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Molecular Evidences for Metallic Cobalt Boosting CO2 Electroreduction on Pyridinic Nitrogen
Angewandte Chemie International Edition ( IF 12.257 ) Pub Date : 2020-01-14 , DOI: 10.1002/anie.201916520
Chao He; Yun Zhang; Yuefeng Zhang; Lu Zhao; Lu-Pan Yuan; Jianan Zhang; Jianmin Ma; Jin-Song Hu

Nitrogen‐doped carbon materials (N‐Cs) are emerging as low‐cost metal‐free electrocatalysts for electrochemical CO 2 reduction reaction (CO 2 RR), although the activities are still unsatisfactory and the genuine active site thereof is still arguable. We herein demonstrate that CO 2 RR to CO preferentially take place on pyridinic N rather than pyrrolic N using phthalocyanine (Pc) and porphyrin with well‐defined N‐C configurations as molecular model catalysts. Systematic experiments and theoretic calculations further discover that the CO 2 RR 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 the new insights into the CO 2 RR on N‐Cs, which may guide the exploration of cost‐effective electrocatalysts for efficient CO 2 RR.
更新日期:2020-01-14

 

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