Dong Jianwu, Cheng Ying, Li Ying, Peng Xianyun, Zhang Rui, Wang Hsiao-Tsu, Wang Chunyang, Li Xiaoyan, Ou Pengfei, Pao Chih-Wen, Han Lili, Pong Way-Faung, Lin Zhang, Luo Jun, Xin Huolin L
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China.
Institute for New Energy Materials and Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials and Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.
ACS Appl Mater Interfaces. 2022 Sep 21;14(37):41969-41977. doi: 10.1021/acsami.2c09615. Epub 2022 Sep 7.
Electrochemical conversion of CO to high-value chemical fuels offers a promising strategy for managing the global carbon balance but faces huge challenges due to the lack of effective electrocatalysts. Here, we reported PdCu alloy nanoparticles with abundant exposed (110) facets supported on N-doped three-dimensional interconnected carbon frameworks (PdCu/NC) as an efficient and durable electrocatalyst for electrochemical CO reduction to CO. The catalyst exhibits extremely high intrinsic CO reduction selectivity for CO production with a Faraday efficiency of nearly 100% at a mild potential of -0.5 V. Moreover, a rechargeable high-performance Zn-CO battery with PdCu/NC as a cathode is developed to deliver a record-high energy efficiency of 99.2% at 0.5 mA cm and rechargeable stability of up to 133 h. Theoretical calculations elucidate that the exposed (110) facet over PdCu/NC is the active center for CO activation and rapid formation of the key *COOH intermediate.
将CO电化学转化为高价值化学燃料为管理全球碳平衡提供了一种有前景的策略，但由于缺乏有效的电催化剂而面临巨大挑战。在此，我们报道了负载在氮掺杂三维互连碳框架（PdCu/NC）上具有大量暴露（110）面的PdCu合金纳米颗粒，作为一种高效且耐用的电催化剂用于将电化学CO还原为CO。该催化剂在-0.5 V的温和电位下对CO生成表现出极高的本征CO还原选择性，法拉第效率接近100%。此外，开发了一种以PdCu/NC作为阴极的可充电高性能Zn-CO电池，在0.5 mA cm下可实现创纪录的99.2%的高能效以及高达133 h的可充电稳定性。理论计算表明，PdCu/NC上暴露的（110）面是CO活化和关键*COOH中间体快速形成的活性中心。
