CO2催化氢化制清洁能源的研究进展及趋势

doi:10.11949/0438-1157.20200115

摘要/Abstract

摘要：

CO₂的过量排放引发了严重的温室效应，采用CO₂氢化技术在实现CO₂减排的同时又可生成高价值的产物，因此受到研究人员的广泛关注。近年来，关于CO₂氢化的研究逐渐增多，但是综合探讨多种催化技术的相关综述较少。本文将较为新型的CO₂氢化技术大致分为光催化、电催化、生物催化以及等离子体催化4种。主要从催化剂的角度，对以上4种新型CO₂氢化技术的研究现状和最新进展进行了归纳，并简要介绍了其反应机理。同时，基于研究现状的分析，指出了4种氢化技术的进一步研究方向和需要解决的相关问题，并对CO₂氢化技术的发展作出了展望。

关键词: CO₂, 氢化, 光催化, 电催化, 生物催化, 等离子体催化

Abstract:

Excessive CO₂ emissions have caused a serious greenhouse effect. The use of CO₂ hydrogenation technology can achieve high-value products while reducing CO₂emissions. Therefore, it has been widely concerned by researchers. In recent years, the research on the hydrogenation of CO₂ has gradually increased, but there are few related reviews to comprehensively explore multiple catalytic methods. In this paper, the relatively new CO₂ hydrogenation technologies are roughly divided into 4 types: photocatalysis, electrocatalysis, biocatalysis, and plasma catalysis. From the perspective of catalysts, the research status and latest progress of four new CO₂ hydrogenation technologies above are summarized, and their reaction mechanisms are briefly introduced. At the same time, based on the analysis of the current research status, the related problems that need to be further studied and solved for the four hydrogenation technologies are pointed out, and the development and industrialization of CO₂ hydrogenation technology are prospected.

Key words: CO₂, hydrogenation, photocatalysis, electrocatalysis, biocatalysis, plasma catalysis

中图分类号:

X 701.7

周柒, 丁红蕾, 郭得通, 潘卫国, 杜威. CO₂催化氢化制清洁能源的研究进展及趋势[J]. 化工学报, 2020, 71(8): 3428-3443.

Qi ZHOU, Honglei DING, Detong GUO, Weiguo PAN, Wei DU. Recent advances in catalytic methods of CO₂ hydrogenation to clean energy[J]. CIESC Journal, 2020, 71(8): 3428-3443.

图/表 14

参考文献 131

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催化剂	主要产物	产率/(μmol/(g·h))	选择性/%	文献
Pd/Ce-TiO₂	CH₄	73.5	—	[12]
TiO₂/Ti₃C₂	CH₄	4.4	—	[16]
SCN-H-Ni-TiO₂	CH₃CHO	11.3	—	[21]
Cu/plate ZnO/Al₂O₃	CH₃OH	—	72.7	[24]
Cu-g-C₃N₄-ZnO/Al₂O₃	CH₃OH	5730.0	—	[25]
Cu/ZnGa₂O₄–ZnO	CH₃OH	—	50.0	[26]
Cu/ZnO	CH₃OH	127.8	—	[27]
In₂O₃/ZrO₂	CH₃OH	—	100.0	[28]
In₂O₃-WO₃	CH₃OH	496.0	—	[29]
In₂O_3-_x(OH)_y	CH₃OH	60.0	50.0	[32]
Cu₃SnS₄	CH₄	14.0	80.0	[33]
CdV₂O₆	CH₄	1.0	—	[39]
CdS/CdV₂O₆	CH₄	2.8	—	[39]
2%Cd/ZnS:0.2%Cu	HCOOH	3.2	99.0	[41]
g-C₃N₄/(Cu/TiO₂)	CH₃OH	429.0	—	[51]
TiO₂/rGO	CH₄	49.0	—	[52]
HCP-TiO₂-FG	CH₄	27.6	87.4	[53]

催化剂	主要产物	产率/(μmol/(g·h))	选择性/%	文献
Pd/Ce-TiO₂	CH₄	73.5	—	[12]
TiO₂/Ti₃C₂	CH₄	4.4	—	[16]
SCN-H-Ni-TiO₂	CH₃CHO	11.3	—	[21]
Cu/plate ZnO/Al₂O₃	CH₃OH	—	72.7	[24]
Cu-g-C₃N₄-ZnO/Al₂O₃	CH₃OH	5730.0	—	[25]
Cu/ZnGa₂O₄–ZnO	CH₃OH	—	50.0	[26]
Cu/ZnO	CH₃OH	127.8	—	[27]
In₂O₃/ZrO₂	CH₃OH	—	100.0	[28]
In₂O₃-WO₃	CH₃OH	496.0	—	[29]
In₂O_3-_x(OH)_y	CH₃OH	60.0	50.0	[32]
Cu₃SnS₄	CH₄	14.0	80.0	[33]
CdV₂O₆	CH₄	1.0	—	[39]
CdS/CdV₂O₆	CH₄	2.8	—	[39]
2%Cd/ZnS:0.2%Cu	HCOOH	3.2	99.0	[41]
g-C₃N₄/(Cu/TiO₂)	CH₃OH	429.0	—	[51]
TiO₂/rGO	CH₄	49.0	—	[52]
HCP-TiO₂-FG	CH₄	27.6	87.4	[53]

催化剂	主要产物	产率/ (μmol/(g ·h))	选择性/%	文献
MoO_3-_x	CH₄	2.1	—	[54]
Ru/Al₂O₃	CH₄	—	99.2	[56]
Pd/Al₂O₃	CH₄	—	98.6	[56]
Ni/Al₂O₃	CH₄	—	99.0	[56]
CoFeAl-LDH-650	CH₄	—	60.6	[53]
Ru@FL-LDHs	CH₄	277000.0	99.3	[57]
CA-LDO	CH₃OH	—	40.0	[58]
CZA-LDO	CH₃OH	—	88.0	[58]

催化剂	主要产物	产率/ (μmol/(g ·h))	选择性/%	文献
MoO_3-_x	CH₄	2.1	—	[54]
Ru/Al₂O₃	CH₄	—	99.2	[56]
Pd/Al₂O₃	CH₄	—	98.6	[56]
Ni/Al₂O₃	CH₄	—	99.0	[56]
CoFeAl-LDH-650	CH₄	—	60.6	[53]
Ru@FL-LDHs	CH₄	277000.0	99.3	[57]
CA-LDO	CH₃OH	—	40.0	[58]
CZA-LDO	CH₃OH	—	88.0	[58]

催化剂	主要产物	产率	TON	文献
50%-Pd@ICRM	HCOOH	—	204	[88]
Pd@ICRM	HCOOH	—	250	[88]
C. necator FdsABG	HCOOH	—	1.9	[90]
Mn₂(bipy)₂(CO)₆-DBU	HCOOH	98.0%	6250	[94]
D. desulfuricans	HCOOH	14000.0 μmol/(g·h)	—	[96]
microbial-FeCl₃	HCOOH	34.6 mg/(L·h)	—	[97]
PANi-ClFDH	HCOOH	1.4 μmol/(h·cm²)	—	[101]
Fe(PNP^H-iPr)(H)(CO)(Br)	HCOOH	98.0%	1220	[103]
Fe(PNP^Me-iPr)(H)(CO)(Br)	HCOOH	98.0%	9840	[103]
Fe(PNP^NMe-iPr)(H)2(CO)	HCOOH	>99.0%	10000	[104]
Mn(PNPNHiPr)(H)(CO)2	HCOOH	63.0%	31600	[104]
Ni(BF₄)₂/NP₃	HCOOH	—	4650710	[105]

CO₂催化氢化制清洁能源的研究进展及趋势

Recent advances in catalytic methods of CO₂ hydrogenation to clean energy

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催化剂	主要产物	法拉第效率(FE)/%	选择性/%	过电位/V	文献
Cu/ZrO₂	CH₃OH	—	28.3	—	[67]
Cu/TiO₂	CH₃OH	—	19.1	—	[67]
K/Mn/Fe/NCNT	CO	—	72.1	—	[72]
Cu-ZrO₂/CNFs	CH₃OH	—	67.0	—	[77]
5% Ru/NCNF	CH₄	—	99.0	—	[78]
2b-AuNP	CO	71	—	0.47	[82]
SL-NG@Sn	formate	92	—	-1.00	[83]

类型	催化剂	主要产物	选择性/%	能源效率/%	CO₂转化率/%	文献
DBD	Mn/γ-Al₂O₃	CO	77.7		10.2	[109]
	PbTiO₃	CH₄	75	—	15.0	[111]
	ZrO₂ pellets	CO	95	7.0	52.1	[114]
	Ni/Al₂O₃-60% Ar	CH₄	7.6	2.2	56.1	[117]
	Pd/ZnO	CH₄; CO	—	—	32.5	[118]
GA	N₂：10%→95%	CO	—	12.0	12.7	[121]
MW	NiO/TiO₂(Ar-P)	CO	—	18.0	43.0	[126]
	(20000 Pa)	CO	—	23.0	38.0	[127]
	（H₂∶CO₂ = 1）	CO	100	—	60.0	[129]
	（H₂∶CO₂ = 3）	CO		6	80	[128]
RF	pure CO₂	CO	—	—	66.0	[130]
	25% H₂	CO	—	—	21.6	[130]
	91% H₂	CO	—	—	65.2	[130]

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