Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst

Gao-Feng Chen, Yifei Yuan, Haifeng Jiang, Shi-Yu Ren, Liang-Xin Ding, Lu Ma, Tianpin Wu, Jun Lu () and Haihui Wang ()
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Gao-Feng Chen: South China University of Technology
Yifei Yuan: Argonne National Laboratory
Haifeng Jiang: South China University of Technology
Shi-Yu Ren: South China University of Technology
Liang-Xin Ding: South China University of Technology
Lu Ma: Argonne National Laboratory
Tianpin Wu: Argonne National Laboratory
Jun Lu: Argonne National Laboratory
Haihui Wang: South China University of Technology

Nature Energy, 2020, vol. 5, issue 8, 605-613

Abstract: Abstract Ammonia (NH3) is essential for modern agriculture and industry and is a potential energy carrier. NH3 is traditionally synthesized by the Haber–Bosch process at high temperature and pressure. The high-energy input of this process has motivated research into electrochemical NH3 synthesis via nitrogen (N2)–water reactions under ambient conditions. However, the future of this low-cost process is compromised by the low yield rate and poor selectivity, ascribed to the inert N≡N bond and ultralow solubility of N2. Obtaining NH3 directly from non-N2 sources could circumvent these challenges. Here we report the eight-electron direct electroreduction of nitrate to NH3 catalysed by copper-incorporated crystalline 3,4,9,10-perylenetetracarboxylic dianhydride. The catalyst exhibits an NH3 production rate of 436 ± 85 μg h−1 cm−2 and a maximum Faradaic efficiency of 85.9% at −0.4 V versus a reversible hydrogen electrode. This notable performance is achieved by the catalyst regulating the transfer of protons and/or electrons to the copper centres and suppressing hydrogen production.

Date: 2020
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DOI: 10.1038/s41560-020-0654-1

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