CO2RR稀土基催化剂的研究进展

doi:10.12422/j.issn.1006-396X.2023.04.001

摘要/Abstract

摘要：

化石燃料的大规模使用导致CO₂过度排放，造成气温升高、冰川融化、病虫害加剧等一系列问题。通过电化学还原CO₂（CO₂RR）将CO₂转化为有价值的化学品和燃料，已成为实现碳循环的一种途径。多年来，已将金属及其氧化物、碳基材料、单原子催化剂等不同电催化剂用于CO₂RR并取得了一定的进展，但作为“工业维生素”的稀土元素用于CO₂RR的报道较少。综述了稀土元素作为载体、主催化剂、助催化剂用于CO₂RR的情况，探究了稀土元素材料在CO₂RR中的催化性能，以期促进对工业应用的研究。

关键词: 主催化剂, 助催化剂, 载体, CO₂还原, 二氧化铈, 催化剂

Abstract:

The large?scale use of fossil fuels has led to excessive CO₂ emissions, resulting in a series of problems such as rising temperatures, melting glaciers, and the accumulation of diseases and pests. Using electrochemical reduction of CO₂ (CO₂RR) to convert CO₂ into valuable chemicals and fuels has become a way to realize the carbon cycle. Over the years, good progress has been made in using metals and their oxides, carbon based materials, monatomic catalysts and other electrocatalysts for CO₂RR, but rare earth metals as "industrial vitamins" have been rarely reported for CO₂RR. This paper summarizes the application of rare earth elements as carriers, main catalysts and cocatalysts in CO₂RR, and explores the catalytic performance of rare earth materials in CO₂RR, so as to promote practical research of industrial application.

Key words: Main catalyst, Cocatalyst, Support, CO₂ reduction, Cerium dioxide, Catalyst

中图分类号:

TQ013

刘嘉敏, 越婷婷, 常迎, 郭少红, 贾晶春, 贾美林. CO₂RR稀土基催化剂的研究进展[J]. 石油化工高等学校学报, 2023, 36(4): 1-12.

Jiamin Liu, Tingting Yue, Ying Chang, Shaohong Guo, Jingchun Jia, Meilin Jia. Research Progress on Rare Earth⁃Based Catalysts for CO₂ Reduction Reaction（CO₂RR）[J]. Journal of Petrochemical Universities, 2023, 36(4): 1-12.

图/表 9

表1 标准实验条件下CO2RR半反应的电极电位[25?26]

Table 1 Electrode potential of CO2RR half reaction under standard experimental conditions[25?26]

半反应	电极电位（vs.RHE）/V
$C O 2 + 2 H + + 2 e - → C O + H 2 O$	－0.53
$C O 2 + H + + e - → H C O O -$	－0.61
$C O 2 + 8 H + + 8 e - → C H 4 + 2 H 2 O$	－0.24
$2 C O 2 + 12 H + + 12 e - → C 2 H 4 + 4 H 2 O$	0.06
$C O 2 + 5 H + + 5 e - → C H 3 O H + H 2 O$	－0.38
$2 C O 2 + 12 H + + 12 e - → C 2 H 5 O H + 3 H 2 O$	0.08

表1 标准实验条件下CO2RR半反应的电极电位[25?26]

Table 1 Electrode potential of CO2RR half reaction under standard experimental conditions[25?26]

半反应	电极电位（vs.RHE）/V
$C O 2 + 2 H + + 2 e - → C O + H 2 O$	－0.53
$C O 2 + H + + e - → H C O O -$	－0.61
$C O 2 + 8 H + + 8 e - → C H 4 + 2 H 2 O$	－0.24
$2 C O 2 + 12 H + + 12 e - → C 2 H 4 + 4 H 2 O$	0.06
$C O 2 + 5 H + + 5 e - → C H 3 O H + H 2 O$	－0.38
$2 C O 2 + 12 H + + 12 e - → C 2 H 5 O H + 3 H 2 O$	0.08

图1 C1/C2产物的生成过程[33]

Fig.1 Product generation process of C1/C2[33]

图2 Y/NC及Sc/NC的电子结构和电化学性能测试图[56]

Fig.2 Electronic structure and electrochemical performance test diagram of Y/NC and Sc/NC[56]

图3 Pr?NC?8的电子结构和DFT计算结果[57]

Fig.3 Electronic structure and DFT calculation of Pr?NC?8[57]

图4 CeO2保护Cu2+的自牺牲方案和在CO2RR过程中的变化[68]（a） CeO2保护Cu2+的自牺牲方案（b）经过CO2RR后Cu?Ce?O x 和CuO/CeO2的CV图

Fig.4 CeO2 protects Cu2+ from Self sacrifice schemex and its changes in the process of CO2RR[68]

图5 CeO x /Au（111）与CO2之间的相互作用和Cu/ CeO2还原CO2的DFT计算[72?73]

Fig.5 Interaction between CeO x /Au (111) and CO2 and DFT calculation of Cu/CeO2 reducing CO2[72?73]

图6 Ag/CeO2 和Au?CeO2?DP加速CO2RR的机理[74?75]（a） Ag/CeO2界面用于CO2RR （b） Au?CeO2?DP上生成Auδ+的机制

Fig.6 Mechanism of Ag/CeO2 interface and Au?CeO2?DP accelerating CO2RR[74?75]

图7 CBNGd的电子结构变化图和CO2RR性能测试图[78]

Fig.7 Electronic structure change diagram of CBNGd and CO2RR performance test diagram[78]

图8 ZnLa的XPS精细谱图和部分态密度图[79]

Fig.8 XPS fine spectrum and partial density of states of ZnLa[79]

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CO₂RR稀土基催化剂的研究进展

Research Progress on Rare Earth⁃Based Catalysts for CO₂ Reduction Reaction（CO₂RR）

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