铁基催化剂光催化还原CO2研究进展

doi:10.11949/0438-1157.20210617

摘要/Abstract

摘要：

利用可再生清洁能源——太阳能，将CO₂转化为一氧化碳、甲烷、甲醇等，因同时具有提供可持续燃料和解决全球变暖问题的潜力而受到越来越多的关注。铁基材料因具有金属/半导体的特性和独特的电子结构，在光催化还原CO₂领域具有广阔的应用潜力。基于此，各种具有高催化活性的铁基催化剂已经被设计来提高光催化还原CO₂的效率。概述了近年来铁基催化剂在光催化还原二氧化碳中的研究进展，对它们的结构特征和催化活性进行了阐述和比较，最后总结了铁基催化剂在光催化还原CO₂领域中待解决的问题，并展望了未来发展的方向。

关键词: 二氧化碳, 还原, 光催化, 铁基催化剂

Abstract:

Using renewable clean energy-solar energy to convert CO₂ into carbon monoxide, methane, methanol, etc., has attracted more and more attention because of its potential to provide sustainable fuels and solve global warming problems. Iron-based materials have broad application potential in the field of photocatalytic reduction of CO₂ due to their metal/semiconductor properties and unique electronic structure. According to this, various iron-based catalysts with high catalytic activity have been designed to enhance the efficiency of photocatalytic reduction of CO₂. This article reviews recent advances in the field of photocatalytic reduction of carbon dioxide based on iron-based catalysts. The structural characteristics and catalytic activity of iron-based catalysts are described and compared. Finally, the problems to be solved and the future development direction of iron-based catalysts in the field of photocatalytic reduction of CO₂ are summarized and prospected.

Key words: carbon dioxide, reduction, photocatalysis, iron-based catalyst

中图分类号:

TQ 138.1

党永强,李博妮,李可可,张建兰,冯香钰,张亚婷. 铁基催化剂光催化还原CO₂研究进展[J]. 化工学报, 2021, 72(10): 5016-5027.

Yongqiang DANG,Boni LI,Keke LI,Jianlan ZHANG,Xiangyu FENG,Yating ZHANG. Research progress in photocatalytic reduction of CO₂ with iron-based catalysts[J]. CIESC Journal, 2021, 72(10): 5016-5027.

图/表 12

图1 半导体光催化剂上光催化CO2转化的可能机理 [19]

Fig.1 Schematic illustration of probable mechanism of photocatalytic CO2 conversion over a semiconducting photocatalyst[19]

图2 不同异质结上光生载流子的转移路径

Fig.2 Transfer paths of photogenerated carriers on different heterojunctions

图3 金属配合物在CO2光催化转化中还原淬灭的示意性机理

Fig.3 Schematic description of reductive quenching pathway of metal complexes in photocatalytic conversion of CO2

表1 在25℃、101.325 kPa、pH 7的水溶液中CO2还原的标准电势

Table 1 Standard potentials of CO2 reduction to various products in aqueous solutions at 25 ℃， 101.325 kPa and pH 7

Reaction	E^o (vs NHE)/V
CO₂ + 2H⁺ + 2e^- HCOOH	-0.61
CO₂+ 2H⁺ + 2e^- CO + H₂O	-0.53
CO₂ + 4H⁺ + 4e^- ΗCHO + H₂O	-0.48
CO₂ + 6H⁺ + 6e^- CH₃OH + H₂O	-0.38
CO₂ + 8H⁺ + 8e^- CH₄ + 2H₂O	-0.24
2CO₂ + 12H⁺ + 12e^- C₂H₄ + 4H₂O	-0.34
2CO₂ + 12H⁺ + 12e^- C₂H₅OH + 3H₂O	-0.33
2CO₂ + 14H⁺ + 14e^- C₂H₆ + 4H₂O	-0.27

图4 空白反应、rGO、InVO4/Fe2O3、InVO4、rGO/InVO4/Fe2O3上CO2转化成甲醇的产率[37]

Fig.4 Conversion of CO2 to methanol over time using blank reaction, rGO, InVO4/Fe2O3, InVO4 and rGO/InVO4/Fe2O3 [37]

图5 Fe-p-TMA、FeTPP-p-TMA和FeTPP-o-OH的结构

Fig.5 The structure of Fe-p-TMA, FeTPP-p-TMA and FeTPP-o-OH

图6 光敏剂的结构：三[2-苯基吡啶-C2，N]铱(Ⅲ)、9-氰基蒽和红紫素

Fig.6 Structures of the tris(2-phenylpyridine)iridium, 9-anthrracenecarbonitrile and purpurin

表2 近几年铁配合物催化剂在光催化还原CO2方面的应用

Table 2 Application of iron complex catalyst in photocatalytic reduction of CO2 in recent years

光催化剂	光敏剂	还原剂	溶剂^①	产物	TON	选择性	文献
FeTPP	FeTPP	TEA	DMF	CO	70	—	[50]
Fe-p-TMA	Ir(ppy)₃	TEA	ACN∶H₂O(3∶8)	CH₄	81	81%	[51]
FeTMA	CuInS₂/ZnS QD	—	H₂O	CO	450	99%	[61]
FeTPP-p-TMA	无	BIH	CAN	CO	63	—	[52]
FeTPP-p-TMA	无	TEA	CAN	CO	33	100%	[52]
FeTPP-p-TMA	Ir(ppy)₃	TEA	CAN	CH₄	89	82%	[53]
FeTPP-o-OH	Ir(ppy)₃	TEA	CAN	CO	140	93%	[54]
Fe₃(CO)₁₂	[Ru(bpy)₃]Cl₂	TEOA	NMP∶TEOA(5∶1)	CO	36	—	[55]
Fe(CO)₃bpy	[Ru(bpy)₃]Cl₂	TEOA	NMP∶TEOA(5∶1)	CO	42	—	[55]
（环戊二烯酮）铁-三羰基配合物	Ir PS	TEOA	NMP	CO	596	—	[56]
环戊二烯酮铁配合物	Cu PS	BNAH	NMP∶TEOA(5∶1)	CO	487	99%	[57]
四联吡啶铁配合物	$R u (b p y) 3 2 +$	BIH	MeCN∶TEOA(4∶1)	CO	384	85%	[58]
四联吡啶铁配合物	Purpurin	BIH	DMF	CO	1365	92%	[58]
四联吡啶铁配合物	mpg-C₃N₄	TEOA	ACN∶TEOA (4∶1)	CO	155	97%	[59]

表2 近几年铁配合物催化剂在光催化还原CO2方面的应用

Table 2 Application of iron complex catalyst in photocatalytic reduction of CO2 in recent years

光催化剂	光敏剂	还原剂	溶剂^①	产物	TON	选择性	文献
FeTPP	FeTPP	TEA	DMF	CO	70	—	[50]
Fe-p-TMA	Ir(ppy)₃	TEA	ACN∶H₂O(3∶8)	CH₄	81	81%	[51]
FeTMA	CuInS₂/ZnS QD	—	H₂O	CO	450	99%	[61]
FeTPP-p-TMA	无	BIH	CAN	CO	63	—	[52]
FeTPP-p-TMA	无	TEA	CAN	CO	33	100%	[52]
FeTPP-p-TMA	Ir(ppy)₃	TEA	CAN	CH₄	89	82%	[53]
FeTPP-o-OH	Ir(ppy)₃	TEA	CAN	CO	140	93%	[54]
Fe₃(CO)₁₂	[Ru(bpy)₃]Cl₂	TEOA	NMP∶TEOA(5∶1)	CO	36	—	[55]
Fe(CO)₃bpy	[Ru(bpy)₃]Cl₂	TEOA	NMP∶TEOA(5∶1)	CO	42	—	[55]
（环戊二烯酮）铁-三羰基配合物	Ir PS	TEOA	NMP	CO	596	—	[56]
环戊二烯酮铁配合物	Cu PS	BNAH	NMP∶TEOA(5∶1)	CO	487	99%	[57]
四联吡啶铁配合物	$R u (b p y) 3 2 +$	BIH	MeCN∶TEOA(4∶1)	CO	384	85%	[58]
四联吡啶铁配合物	Purpurin	BIH	DMF	CO	1365	92%	[58]
四联吡啶铁配合物	mpg-C₃N₄	TEOA	ACN∶TEOA (4∶1)	CO	155	97%	[59]

图7 氨基功能化铁基MOFs上的双重激发途径[67]

Fig.7 Dual excitation pathways over amino-functionalized Fe-based MOFs[67]

图8 [FeⅡ(Por2-)(COOH-)]-和[CoⅡ(Por2-)(COOH-)]-中金属中心的电子构型对金属-碳相互作用的影响[72]

Fig.8 Influence of the electron configurations of the metal centers on the metal-carbon interactions in [FeⅡ(Por2-)(COOH-)]- and[CoⅡ(Por2-)(COOH-)]-[72]

图9 LaFeO3及其复合材料在光催化二氧化碳转化过程中的产物量[81]

Fig.9 Product amounts of LaFeO3 and its composites during the photocatalytic CO2 conversion[81]

表3 近几年铁基催化剂在光催化还原CO2方面的应用

Table 3 Application of iron-based catalysts in photocatalytic reduction of CO2 in recent years

光催化剂	合成方法	产物	产率	文献
g-C₃N₄/α-Fe₂O₃	超声波辅助法	CO/CH₄	15.8/3.1 μmol/(g·h)	[35]
CN-Al-F	湿化学法	CO	24 μmol/(g·h)	[35]
g-C₃N₄/α-Fe₂O₃	水热法	CH₃OH	5.63 μmol/(g·h)	[36]
rGO/InVO₄/Fe₂O₃	沉积-沉淀法	CH₃OH	16.9 mmol/g(24 h）	[37]
FeO_x/ZSM-5	功能离子预吸附法	CO/CH₃CHO	10.01/3.8 μmol/(g·h)	[38]
ZnFe₂O₄	溶剂热法	CH₃CHO/CH₃CH₂OH	57.8/13.7 μmol/(g·h)	[42]
ZnFe₂O₄/Ag/TiO₂	水热法	CO/CH₄/CH₃OH	606.25/132/31 μmol/(g·h)	[43]
Au/CuFe₂O₄	溶剂热法	CO	537.6 μl/(g·h)	[39]
NH₂-MIL-101（Fe）	水热法	HCOO^-	178 μmol(4 h)	[67]
NH₂-MIL-101（Fe）	水热法	CO	17.52 μmol/(g·h)	[68]
MAPbI₃@PCN-221(Fe_x)	顺序沉积法	CO/CH₄	6.625/12.85 μmol/(g·h)	[70]
NH₂-MIL-101(Fe)/g-C₃N₄	水热法	CO	132.8 μmol/g(6 h)	[71]
In-Fe_nTCPP-MOF	超声波辅助法	CO	3469 μmol/g(24 h)	[72]
BiFeO₃/SWCNTs	溶胶-凝胶法	CH₃OH	1000 μmol/g(4~6 h)	[76]
BiFeO₃-ZnO	水热法	—	CO₂转化率：21%	[77]
Ag₂CrO₄/Ag/BiFeO₃@RGO	—	CH₄	260 μmol/g(8 h)	[78]
TiO₂/碳纳米球/N-LaFeO₃	水热法，热解法	CO/CH₄	150/110 μmol/g(8 h)	[81]
Fe–TiO₂	水热法	CH₄	7.73 μmol/g(12 h)	[85]
Fe–TiO₂	溶胶-凝胶法	CH₃OH	约2125 μmol/g(12 h)	[86]
Fe-N-TiO₂	溶胶-凝胶法	CH₄/CH₃OH	38.72/1.73 μmol/(g·h)	[87]
Fe–CeO₂	纳米铸造法	CO/CH₄	12.38/2.88 μmol/(g·h)	[17]

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铁基催化剂光催化还原CO₂研究进展

Research progress in photocatalytic reduction of CO₂ with iron-based catalysts

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