Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Han, Lili; Liu, Xijun; Chen, Jinping; Lin, Ruoqian; Liu, Haoxuan; Lü, Fang; Bak, Seongmin; Liang, Zhixiu; Zhao, Shunzheng; Stavitski, Eli; Luo, Jun; Adzic, Radoslav R.; Xin, Huolin L.

doi:10.1002/ange.201811728

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Journal Article · Fri Jan 18 00:00:00 EST 2019 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201811728· OSTI ID:1786172

Han, Lili ^[1]; Liu, Xijun ^[2]; Chen, Jinping ^[2]; Lin, Ruoqian ^[3]; Liu, Haoxuan ^[2]; Lü, Fang ^[2]; Bak, Seongmin ^[4]; Liang, Zhixiu ^[4]; Zhao, Shunzheng ^[5]; Stavitski, Eli ^[6]; Luo, Jun ^[2]; Adzic, Radoslav R. ^[4]; ^[7]

Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials Institute for New Energy Materials &, Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China, Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials Institute for New Energy Materials &, Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Chemistry Division Brookhaven National Laboratory Upton NY 11973 USA
Department of Environmental Engineering University of Science and Technology Beijing Beijing 100083 China
National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA
Department of Physics and Astronomy University of California Irvine CA 92697 USA

Abstract

NH ₃ synthesis by the electrocatalytic N ₂ reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen‐doped porous carbon as a cost‐effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH ₃ yield rate (34.0±3.6 μg h ⁻¹ mg _cat. ⁻¹ ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non‐precious‐metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single‐atom non‐precious‐metal catalysts for the electrocatalytic NRR.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0012704

OSTI ID:: 1786172

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 8 Vol. 131; ISSN 0044-8249

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

Country of Publication:: Germany

Language:: English

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