4.8 Article

Amorphous Chromium Oxide with Hollow Morphology for Nitrogen Electrochemical Reduction under Ambient Conditions

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 12, Pages 14474-14481

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c00018

Keywords

amorphous structure; nitrogen reduction reaction; ammonia electrosynthesis; chromium oxide catalyst; metal-organic frameworks; hierarchical porous structure

Funding

  1. National Science Funds for Distinguished Young Scholars [21625401]
  2. National Natural Science Foundation of China [21701086, 21971114]
  3. Jiangsu Provincial Founds for Natural Science Foundation [BK20200090]

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In this study, a hierarchically porous amorphous metal oxide catalyst was constructed, exhibiting superior electrocatalytic performance for NRR under ambient conditions. It has the potential to serve as an alternative electrocatalyst for NH3 synthesis.
The electrocatalytic nitrogen reduction reaction (NRR), an alternative method of nitrogen fixation and conversion under ambient conditions, represents a promising strategy for tackling the energy-intensive issue. The design of high-performance electrocatalysts is one of the key issues to realizing the application of NRR, but most of the current catalysts rely on the use of crystalline materials, and shortcomings such as a limited number of catalytic active sites and sluggish reaction kinetics arise. Herein, an amorphous metal oxide catalyst H-CrOx/C-550 with hierarchically porous structure is constructed, which shows superior electrocatalytic performance toward NRR under ambient conditions (yield of 19.10 mu g h(-1) Mg-cat(-1) and Faradaic efficiency of 1.4% at -0.7 V vs a reversible hydrogen electrode, higher than that of crystalline Cr2O3 and solid counterparts). Notably, the amorphous metal oxide obtained by controlled pyrolysis of metal-organic frameworks (MOFs) possess abundant unsaturated catalytic sites and optimized conductivity due to the controllable degree of metal-oxygen bond reconstruction and the doping of carbon materials derived from organic ligands. This work demonstrates MOF-derived porous amorphous materials as a viable alternative to current electrocatalysts for NH3 synthesis at ambient conditions.

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