Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 8, Issue 35, Pages 13430-13439Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c04021
Keywords
electrocatalytic nitrogen fixation; cobalt coordinated with nitrogen; structure activity relationship; reaction pathway; rate-determining step; Co-N-x active centers
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Funding
- Key Project of the National Ministry of Science and Technology [2016YFC0204204]
- Major Program of the National Natural Science Foundation of China [21590813]
- National Natural Science Foundation of China [21377015, 21677022, 21577012]
- Program of Introducing Talents of Discipline to Universities [B13012]
- Key Laboratory of Industrial Ecology and Environmental Engineering, China Ministry of Education
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Electrocatalytic ammonia (NH3) synthesis under ambient temperature and pressure is an emerging sustainable method for dinitrogen (N-2) fixation, providing a potential environmentally benign pathway for N-2 fixation using renewable power of electricity. However, this strategy is subjected to the low activity of electrocatalysts. In this work, a Co-N-x-C hybrid derived from the metal-organic framework with built-in Co-N-x active sites was fabricated. A high NH3 yield (37.6 mu g mg(-1) h(-1) at -0.9 V vs a reversible hydrogen electrode) and favorable faradaic efficiency (17.6% at -0.3 V vs a reversible hydrogen electrode) were achieved in a 0.05 M H2SO4 electrolyte. The dominating coordination environment of Co-N-x was finally determined by combining X-ray absorption fine structure spectroscopy and theoretical calculation. Co-N-3 demonstrated pivotal active centers that facilitated N-2 adsorption, lowered the free energy of the rate-determining step, inhibited hydrogen evolution reaction, and promoted the N-2 reduction reaction (N2RR). The hierarchical pore structure of catalysts also promoted N-2 adsorption, and the produced high pressure contributed to the further reaction of N-2 fixation. This work also provides a new strategy for developing cost-effective electrocatalytic materials for N2RR.
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