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Molecular Evidence for Metallic Cobalt Boosting CO 2 Electroreduction on Pyridinic Nitrogen
Author(s) -
He Chao,
Zhang Yun,
Zhang Yuefeng,
Zhao Lu,
Yuan LuPan,
Zhang Jianan,
Ma Jianmin,
Hu JinSong
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201916520
Subject(s) - faraday efficiency , cobalt , electrochemistry , porphyrin , catalysis , phthalocyanine , chemistry , metal , boosting (machine learning) , nitrogen , density functional theory , nanoparticle , metal organic framework , inorganic chemistry , materials science , nanotechnology , photochemistry , electrode , organic chemistry , computational chemistry , computer science , adsorption , machine learning
Nitrogen‐doped carbon materials (N‐C mat ) are emerging as low‐cost metal‐free electrocatalysts for the electrochemical CO 2 reduction reaction (CO 2 RR), although the activities are still unsatisfactory and the genuine active site is still under debate. We demonstrate that the CO 2 RR 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 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 new insights into the CO 2 RR on N‐C mat , which may guide the exploration of cost‐effective electrocatalysts for efficient CO 2 reduction.