CO2光热催化还原研究进展

doi:10.11949/0438-1157.20220863

摘要/Abstract

摘要：

CO₂光热催化转化是一种新型的CO₂利用技术，该过程绿色、经济且无须额外能量输入，是当下的热门研究领域之一。本文主要总结了CO₂光热催化转化领域的最新研究进展，介绍了基于光热转化的光热催化剂设计方法，同时从光热催化机理出发解析了CO₂还原反应的光热催化剂构建策略，并揭示了CO₂还原反应中的光热协同耦合机制，为光热催化剂的设计以及CO₂的高效转化和利用提供参考。

关键词: CO₂利用, 光热催化, 光热转化, 催化剂设计

Abstract:

Photothermal catalytic conversion of CO₂ is a new type of CO₂ utilization technology. The process is green, economical, and requires no additional energy input. It is one of the current hot research fields. This paper introduced recent advances in photothermal catalytic conversion of CO₂ and summarized design methods for photothermal catalysts based on photo-to-thermal conversion. In addition, fabrication strategies were also investigated in the perspective of photothermal catalytic mechanism and the synergy between photo- and thermo- effects was also discussed. This work aims to promote the understanding of photothermal synergy for CO₂ reduction reaction and provides reference for the design of photothermal catalysts and CO₂ valorization.

Key words: CO₂ utilization, photothermal catalysis, photothermal conversion, catalysts design

中图分类号:

TQ 032

闫帅, 杨海平, 陈应泉, 王贤华, 曾阔, 陈汉平. CO₂光热催化还原研究进展[J]. 化工学报, 2022, 73(10): 4298-4310.

Shuai YAN, Haiping YANG, Yingquan CHEN, Xianhua WANG, Kuo ZENG, Hanping CHEN. Recent advances in photothermal catalysis of CO₂ reduction[J]. CIESC Journal, 2022, 73(10): 4298-4310.

图/表 7

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序号	反应名称	反应式	ΔH_{298 K}/(kJ·mol^-1)	常用催化剂
（1）	逆水煤气变换(RWGS)	CO₂ + H₂ CO + H₂O	+41.0	Fe₃O₄、Cu/CeO₂、Ru/Al₂O₃等
（2）	Sabatier	CO₂ + 4H₂ CH₄ + 2H₂O	-165.1	Ni/SiO₂、Ru/CeO₂、Co/Al₂O₃等
（3）	甲醇合成	CO₂ + 3H₂ CH₃OH + H₂O	-49.4	Cu/ZnO、Pd/ZnO、In₂O₃等
（4）	甲烷干重整	CO₂ + CH₄ 2CO + 2H₂	+247.3	Ni/CeO₂、Ni/Al₂O₃等

序号	反应名称	反应式	ΔH_{298 K}/(kJ·mol^-1)	常用催化剂
（1）	逆水煤气变换(RWGS)	CO₂ + H₂ CO + H₂O	+41.0	Fe₃O₄、Cu/CeO₂、Ru/Al₂O₃等
（2）	Sabatier	CO₂ + 4H₂ CH₄ + 2H₂O	-165.1	Ni/SiO₂、Ru/CeO₂、Co/Al₂O₃等
（3）	甲醇合成	CO₂ + 3H₂ CH₃OH + H₂O	-49.4	Cu/ZnO、Pd/ZnO、In₂O₃等
（4）	甲烷干重整	CO₂ + CH₄ 2CO + 2H₂	+247.3	Ni/CeO₂、Ni/Al₂O₃等

催化剂	反应条件				产物	(选择性/%)/ [产率/(mmol·g^-1·h^-1)]	文献
催化剂	温度/℃	压力/MPa	批次/流动	光功率/(W·cm^-2)	产物	(选择性/%)/ [产率/(mmol·g^-1·h^-1)]	文献
逆水煤气变换RWGS
In-Em In₂O₃	300	0.18	批次	—	CO	99.99%	[28]
Fe₂Ce₁-300	419	0.18	批次	2.2	CO	约100%	[29]
Ni₁₂P₅/SiO₂	约400	0.12	批次	2.3	CO	99.7%/960	[30]
C-In₂O_3-_x	约400	—	批次	2.98	CO	约100%/123.6	[31]
Sabatier
Ru@FL-LDHs	约350	—	流动	约1.0	CH₄	约100%/277.0	[32]
Ni/Ce_0.9Si_0.1O₂	约300	0.075	批次	—	CH₄	约100%	[33]
Ni-BaTiO₃	约250	—	批次	—	CH₄	约100%/103.7	[34]
Rh/Al	约700	1.5	批次	11.3	CH₄	约100%/550	[35]
Co/CeO₂	300	—	流动	0.5	CH₄	94%	[36]
Ni/Nb₂C	330	0.1	批次	1.5	CH₄	83.4%	[37]
甲醇合成
H _z In₂O_3-_x (OH) _y	—	约0.21	批次	2.0	CH₃OH	36.7%	[38]
H _z In₂O_3-_x (OH) _y	—	约0.21	批次	2.0	CO	63.3%	[38]
Cu/ZnO/Al₂O₃	275	2.1	流动	0.6	CH₃OH	约90%	[39]
Cu/ZnO/Al₂O₃	275	2.1	流动	0.6	CO	约10%	[39]
Pd/ZnO	250	—	流动	—	CH₃OH	3.8	[40]
甲烷干重整
Co/Co-Al₂O₃	665	—	流动	35.39	CO	2607.6	[41]
Co/Co-Al₂O₃	665	—	流动	35.39	H₂	1192.2	[41]
Pt/Co-Al₂O₃	666	—	流动	34.3	CO	5364.6	[42]
Pt/Co-Al₂O₃	666	—	流动	34.3	H₂	4536.0	[42]
Ni/m-TiO₂	600	—	流动	—	CO	131.72	[43]
Ni/m-TiO₂	600	—	流动	—	H₂	95.34	[43]
Rh/WO₃	500	—	流动	—	CO	约370	[44]
Rh/WO₃	500	—	流动	—	H₂	约355	[44]
其他
CoFeAl LDH-650	约310	0.18	批次	5.2	CH₄	60%	[45]
					CO	5%
					C₂₊	35%
θ-Fe₃C	310	0.1	批次	2.05	CO	25.3%	[46]
					CH₄	63.3%
					C₂₊	11.4%
Na-Co@C	235	0.28	批次	2.4	CH₄	50.2%	[47]
					CO	4.8%
					EtOH	6.5%
					C₂₊	36.2%
					other	2.3%
Co₇Cu₁Mn₁O _x	200	—	流动	—	CO	6.8%	[48]
					CH₄	85.8%
					C₂₊	7.4%

催化剂	反应条件				产物	(选择性/%)/ [产率/(mmol·g^-1·h^-1)]	文献
催化剂	温度/℃	压力/MPa	批次/流动	光功率/(W·cm^-2)	产物	(选择性/%)/ [产率/(mmol·g^-1·h^-1)]	文献
逆水煤气变换RWGS
In-Em In₂O₃	300	0.18	批次	—	CO	99.99%	[28]
Fe₂Ce₁-300	419	0.18	批次	2.2	CO	约100%	[29]
Ni₁₂P₅/SiO₂	约400	0.12	批次	2.3	CO	99.7%/960	[30]
C-In₂O_3-_x	约400	—	批次	2.98	CO	约100%/123.6	[31]
Sabatier
Ru@FL-LDHs	约350	—	流动	约1.0	CH₄	约100%/277.0	[32]
Ni/Ce_0.9Si_0.1O₂	约300	0.075	批次	—	CH₄	约100%	[33]
Ni-BaTiO₃	约250	—	批次	—	CH₄	约100%/103.7	[34]
Rh/Al	约700	1.5	批次	11.3	CH₄	约100%/550	[35]
Co/CeO₂	300	—	流动	0.5	CH₄	94%	[36]
Ni/Nb₂C	330	0.1	批次	1.5	CH₄	83.4%	[37]
甲醇合成
H _z In₂O_3-_x (OH) _y	—	约0.21	批次	2.0	CH₃OH	36.7%	[38]
H _z In₂O_3-_x (OH) _y	—	约0.21	批次	2.0	CO	63.3%	[38]
Cu/ZnO/Al₂O₃	275	2.1	流动	0.6	CH₃OH	约90%	[39]
Cu/ZnO/Al₂O₃	275	2.1	流动	0.6	CO	约10%	[39]
Pd/ZnO	250	—	流动	—	CH₃OH	3.8	[40]
甲烷干重整
Co/Co-Al₂O₃	665	—	流动	35.39	CO	2607.6	[41]
Co/Co-Al₂O₃	665	—	流动	35.39	H₂	1192.2	[41]
Pt/Co-Al₂O₃	666	—	流动	34.3	CO	5364.6	[42]
Pt/Co-Al₂O₃	666	—	流动	34.3	H₂	4536.0	[42]
Ni/m-TiO₂	600	—	流动	—	CO	131.72	[43]
Ni/m-TiO₂	600	—	流动	—	H₂	95.34	[43]
Rh/WO₃	500	—	流动	—	CO	约370	[44]
Rh/WO₃	500	—	流动	—	H₂	约355	[44]
其他
CoFeAl LDH-650	约310	0.18	批次	5.2	CH₄	60%	[45]
					CO	5%
					C₂₊	35%
θ-Fe₃C	310	0.1	批次	2.05	CO	25.3%	[46]
					CH₄	63.3%
					C₂₊	11.4%
Na-Co@C	235	0.28	批次	2.4	CH₄	50.2%	[47]
					CO	4.8%
					EtOH	6.5%
					C₂₊	36.2%
					other	2.3%
Co₇Cu₁Mn₁O _x	200	—	流动	—	CO	6.8%	[48]
					CH₄	85.8%
					C₂₊	7.4%

[1]	李富恒. 石墨烯纳米片-乙二醇纳米流体光热转化特性研究[J]. 化工学报, 2020, 71(S1): 479-485.
[2]	芮泽宝, 杨晓庆, 陈俊妃, 纪红兵. 光热协同催化净化挥发性有机物的研究进展及展望[J]. 化工学报, 2018, 69(12): 4947-4958.
[3]	李永旺,马文平,孙予罕,徐元源,钟炳. 走向分子水平的催化剂设计:科学与工程 [J]. CIESC Journal, 1998, 49(S1): 10-18.

CO₂光热催化还原研究进展

Recent advances in photothermal catalysis of CO₂ reduction

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