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Atomically dispersed bimetallic Fe–Co electrocatalysts for green production of ammonia

Shengbo Zhang, Miaomiao Han, Tongfei Shi, Haimin Zhang (), Yue Lin, Xusheng Zheng, Li Rong Zheng, Hongjian Zhou, Chun Chen, Yunxia Zhang, Guozhong Wang, Huajie Yin and Huijun Zhao ()
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Shengbo Zhang: Chinese Academy of Sciences
Miaomiao Han: Huzhou University
Tongfei Shi: Chinese Academy of Sciences
Haimin Zhang: Chinese Academy of Sciences
Yue Lin: University of Science and Technology of China
Xusheng Zheng: University of Science and Technology of China
Li Rong Zheng: Chinese Academy of Sciences
Hongjian Zhou: Chinese Academy of Sciences
Chun Chen: Chinese Academy of Sciences
Yunxia Zhang: Chinese Academy of Sciences
Guozhong Wang: Chinese Academy of Sciences
Huajie Yin: Chinese Academy of Sciences
Huijun Zhao: Griffith University, Gold Coast Campus

Nature Sustainability, 2023, vol. 6, issue 2, 169-179

Abstract: Abstract The dominant Haber–Bosch process to produce ammonia, arguably the most important chemical in support of global food supply, is both energy and carbon intensive, resulting in substantial environmental impacts. Electrocatalytic nitrogen reduction reaction (NRR) powered by renewable electricity provides a green synthetic route for ammonia, but still suffers from insufficient yield rate and Faradaic efficiency. Single-atom electrocatalysts (SACs) have the potential to transform this catalytic process; however, controllable synthesis of SACs with high loading of active sites remains a big challenge. Here we utilize bacterial cellulose with rich oxygen functional groups to anchor iron (Fe) and cobalt (Co), realizing high density, atomically dispersed, bimetallic Fe–Co active sites. For electrocatalytic NRR, our catalyst design delivers a remarkable ammonia yield rate of 579.2 ± 27.8 μg h−1 mgcat.−1 and an exceptional Faradaic efficiency of 79.0 ± 3.8%. The combined theoretical and experimental investigations reveal that the operando change in coordination configuration from [(O-C2)3Fe–Co(O-C2)3] to [(O-C2)3Fe–Co(O-C)C2] is the enabling chemistry. Our findings suggest a general approach to engineer SACs that can drive critical reactions of relevance for sustainability.

Date: 2023
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DOI: 10.1038/s41893-022-00993-7

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