Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites

被引：72

作者：

Li, Xiaoxin ^{[1
,2
]}

Chai, Guoliang ^{[3
]}

Xu, Xiao ^{[1
]}

Liu, Jingjing ^{[1
]}

Zhong, Zhou ^{[1
,2
]}

Cao, Aihui ^{[1
,2
]}

Tao, Zhijie ^{[1
]}

You, Weifeng ^{[1
,2
]}

Kang, Longtian ^{[1
]}

机构：

[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, Fujian Prov Key Lab Nanomat, Key Lab Design & Assembly Funct Nanostruct, Fuzhou 350002, Fujian, Peoples R China

[2] Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[3] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China

来源：

CARBON | 2020年 / 167卷

基金：

中国国家自然科学基金;

关键词：

Iron phthalocyanine; Graphene; CO2 reduction reaction; Synergistic catalysis; Single-atom catalyst; OXYGEN REDUCTION; CARBON-DIOXIDE; ACTIVE-SITES; ELECTROCHEMICAL REDUCTION; NITROGEN; METAL; ELECTROREDUCTION; PERFORMANCE; CATALYSTS; OXIDE;

D O I：

10.1016/j.carbon.2020.06.036

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe-N-C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe-N-4-C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of *COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+-pyrrolic N-4-C on the CO2RR. (C) 2020 Elsevier Ltd. All rights reserved.

引用

页码：658 / 667

页数：10

共 52 条

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