CO2 Overall Splitting by a Bifunctional Metal-Free Electrocatalyst

被引：80

作者：

Ghausi, Muhammad Arsalan ^{[1
,2
]}

Xie, Jiafang ^{[1
]}

Li, Qiaohong ^{[1
]}

Wang, Xueyuan ^{[1
,2
]}

Yang, Rui ^{[1
,2
]}

Wu, Maoxiang ^{[1
]}

Wang, Yaobing ^{[1
]}

Dai, Liming ^{[3
,4
]}

机构：

[1] Chinese Acad Sci, CAS Key Lab Design & Assembly Funct Nanostruct, State Key Lab Struct Chem,Key Lab Optoelect Mat C, Fujian Prov Key Lab Nanomat,Fujian Inst Res Struc, YangQiao West Rd 155, Fuzhou, Fujian, Peoples R China

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

[3] Case Western Reserve Univ, Case Sch Engn, Dept Macromol Sci & Engn, 10900 Euclid Ave, Cleveland, OH 44106 USA

[4] Univ New South Wales, Sch Chem Engn, UNSW CWRU Int Joint Lab, Sydney, NSW 2051, Australia

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2018年 / 57卷 / 40期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

bifunctional systems; CO2; reduction; electrocatalysis; metal-free electrodes; nanomaterials; OXYGEN REDUCTION; ELECTROCHEMICAL REDUCTION; FREE CATALYSTS; EFFICIENT; EVOLUTION; DEFECTS; O-2;

D O I：

10.1002/anie.201807571

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Photo/electrochemical CO2 splitting is impeded by the low cost-effective catalysts for key reactions: CO2 reduction (CDRR) and water oxidation. A porous silicon and nitrogen co-doped carbon (SiNC) nanomaterial by a facile pyrolyzation was developed as a metal-free bifunctional electrocatalyst. CO2-to-CO and oxygen evolution (OER) partial current density under neutral conditions were enhanced by two orders of magnitude in the Tafel regime on SiNC relative to single-doped comparisons beyond their specific area gap. The photovoltaic-driven CO2 splitting device with SiNC electrodes imitating photosynthesis yielded an overall solar-to-chemical efficiency of advanced 12.5% (by multiplying energy efficiency of CO2 splitting cell and photovoltaic device) at only 650mV overpotential. Mechanism studies suggested the elastic electron structure of -Si(O)-C-N- unit in SiNC as the highly active site for CDRR and OER simultaneously by lowering the free energy of CDRR and OER intermediates adsorption.

引用

页码：13135 / 13139

页数：5

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