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Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [2];  [3];  [2];  [2];  [4];  [4];  [5];  [6];  [2];  [4];  [7]
  1. 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
  2. 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
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  5. Univ. of Science and Technology Beijing (China). Dept. of Environmental Engineering
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
  7. Univ. of California, Irvine, CA (United States). Dept. of Physics and Astronomy

NH3 synthesis by the electrocatalytic N2 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 here 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 NH3 yield rate (34.0±3.6 μgNH3 h-1 mgcat.-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.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Tianjin Univ. of Technology (China); Univ. of Science and Technology Beijing (China)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Key R&D 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)
Grant/Contract Number:
SC0012704
OSTI ID:
1498864
Alternate ID(s):
OSTI ID: 1491272
Report Number(s):
BNL--211355-2019-JAAM
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 8 Vol. 58; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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