期刊
ADVANCED FUNCTIONAL MATERIALS
卷 31, 期 45, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202104377
关键词
carbon aerogels; CO; (2) electroreduction; cross-linked nanostructures; isolated M; -N sites; Zn; -CO; (2) batteries
类别
资金
- National Natural Science Foundation of China [21922811, 21878270, 21961160742]
- Fundamental Research Funds for the Central Universities [2020XZZX002-09]
- Zhejiang Provincial Natural Science Foundation of China [LR19B060002]
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2019R01006]
- Zhejiang Key Laboratory of Marine Materials and Protective Technologies [2020K10]
- Key Laboratory of Marine Materials and Related Technologies, CAS
- Startup Foundation for Hundred-Talent Program of Zhejiang University
Developing highly efficient carbon aerogels with transition metal-nitrogen sites is critical for CO2 electroreduction. An optimal CA/N-Ni aerogel shows exceptional CO2RR activity, achieving a CO FE of 98% at -0.8 V and industrial current density of 300 mA cm(-2). Analysis suggests the rate-determining step in CO2RR is the formation of *COOH intermediate, with CA/N-Ni outperforming other M-N/carbon catalysts.
Developing highly efficient carbon aerogels (CA) electrocatalysts based on transition metal-nitrogen sites is critical for the CO2 electroreduction reaction (CO2RR). However, simultaneously achieving a high current density and high Faradaic efficiency (FE) still remains a big challenge. Herein, a series of unique 3D hierarchical cross-linked nanostructured CA with metal-nitrogen sites (M-N, M = Ni, Fe, Co, Mn, Cu) is developed for efficient CO2RR. An optimal CA/N-Ni aerogel, featured with unique hierarchical porous structure and highly exposed M-N sites, exhibits an unusual CO2RR activity with a CO FE of 98% at -0.8 V. Notably, an industrial current density of 300 mA cm(-2) with a high FE of 91% is achieved on CA/N-Ni aerogel in a flow-cell reactor, which outperforms almost all previously reported M-N/carbon based catalysts. The CO2RR activity of different CA/N-M aerogels can be arranged as Ni, Fe, Co, Mn, and Cu from high to low. In situ spectroelectrochemistry analyses validate that the rate-determining step in the CO2RR is the formation of *COOH intermediate. A Zn-CO2 battery is further assembled with CA/N-Ni as the cathode, which shows a maximum power density of 0.5 mW cm(-2) and a superior rechargeable stability.
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