Optimization strategy for producing carbon based fuels by photocatalytic CO2 reduction

doi:10.11949/0438-1157.20221120

Abstract

Abstract:

The photocatalytic CO₂ reduction to hydrocarbon fuel technology is directly driven by solar energy and converts CO₂ into directly usable chemicals. It is a transformative technology to help carbon peak and carbon neutrality. The efficient and low-cost operation of this technology is determined by light absorption and utilization, the morphology and structure of photocatalysts, the interfacial catalytic reaction, and mass transfer etc. In general, the internal energy and mass transfer of this technology is a multi-scale spatio-temporal process and needs to be studied by using a multi-physics field coupling model from both theoretical and application aspects. In this paper, the fundamental theory and the state-of-the-art are summarized. Also, we present the development tendency of photocatalytic CO₂ reduction technology from aspects of light absorption expansion and utilization, photogenerated carrier separation enhancement, oxidation/reduction half-reaction optimization, and mass transfer enhancement. Then we discuss the matching strategy between energy transfer and chemical reaction within the whole process, which provide the way for reducing the energy loss, promoting performance, and future industrial application of solar-driven CO₂ reduction.

Key words: solar energy, photocatalytic, CO₂ reduction, hydrocarbon fuel, optimization strategy

摘要：

光催化CO₂还原制碳氢燃料技术由太阳能直接驱动，将CO₂转化为可直接利用的化学品，是助力碳达峰、碳中和的变革性技术。该技术的高效、低成本运行受光吸收利用、光催化剂形貌结构、界面催化反应及传质等因素影响，其内部能质传输是多时空尺度、多物理场耦合的复杂过程，需要从理论和应用两方面结合多个学科展开系统研究。梳理了光催化CO₂还原基本理论及国内外研究进展，并针对技术瓶颈从光吸收拓展与利用、光生载流子分离强化、氧化/还原半反应优化及传质强化四个优化策略指出了该技术发展方向，探讨了该技术全流程能量传递和物质转化之间的耦合匹配准则，为降低反应能耗、促进性能及产率提升甚至未来工业化大规模太阳能驱动CO₂还原应用铺垫道路。

关键词: 太阳能, 光催化, CO₂还原, 碳氢燃料, 优化策略

CLC Number:

TK 01

Feng WANG, Shunxin ZHANG, Fangbo YU, Ya LIU, Liejin GUO. Optimization strategy for producing carbon based fuels by photocatalytic CO₂ reduction[J]. CIESC Journal, 2023, 74(1): 29-44.

王峰, 张顺鑫, 余方博, 刘亚, 郭烈锦. 光催化CO₂还原制碳氢燃料系统优化策略研究[J]. 化工学报, 2023, 74(1): 29-44.

Figures/Tables 9

Table 1 Common products of CO2 reduction and their simplified Redox equations and Redox potentials at pH=7

产物	反应	氧化还原电位(vs NHE)/V
O₂	H₂O $→$ 1/2O₂+2H⁺+2e^-	+0.82
H₂	2H⁺+2e^- $→$ H₂	-0.41
CH₄	CO₂+8H⁺+8e^- $→$ CH₄+2H₂O	-0.24
C₂H₆	2CO₂+14H⁺+14e^- $→$ C₂H₆+4H₂O	-0.27
CO	CO₂+2H⁺+2e^- $→$ CO+H₂O	-0.51
CH₃OH	CO₂+6H⁺+6e^- $→$ CH₃OH+H₂O	-0.39
C₂H₅OH	2CO₂+12H⁺+12e^- $→$ C₂H₅OH+3H₂O	-0.33
CH₃CH₂CH₂OH	3CO₂+18H⁺+18e^- $→$ CH₃CH₂CH₂OH+5H₂O	-0.31
CH₃CH(OH)CH₃	3CO₂+18H⁺+18e^- $→$ CH₃CH(OH)CH₃+5H₂O	-0.30
HCHO	CO₂+4H⁺+4e^- $→$ HCHO+H₂O	-0.55
CH₃CHO	2CO₂+10H⁺+10e^- $→$ CH₃CHO+3H₂O	-0.36
CH₃CH₂CHO	3CO₂+16H⁺+16e^- $→$ CH₃CH₂CHO+5H₂O	-0.32
CH₃COCH₃	3CO₂+16H⁺+16e^- $→$ CH₃COCH₃+5H₂O	-0.31
HCOOH	CO₂+2H⁺+2e^- $→$ HCOOH	-0.58
CH₃COOH	2CO₂+8H⁺+8e^- $→$ CH₃COOH+2H₂O	-0.31

Table 1 Common products of CO2 reduction and their simplified Redox equations and Redox potentials at pH=7

产物	反应	氧化还原电位(vs NHE)/V
O₂	H₂O $→$ 1/2O₂+2H⁺+2e^-	+0.82
H₂	2H⁺+2e^- $→$ H₂	-0.41
CH₄	CO₂+8H⁺+8e^- $→$ CH₄+2H₂O	-0.24
C₂H₆	2CO₂+14H⁺+14e^- $→$ C₂H₆+4H₂O	-0.27
CO	CO₂+2H⁺+2e^- $→$ CO+H₂O	-0.51
CH₃OH	CO₂+6H⁺+6e^- $→$ CH₃OH+H₂O	-0.39
C₂H₅OH	2CO₂+12H⁺+12e^- $→$ C₂H₅OH+3H₂O	-0.33
CH₃CH₂CH₂OH	3CO₂+18H⁺+18e^- $→$ CH₃CH₂CH₂OH+5H₂O	-0.31
CH₃CH(OH)CH₃	3CO₂+18H⁺+18e^- $→$ CH₃CH(OH)CH₃+5H₂O	-0.30
HCHO	CO₂+4H⁺+4e^- $→$ HCHO+H₂O	-0.55
CH₃CHO	2CO₂+10H⁺+10e^- $→$ CH₃CHO+3H₂O	-0.36
CH₃CH₂CHO	3CO₂+16H⁺+16e^- $→$ CH₃CH₂CHO+5H₂O	-0.32
CH₃COCH₃	3CO₂+16H⁺+16e^- $→$ CH₃COCH₃+5H₂O	-0.31
HCOOH	CO₂+2H⁺+2e^- $→$ HCOOH	-0.58
CH₃COOH	2CO₂+8H⁺+8e^- $→$ CH₃COOH+2H₂O	-0.31

Fig.1 Schematic diagram of photocatalytic CO2 reduction

Table 2 Representative work of photocatalytic CO2 reduction in recent years

体系	催化剂	反应体系	还原产物	氧化产物	产率	文献
无牺牲剂体系	In₄SnS₈	H₂O+CO₂	CH₄ CO	O₂	10.70 μl·h^-1 9.39 μl·h^-1	[29]
	Pt-TiO₂	H₂O+CO₂	CH₄		1361 μmol·g^-1·h^-1	[30]
	SnS₂-C	H₂O+CO₂	CH₃CHO		96.66 μmol·g^-1·h^-1	[31]
	CdS/Mn₂O₃/PAA	H₂O+CO₂	HCOOH CH₃CH₂OH H₂		1392.3 μmol·g^-1·h^-1 52.2 μmol·g^-1·h^-1 2766 μmol·g^-1·h^-1	[32]
	In₂S₃/Bi₂MoO₆	H₂O+CO₂	CO		28.54 μmol·g^-1·h^-1	[33]
	CuIn₅S₈	H₂O+CO₂	CH₄		8.7 μmol·g^-1·h^-1	[34]
	Cu₂O	H₂O+CO₂	CH₃OH		1.2 mol·g^-1·h^-1	[17]
	^mCD/CN	H₂O+CO₂	CH₃OH		13.9 μmol·g^-1·h^-1	[35]
	g-CN-MI-40	H₂O+CO₂	CH₃OH	H₂O₂	4.18 mmol·g^-1	[36]
	Ag-MnO _x /CaTiO₃	H₂O+CO₂	CO	H₂O₂	11.8 μmol·h^-1	[37]
牺牲剂体系	Ni-ZnS	K₂CO₃+K₂SO₃	HCOOH	—	427.5 μmol·g^-1·h^-1	[38]
	VZn-3D-ZnIn₂S₄	H₂O+TEOA	CO	—	276.7 μmol·g^-1·h^-1	[39]
	CdIn₂S₄/Co₃O₄	H₂O+TEOA+Co $3 2 +$	CO	—	5300 μmol·g^-1·h^-1	[40]
	O-ZnIn₂S₄	H₂O+TEOA+CH₃CN+Co $3 2 +$	CO	—	1680 μmol·g^-1·h^-1	[41]
	CdS/TiO₂	H₂O+NaHCO₃+HCl	CH₄	—	11.9 mmol·m^-2·h^-1	[42]
	CdS/NH₂-UiO-66	H₂O+TEOA	CO	—	87 μmol·g^-1·h^-1	[43]
	COF-5/CoAl-LDH	H₂O+ acetonitrile	CO	—	53.08 μmol·g^-1·h^-1	[44]
	Cu/Cd_0.5Zn_0.5S	TEOA+KHCO₃(aq)	C₂₊	—	6.54 μmol·h^-1	[45]

Table 2 Representative work of photocatalytic CO2 reduction in recent years

体系	催化剂	反应体系	还原产物	氧化产物	产率	文献
无牺牲剂体系	In₄SnS₈	H₂O+CO₂	CH₄ CO	O₂	10.70 μl·h^-1 9.39 μl·h^-1	[29]
	Pt-TiO₂	H₂O+CO₂	CH₄		1361 μmol·g^-1·h^-1	[30]
	SnS₂-C	H₂O+CO₂	CH₃CHO		96.66 μmol·g^-1·h^-1	[31]
	CdS/Mn₂O₃/PAA	H₂O+CO₂	HCOOH CH₃CH₂OH H₂		1392.3 μmol·g^-1·h^-1 52.2 μmol·g^-1·h^-1 2766 μmol·g^-1·h^-1	[32]
	In₂S₃/Bi₂MoO₆	H₂O+CO₂	CO		28.54 μmol·g^-1·h^-1	[33]
	CuIn₅S₈	H₂O+CO₂	CH₄		8.7 μmol·g^-1·h^-1	[34]
	Cu₂O	H₂O+CO₂	CH₃OH		1.2 mol·g^-1·h^-1	[17]
	^mCD/CN	H₂O+CO₂	CH₃OH		13.9 μmol·g^-1·h^-1	[35]
	g-CN-MI-40	H₂O+CO₂	CH₃OH	H₂O₂	4.18 mmol·g^-1	[36]
	Ag-MnO _x /CaTiO₃	H₂O+CO₂	CO	H₂O₂	11.8 μmol·h^-1	[37]
牺牲剂体系	Ni-ZnS	K₂CO₃+K₂SO₃	HCOOH	—	427.5 μmol·g^-1·h^-1	[38]
	VZn-3D-ZnIn₂S₄	H₂O+TEOA	CO	—	276.7 μmol·g^-1·h^-1	[39]
	CdIn₂S₄/Co₃O₄	H₂O+TEOA+Co $3 2 +$	CO	—	5300 μmol·g^-1·h^-1	[40]
	O-ZnIn₂S₄	H₂O+TEOA+CH₃CN+Co $3 2 +$	CO	—	1680 μmol·g^-1·h^-1	[41]
	CdS/TiO₂	H₂O+NaHCO₃+HCl	CH₄	—	11.9 mmol·m^-2·h^-1	[42]
	CdS/NH₂-UiO-66	H₂O+TEOA	CO	—	87 μmol·g^-1·h^-1	[43]
	COF-5/CoAl-LDH	H₂O+ acetonitrile	CO	—	53.08 μmol·g^-1·h^-1	[44]
	Cu/Cd_0.5Zn_0.5S	TEOA+KHCO₃(aq)	C₂₊	—	6.54 μmol·h^-1	[45]

Fig.2 Light absorption expansion and utilization of photocatalysts under different optimization strategies

Fig.3 Effect of morphology, heterojunction and surface engineering on carrier separation and enhancement

Fig.4 Effects of interfacial chemical reaction regulation on CO2 reduction and water oxidation half reactions

Fig.5 Schematic diagram of energy losses in the whole photocatalytic process [7]

Fig.6 Effect of enhanced mass transfer on photocatalytic performance

Fig.7 Future challenges for photocatalytic CO2 reduction systems

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Optimization strategy for producing carbon based fuels by photocatalytic CO₂ reduction

光催化CO₂还原制碳氢燃料系统优化策略研究

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