Journal
ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 11, Pages 12128-12136Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c01656
Keywords
metal-organic frameworks; electrocatalysis; nitrogen reduction reaction; self-supporting electrode; cerium oxide
Funding
- National Natural Science Foundation of China [21971129, 21961022, 21661023]
- China Postdoctoral Science Foundation [2019M663867XB]
- 111 Project [D20033]
- Program of Higher-Level Talents of IMU [21300-5215101]
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The study demonstrated the electrochemical synthesis of ammonia using metal-organic frameworks on a copper mesh substrate. The Ce-MOF underwent structural reconstruction at negative potential and formed catalytically active CeO2, providing insights for the rational design of MOF-based electrocatalysts.
The electrochemical synthesis of ammonia from N2 under mild conditions is a promising alternative to the energy-consuming Haber-Bosch process. Metal-organic frameworks (MOFs) are promising electrocatalysts for the N-2 reduction reaction, but most of them are active for the undesirable and competitive hydrogen evolution reaction. Herein, we developed a facile strategy to grow a Ce-MOF on copper mesh substrate. The Ce-MOF with a self-supporting structure could be directly used as an electrode for the N-2 reduction reaction, demonstrating highly efficient electrocatalytic performance with an NH3 yield of 14.83 mu g h(-1) cm(-2) and a Faradaic efficiency of 10.81% at -0.2 V versus a reversible hydrogen electrode. Structural characterizations of Ce-MOF after electrocatalysis revealed that Ce-MOF as precatalyst underwent structural reconstruction at negative potential, forming catalytically active CeO2 with oxygen vacancies embedded in the amorphous CeMOF. In addition, the self-supporting structure formed by in situ growth of Ce-MOF on porous and conductive cooper mesh endowed the electrocatalyst with enhanced stability, conductivity, and mass transport. This work demonstrated the structural transformation of Ce-MOF during the electrocatalytic process and provided new insight for the rational design of MOF-based electrocatalysts.
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