化学
电化学
电催化剂
二氧化碳电化学还原
催化作用
纳米技术
还原(数学)
生化工程
电极
材料科学
有机化学
一氧化碳
物理化学
几何学
数学
工程类
作者
Shenzhen Xu,Emily A. Carter
出处
期刊:Chemical Reviews
[American Chemical Society]
日期:2018-12-18
卷期号:119 (11): 6631-6669
被引量:488
标识
DOI:10.1021/acs.chemrev.8b00481
摘要
Electrochemical and photoelectrochemical CO2 reduction technologies offer the promise of zero-carbon-emission renewable fuels needed for heavy-duty transportation. However, the inert nature of the CO2 molecule poses a fundamental challenge that must be overcome before efficient (photo)electrochemical CO2 reduction at scale will be achieved. Optimal catalysts exhibit enduring stability, fast kinetics, high selectivity, and low manufacturing cost. Identifying catalytic mechanisms of CO2 reduction in (photo)electrochemical systems could accelerate design of efficient catalysts. In recent decades, numerous theoretical studies have contributed to our understanding of CO2 reduction pathways and identifying rate-limiting steps. Although a significant body of work exists regarding homogeneous electrocatalysis for CO2 reduction, this review focuses specifically on the theory of heterogeneous (photo)electrochemical reduction. We first give an overview of the relevant thermodynamics and semiconductor physics. We then introduce important, widely used theoretical techniques and modeling approaches to catalysis. Recent progress in elucidating mechanisms of heterogeneous (photo)electrochemical CO2 reduction is discussed through the lens of two experimental systems: pyridine (Py)-catalyzed CO2 (photo)electrochemical reduction at p-GaP photoelectrodes and electrochemical CO2 reduction at Cu electrodes. We close by proposing strategies and principles for the future design of (photo)electrochemical catalysts to improve the selectivity and reaction kinetics of CO2 reduction.
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