期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 12, 页码 4914-4919出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201916520
关键词
cobalt nanoparticles; in situ XANES; nitrogen-doped carbon materials; phthalocyanine; pyridinic nitrogen
资金
- National Key Research and Development Program of China [2016YFB0101202]
- National Natural Science Foundation of China [91645123, 21773263]
Nitrogen-doped carbon materials (N-C-mat) are emerging as low-cost metal-free electrocatalysts for the electrochemical CO2 reduction reaction (CO2RR), although the activities are still unsatisfactory and the genuine active site is still under debate. We demonstrate that the CO2RR to CO preferentially takes place on pyridinic N rather than pyrrolic N using phthalocyanine (Pc) and porphyrin with well-defined N-C-mat configurations as molecular model catalysts. Systematic experiments and theoretic calculations further reveal that the CO2RR performance on pyridinic N can be significantly boosted by electronic modulation from in-situ-generated metallic Co nanoparticles. By introducing Co nanoparticles, Co@Pc/C can achieve a Faradaic efficiency of 84 % and CO current density of 28 mA cm(-2) at -0.9 V, which are 18 and 47 times higher than Pc/C without Co, respectively. These findings provide new insights into the CO2RR on N-C-mat, which may guide the exploration of cost-effective electrocatalysts for efficient CO2 reduction.
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