Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation
Abstract
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.
- Authors:
-
- Tianjin Univ. of Technology (China). Center for Electron Microscopy. Tianjin Key Lab. of Advanced Functional Porous Materials. Inst. for New Energy Materials & Low-Carbon Technologies. School of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Tianjin Univ. of Technology (China). Center for Electron Microscopy. Tianjin Key Lab. of Advanced Functional Porous Materials. Inst. for New Energy Materials & Low-Carbon Technologies. School of Materials Science and Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Univ. of Science and Technology Beijing (China). Dept. of Environmental Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
- Univ. of California, Irvine, CA (United States). Dept. of Physics and Astronomy
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Tianjin Univ. of Technology (China); University of Science and Technology Beijing (China)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); National Program for Thousand Young Talents of China; Tianjin Municipal Science and Technology Commission (China); Tianjin Municipal Education Commission (China); Fundamental Research Fund of Tianjin Univ. of Technology (China)
- OSTI Identifier:
- 1498864
- Alternate Identifier(s):
- OSTI ID: 1491272
- Report Number(s):
- BNL-211355-2019-JAAM
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- SC0012704; 2017YFA0700104; 21601136; 51761165012; 15JCYBJC52600
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 8; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ambient conditions; electrocatalysis; molybdenum; N2 reduction; single-atom catalysis
Citation Formats
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., and Xin, Huolin L. Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation. United States: N. p., 2018.
Web. doi:10.1002/anie.201811728.
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. Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation. United States. https://doi.org/10.1002/anie.201811728
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., and Xin, Huolin L. Wed .
"Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation". United States. https://doi.org/10.1002/anie.201811728. https://www.osti.gov/servlets/purl/1498864.
@article{osti_1498864,
title = {Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation},
author = {Han, Lili and Liu, Xijun and Chen, Jinping and Lin, Ruoqian and Liu, Haoxuan and Lü, Fang and Bak, Seongmin and Liang, Zhixiu and Zhao, Shunzheng and Stavitski, Eli and Luo, Jun and Adzic, Radoslav R. and Xin, Huolin L.},
abstractNote = {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.},
doi = {10.1002/anie.201811728},
journal = {Angewandte Chemie (International Edition)},
number = 8,
volume = 58,
place = {United States},
year = {Wed Dec 12 00:00:00 EST 2018},
month = {Wed Dec 12 00:00:00 EST 2018}
}
Web of Science
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