Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Huang, Libei; Cheng, Le; Ma, Tinghao; Zhang, Jun‐Jie; Wu, Haikun; Su, Jianjun; Song, Yun; Zhu, He; Liu, Qi; Zhu, Minghui; Zeng, Zhiyuan; He, Qiyuan; Tse, Man‐Kit; Yang, Deng‐tao; Yakobson, Boris I.; Tang, Ben Zhong; Ren, Yang; Ye, Ruquan

doi:10.1002/adma.202211856

Title: Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Journal Article · 27 April 2023 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202211856 · OSTI ID:1971920

Huang, Libei ^[1]; Cheng, Le ^[2]; Ma, Tinghao ^[3]; Zhang, Jun‐Jie ^[4]; Wu, Haikun ^[2]; Su, Jianjun ^[2]; Song, Yun ^[2]; Zhu, He ^[5]; Liu, Qi ^[5]; Zhu, Minghui ^[6]; Zeng, Zhiyuan ^[7]; He, Qiyuan ^[7]; Tse, Man‐Kit ^[2]; Yang, Deng‐tao ^[3]; Yakobson, Boris I. ^[4]; Tang, Ben Zhong ^[8]; Ren, Yang ^[9];

^[10]

Department of Chemistry State Key Laboratory of Marine Pollution City University of Hong Kong Hong Kong 999077 P. R. China, Division of Science Engineering and Health Study School of Professional Education and Executive Development (PolyU SPEED) The Hong Kong Polytechnic University Hong Kong 999077 P. R. China
Department of Chemistry State Key Laboratory of Marine Pollution City University of Hong Kong Hong Kong 999077 P. R. China
School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an 710072 P. R. China
Department of Materials Science and Nano Engineering and Department of Chemistry Rice University 6100 Main Street Houston TX 77005 USA
Department of Physics City University of Hong Kong Hong Kong 999077 P. R. China
State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 P. R. China
Department of Materials Science and Engineering City University of Hong Kong Hong Kong 999077 P. R. China
School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong Kong Shenzhen Guangdong 518172 P. R. China
Department of Physics City University of Hong Kong Hong Kong 999077 P. R. China, X‐Ray Science Division Argonne National Laboratory 9700 S. Cass Ave. Argonne IL 60439 USA
Department of Chemistry State Key Laboratory of Marine Pollution City University of Hong Kong Hong Kong 999077 P. R. China, City University of Hong Kong Shenzhen Research Institute Shenzhen Guangdong 518057 China

Abstract Ammonia is an indispensable commodity in the agricultural and pharmaceutical industries. Direct nitrate‐to‐ammonia electroreduction is a decentralized route yet challenged by competing side reactions. Most catalysts are metal‐based, and metal‐free catalysts with high nitrate‐to‐ammonia conversion activity are rarely reported. Herein, it is shown that amorphous graphene synthesized by laser induction and comprising strained and disordered pentagons, hexagons, and heptagons can electrocatalyze the eight‐electron reduction of NO ₃ ⁻ to NH ₃ with a Faradaic efficiency of ≈100% and an ammonia production rate of 2859 µg cm ⁻² h ⁻¹ at −0.93 V versus reversible hydrogen electrode. X‐ray pair‐distribution function analysis and electron microscopy reveal the unique molecular features of amorphous graphene that facilitate NO ₃ ⁻ reduction. In situ Fourier transform infrared spectroscopy and theoretical calculations establish the critical role of these features in stabilizing the reaction intermediates via structural relaxation. The enhanced catalytic activity enables the implementation of flow electrolysis for the on‐demand synthesis and release of ammonia with >70% selectivity, resulting in significantly increased yields and survival rates when applied to plant cultivation. The results of this study show significant promise for remediating nitrate‐polluted water and completing the NO _x cycle.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC02-06CH11357

OSTI ID:: 1971920

Alternate ID(s):: OSTI ID: 1983397

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 24 Vol. 35; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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