Journal
ACS ENERGY LETTERS
Volume 5, Issue 10, Pages 3237-3243Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c01857
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Funding
- Department of Chemistry and Johns Hopkins University
- Ada Sinz Fellowship from the Department of Chemistry at Hopkins
- DOE Office of Science [DE-AC0206CH11357]
- Materials Research Collaborative Access Team and its member institutions
- International Synchrotron Access Program (ISAP)
- Australian Government
- Research Training Program from the Australian Government
- Scientia PhD Scholarship from UNSW
- U.S. Department of Energy [DE-AC36-08GO28308]
- U.S Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences
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Ammonia is an industrially relevant chemical that can be directly synthesized from water and air using renewable energy through the electrochemical nitrogen reduction reaction (NRR). However, because of the inert nature of nitrogen, current attempts at synthesizing ammonia under aqueous conditions result in low selectivity and yield rates. The poor electrocatalytic performance is mainly attributed to competing hydrogen evolution, underexposed active sites, inadequate electrode contact, and poor stabilization/destabilization of key reaction intermediates. Herein, we present a catalyst composed of MoO2 with surface vacancies dispersed over conductive carbon nanowires that mitigates these obstacles for NRR by providing a high surface area with stable catalytic sites and an underlying conductive support, where a variety of X-ray spectroscopy techniques are used to characterize the MoO2 catalyst. This uniquely engineered catalyst exhibits exceptional Faradaic efficiencies of over 30% and yields of 21.2 mu g h(-1) mg(-1) at a low potential of -0.1 V vs RHE under ambient aqueous conditions.
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