可再生能源驱动的生物催化固定CO2的研究进展

doi:10.16085/j.issn.1000-6613.2022-1795

摘要/Abstract

摘要：

工业发展带来了经济效益的同时，伴随着化石燃料的日益枯竭和CO₂的大量排放，加剧了温室效应，出现了全球变暖的问题。我国在倡导节能减排的同时，大力发展CO₂固定技术，将大气中丰富的CO₂转化为可以供人们利用的化工原料、燃料甚至更高附加值产品，不仅能够保护环境，同时还可提高经济效益。当前全球可再生能源规模的不断扩大缓解了传统能源消耗的压力，同时可再生能源可以为固定CO₂提供可持续的、清洁的驱动能量，并且随着分子生物学的发展，生物法固碳技术越发成熟，同时较其他固定CO₂方法而言，生物法固碳具有条件温和、选择性高、产品多样等优势，因此利用可再生能源耦合生物催化进行CO₂的固定逐渐成为了这一领域的研究重点。本文总结了近年来生物催化与电化学、光化学反应耦合固定CO₂的研究，包括光、电催化与酶催化偶联以及光、电催化与全细胞催化偶联对CO₂的利用，简述了其耦合催化原理与研究进展，并总结了目前研究需要突破的关键技术及提高CO₂催化转化效率的方法。

关键词: 二氧化碳, 生物催化, 电化学, 光化学, 耦合, 可再生能源

Abstract:

Along with the depletion of fossil fuels, industrial development has brought economic benefits, but also leads to large amounts of CO₂ emissions, which has aggravated the greenhouse effect and caused the problem of global warming. Upon the advocacy of energy conservation and pollution reduction, CO₂ fixation technologies are vigorously developed in China to transform the abundant CO₂ into chemical raw materials, fuels and even higher value-added products. It can not only protect the environment but also improve economic benefits. At present, the continuous expansion of the global renewable energy scale has relieved the pressure of traditional energy consumption, while renewable energy can provide a sustainable and clean driving force for CO₂ fixation. Meanwhile, with the development of molecular biology, the bio-fixation technology of CO₂ has become more and more mature. And compared with other fixation technology, bio-fixation of CO₂ has various advantages including mild conditions, high selectivity and the diversity of products, which has gradually become the focus in this field. Herein the recent research on the coupling of biocatalysis with electrochemical and photochemical reactions for CO₂ fixation was summarized including the coupling of photocatalysis or photoelectrocatalysis with enzyme catalysis, and the combination of photocatalysis or electrocatalysis with the whole-cell catalyst technology. The principle and research progress of these strategies were introduced, while the current issues in the field as well as the essential technologies to break through the conversion efficiency of CO₂ were also prospected.

Key words: carbon dioxide (CO₂), bio-fixation, electrochemistry, photochemistry, coupling, renewable energy

中图分类号:

Q819

刘艳辉, 周明芳, 马铭, 王凯, 谭天伟. 可再生能源驱动的生物催化固定CO₂的研究进展[J]. 化工进展, 2023, 42(1): 1-15.

LIU Yanhui, ZHOU Mingfang, MA Ming, WANG Kai, TAN Tianwei. Recent advances on the bio-fixation of CO₂ driven by renewable energy[J]. Chemical Industry and Engineering Progress, 2023, 42(1): 1-15.

图/表 7

表1 常见碳还原相关酶

酶	反应	固碳机制	优点	缺点	参考文献
碳酸酐酶(CA)	$C O 2 + H 2 O ⇌ H C O 3 - + H +$	与Zn²⁺活性位点络合的OH^-亲核进攻CO₂生成HCO $3 -$	转化效率高，不需要辅助因子	价格昂贵，可重用性低	[16-17]
一氧化碳脱氢酶(CODH)	$C O 2 + 2 H + + 2 e - ⇌ C O + H 2 O$	CODH与CO₂分子结合，通过铁硫团簇(Fe₄S₄)催化CO₂生成CO	活性高，产品可转化性高	稳定性差，氧气敏感	[18-20]
重构固氮酶	$C O 2 + 2 H + + 2 e - ⇌ C O + H 2 O$ $C O 2 + 2 H + + 2 e - ⇌ H C O O H$ $C O 2 + 8 H + + 8 e - ⇌ C H 4$	Fe蛋白将电子传递给相应的催化中心	产物谱较大	氧敏感	[16, 21-22]
甲酸脱氢酶(FDH)	$C O 2 + 2 H + + 2 e - ⇌ H C O O H$	利用活性中心还原的金属团簇作为氢化物供体，通过氢化物转移催化CO₂还原	选择性高	部分氧敏感，依赖辅助因子	[16, 23-24]

表1 常见碳还原相关酶

酶	反应	固碳机制	优点	缺点	参考文献
碳酸酐酶(CA)	$C O 2 + H 2 O ⇌ H C O 3 - + H +$	与Zn²⁺活性位点络合的OH^-亲核进攻CO₂生成HCO $3 -$	转化效率高，不需要辅助因子	价格昂贵，可重用性低	[16-17]
一氧化碳脱氢酶(CODH)	$C O 2 + 2 H + + 2 e - ⇌ C O + H 2 O$	CODH与CO₂分子结合，通过铁硫团簇(Fe₄S₄)催化CO₂生成CO	活性高，产品可转化性高	稳定性差，氧气敏感	[18-20]
重构固氮酶	$C O 2 + 2 H + + 2 e - ⇌ C O + H 2 O$ $C O 2 + 2 H + + 2 e - ⇌ H C O O H$ $C O 2 + 8 H + + 8 e - ⇌ C H 4$	Fe蛋白将电子传递给相应的催化中心	产物谱较大	氧敏感	[16, 21-22]
甲酸脱氢酶(FDH)	$C O 2 + 2 H + + 2 e - ⇌ H C O O H$	利用活性中心还原的金属团簇作为氢化物供体，通过氢化物转移催化CO₂还原	选择性高	部分氧敏感，依赖辅助因子	[16, 23-24]

图1 光、电催化酶耦合反应器固定CO2原理

表2 不同电酶耦合催化相关参数汇总

阳极	阴极	酶	转化产物	效率	参考文献
Pt	石墨棒	FDH	HCOOH	928.8μmol·L^-1·mg Enzyme^-1·h^-1	[45]
Co-Pi/α-Fe₂O₃	ITO	TsFDH		6.4μmol·h^-1	[46]
TK/TiO₂	CH₃V(CH₂)₉COOH	FDH		0.01µmol·h^-1	[47]
IO-TiO₂\|dpp\|POs	IO-TiO₂	W-FDH		(0.185 ± 0.017)μmol·cm^-2	[48]
FeOOH/BiVO₄	3D TiN	ClFDH		0.78µmol·h^-1	[49]
Pt	碳布@DA²⁺	FDH		3500µmol·L^-1·h^-1	[50]
Co-Pi/α-Fe₂O₃	BiFeO₃	FDH,F_aldDH,ADH	CH₃OH	220μmol·h^-1	[51]
Pt	ZIF-8@ [Cp*RhCl₂]₂	FDH,F_aldDH,ADH		822μmol·g^-1·h^-1	[52]
Pt	Rh合物	FDH,F_aldDH,ADH		480μmol·L^-1·h^-1	[53]

表3 不同光酶耦合催化相关参数汇总

光催化剂	酶	催化条件	转化产物	效率	参考文献
CCG-IP	FDH，F_aldDH，ADH	可见光	CH₃OH	6.8μmol·L^-1·h^-1	[59]
CNA		[Cp*Rh(bpy)H₂O]²⁺，TEOA，可见光		45μmol·h^-1	[60]
H₂TPPS		TEOA,MV²⁺，可见光		4.08μmol·L^-1·h^-1	[61]
ZnTPyPBr		[Cp*Rh(bpy)H₂O]²⁺，TEOA，氙灯照射		143.3μmol·L^-1·h^-1	[62]
PTi，Cds QDs	FDH FDH，F_aldDH，ADH	[Cp*Rh(bpy)H₂O]²⁺，TEOA，可见光	HCOOH CH₃OH	1500μmol·L^-1·h^-1 99μmol·L^-1·h^-1	[63]
C₆₀聚合物	FDH	Rh[Cp*Rh(bpy)H₂O]²⁺，可见光	HCOOH	119.73μmol·h^-1	[64]
TiO₂		紫外光		51.3μmol·L^-1·h^-1	[65]
TPE-C₃N₄		Rh,TEOA，MAF-8，可见光		1861μmol·L^-1·h^-1	[66]
g-C₃N₄	CA，FateDH	ZIF-8，可见光	HCOOH	48.6μmol·h^-1	[6]

图2 微生物电合成系统固定CO2

表4 不同微生物电合成发酵利用CO2相关参数汇总

菌株	培养类型	产物	效率	阴极材料	参考文献
真罗氏菌LH74D	纯培养	甲酸	0.73mmol·L^-1·d^-1	Pt（多孔陶瓷杯）	[86]
莫氏热自养菌		甲酸乙酸	63.2mmol·m^-2·d^-1 58.2mmol·m^-2·d^-1	碳纳米颗粒	[87]
大肠杆菌		丙酮酸	10mmol·L^-1·d^-1	铟片	[88]
大肠杆菌		琥珀酸	4.36mmol·L^-1·d^-1	Pt+碳布	[89]
大肠杆菌		甲酸	15.64mmol·L^-1·d^-1	酞菁铁分散碳化物衍生碳FePc-CDC	[90]
富养罗尔斯通氏菌		番茄红素	8.06×10^-4mmol·L^-1·d^-1	不锈钢网	[91]
富养罗尔斯通氏菌		α-葎草烯	0.0077mmol·L^-1·d^-1	不锈钢网	[92]
醋酸杆菌、乙酰乙酸菌等	混合培养	乙酸丁酸异丙醇	21g·m^-2·d^-1 3.7g·m^-2·d^-1 3.3g·m^-2·d^-1	碳毡	[93]
嗜热产甲烷菌		甲烷	0.34mmol·L^-1·d^-1	碳化椰子壳	[94]
厌氧菌群		乙酸异丁酸丙酸	0.81mmol·L^-1·d^-1 0.63mmol·L^-1·d^-1 0.44mmol·L^-1·d^-1	石墨毡	[95]
梭菌、脱硫弧菌等		乙酸	35.8g·m^-2·d^-1	石墨毡	[96]
硫酸盐还原菌、铁还原菌		甲醇、乙醇等	0.74g·L^-1·d^-1	石墨板	[97]
厌氧菌群		乙酸正丁酸丙酸	163mmol·L^-1·d^-1 64.69mmol·L^-1·d^-1 27mmol·L^-1·d^-1	碳毡，石墨颗粒	[98]
甲烷球菌		甲烷	(8.81 ± 0.51)mmol·m^-2·d^-1	Pt	[83]
厌氧甲烷菌		甲烷	1.392mmol·L^-1·d^-1	Ti+碳毡	[99]
产甲烷菌		甲烷	47.86mL·L^-1·d^-1	石墨毡	[100]
厚壁菌、变形菌放线菌、拟杆菌等构成的微生物群落		丁酸	(0.428±0.026)mmol·L^-1·d^-1	空心纤维膜和碳毡复合	[101]
变形菌门和热菌门为主的生物群落		丁酸	约0.76mmol·L^-1·d^-1	镍铁氧体（NiFe₂O₄@CF）修饰碳毡	[102]
醋酸杆菌等		己酸	(2.05±0.102)mmol·L^-1·d^-1	碳毡	[103]

表5 人工光合作用的催化剂与固碳微生物总结

催化剂	微生物	固碳途径	产物	固碳效率（较非耦合而言）	参考文献
硫化镉（CdS）	Rhodopseudomonaspalustris	卡尔文循环	类胡萝卜素、PHB和甲烷	生物量提高了39%，产品产量提高了1.17～1.35倍	[126]
	Rhodopseudomonaspalustris	对其Mo Fe固氮酶进行突变，使其具有固碳产甲烷的能力	甲烷	产量提高了1.7倍	[127]
	Clostridiumautoethanogenum	Wood-Ljungdahl	乙酸	产量提高了2～3倍	[128]
	Escherichia coli	异源构建HWLS （half-Wood-Ljungdahl-formolase）途径	L-苹果酸、丁酸	生物量提高了1.5倍，L-苹果酸、丁酸产率分别比对照组菌株高出8%和18%～25%	[5]
CoPi、Co-P	Ralstonia eutropha	卡尔文循环	异丙醇、异丁醇和异戊醇	固碳效率超过了最高产植物的太阳能-生物质效率	[129]
^NCNCN_x	Methanosarcina barkeri	脱氢酶、参与卡尔文循环的各种酶组成的固碳途径^[130]	甲烷	量子产率为50.3%，选择性为92.3%	[131]
AuNCs	Moorella thermoacetica	Wood-Ljungdahl	乙酸	量子效率比CdS耦合的高出33%，可持续性更强	[132]
g-C₃N₄	Ralstonia eutropha	卡尔文循环	生物塑料聚羟基丁酸酯（polyhydroxybutyrate，PHB）	产量提高了约2倍	[133]
CuO/g-C₃N₄	微生物群落	—	乙酸	产量为5.1g/L，且具有长期稳定性	[134]
有机半导体苝二酰亚胺衍生物（perylene diimide derivative, PDI）和聚芴-联苯（fluorene-co-phenylene, PFP）	Moorella thermoacetica	Wood-Ljungdahl	乙酸	效率为约1.6%，与报道的无机生物杂交种系统相当	[135]
沼泽红假单胞菌	Methanosarcina barkeri	脱氢酶、参与卡尔文循环的各种酶组成的固碳途径	甲烷	略高于典型半导体-生物杂交体系的产甲烷速率	[130]

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可再生能源驱动的生物催化固定CO₂的研究进展

Recent advances on the bio-fixation of CO₂ driven by renewable energy

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