期刊
ACS APPLIED ENERGY MATERIALS
卷 2, 期 8, 页码 6071-6077出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.9b01135
关键词
N-2 reduction; electrocatalysis; cobalt; nitrogen-doped carbon; metal-organic frameworks
资金
- State Key Laboratory of Organic Inorganic Composites [oic-201503005, oic-201901001]
- Beijing Natural Science Foundation [2192039]
- Beijing University of Chemical Technology [XK180301]
- State Key Laboratory of Separation Membranes and Membrane Processes (Tianjin Polytechnic University) [M2-201704]
Electrochemical N-2 reduction (ENR) provides a potential approach for NH3 synthesis. To facilitate ENR, the development of naturally abundant, cheap, and effective electrocatalysts is critically important. Herein, we report Co/nitrogen-doped carbon composites comprising a large number of single Co sites for efficient N-2 electrofixation at ambient conditions. The N configurations and Co species in the catalysts are readily tunable by controlling the calcination temperatures. Such low-cost catalysts enhanced electrochemical reduction of dinitrogen to ammonia, yielding a maximum ammonia production rate of about 5.1 mu g(NH3) h(-1) mg(cat).(-1) at -0.4 V (vs. the reversible hydrogen electrode, RHE) and a Faradaic efficiency of up to 10.1% at -0.1 V (vs. RHE) in 0.1 M KOH electrolyte. We inferred that single Co atoms together with pyrrolic N may be major active sites for N-2 activation. This work would provide an easy and alternative method for the synthesis of transition-metal catalysts for ENR.
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