-wave potential E1/2 = 0.936 V) and oxygen evolution reaction (potential E = 1.528 V at 10 mA cm−2). When assembled in a Zn–air battery, it exhibits superior performance over a benchmark Pt/C + RuO2 air cathode. A series of ex situ and in situ characterizations, combined with theoretical calculations, revealed that the bifunctional performance of the catalyst originates from the strong coupling of the Fe–N3 and Co–O3 moieties, which alters the d-orbital energy level of the metal atoms, optimizing the adsorption–desorption of oxygenated intermediates and improving the reaction kinetics of the oxygen reduction and evolution reactions. The in-depth insights gained into the fundamental mechanism of this dual-atom catalyst at the atomic and electronic level will facilitate the rational design of further highly efficient multifunctional catalysts with customized activities for specific reactions.The rational design and synthesis of dual-atom catalysts with structurally uniform and flexible active sites remains challenging. Now the tailored synthesis of a Janus Fe–Co dual-metal catalyst is reported in which the Fe and Co atoms are coordinated to N and O, respectively, and linked through bridging N and O atoms. |
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| AbstractList | Dual-atom catalysts, which exhibit high activity and atom utilization, show promise for sustainable energy conversion and storage technologies. However, the rational design and synthesis of a dual-atom catalyst with structurally homogeneous and flexible active sites remains challenging. In this work, we developed a strategy for the synthesis of a carbon-based catalyst with diatomic Fe–Co sites in which the Fe and Co atoms are coordinated to N and O atoms, respectively, and linked through bridging N and O atoms (FeCo–N3O3@C). The Janus FeCo–N3O3@C quaternary dimer is a stable and efficient bifunctional catalyst in the electrocatalytic oxygen reduction reaction (half-wave potential E1/2 = 0.936 V) and oxygen evolution reaction (potential E = 1.528 V at 10 mA cm−2). When assembled in a Zn–air battery, it exhibits superior performance over a benchmark Pt/C + RuO2 air cathode. A series of ex situ and in situ characterizations, combined with theoretical calculations, revealed that the bifunctional performance of the catalyst originates from the strong coupling of the Fe–N3 and Co–O3 moieties, which alters the d-orbital energy level of the metal atoms, optimizing the adsorption–desorption of oxygenated intermediates and improving the reaction kinetics of the oxygen reduction and evolution reactions. The in-depth insights gained into the fundamental mechanism of this dual-atom catalyst at the atomic and electronic level will facilitate the rational design of further highly efficient multifunctional catalysts with customized activities for specific reactions.The rational design and synthesis of dual-atom catalysts with structurally uniform and flexible active sites remains challenging. Now the tailored synthesis of a Janus Fe–Co dual-metal catalyst is reported in which the Fe and Co atoms are coordinated to N and O, respectively, and linked through bridging N and O atoms. |
| Author | Yang, Shuang Hu, Haibo Yan, Wensheng Wang, Dingsheng Zhang, Lei Tan, Hao Wang, Huijuan Wang, Chao Zhuang, Zechao Ji, Qianqian Tang, Bing Zhou, Yanan Weckhuysen, Bert. M. Mei, Bingbao Song, Fei |
| Author_xml | – sequence: 1 givenname: Bing surname: Tang fullname: Tang, Bing – sequence: 2 givenname: Yanan surname: Zhou fullname: Zhou, Yanan – sequence: 3 givenname: Qianqian surname: Ji fullname: Ji, Qianqian – sequence: 4 givenname: Zechao orcidid: 0000-0003-4788-1119 surname: Zhuang fullname: Zhuang, Zechao – sequence: 5 givenname: Lei surname: Zhang fullname: Zhang, Lei – sequence: 6 givenname: Chao orcidid: 0000-0002-3378-6594 surname: Wang fullname: Wang, Chao – sequence: 7 givenname: Haibo orcidid: 0000-0001-7494-1469 surname: Hu fullname: Hu, Haibo – sequence: 8 givenname: Huijuan surname: Wang fullname: Wang, Huijuan – sequence: 9 givenname: Bingbao orcidid: 0000-0003-4195-7151 surname: Mei fullname: Mei, Bingbao – sequence: 10 givenname: Fei orcidid: 0000-0002-6408-7796 surname: Song fullname: Song, Fei – sequence: 11 givenname: Shuang surname: Yang fullname: Yang, Shuang – sequence: 12 givenname: Bert. M. orcidid: 0000-0001-5245-1426 surname: Weckhuysen fullname: Weckhuysen, Bert. M. – sequence: 13 givenname: Hao orcidid: 0000-0001-9221-4871 surname: Tan fullname: Tan, Hao – sequence: 14 givenname: Dingsheng orcidid: 0000-0003-0074-7633 surname: Wang fullname: Wang, Dingsheng – sequence: 15 givenname: Wensheng orcidid: 0000-0001-6297-4589 surname: Yan fullname: Yan, Wensheng |
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