微生物电合成系统阴极电子传递机制和氢介导强化措施

doi:10.16085/j.issn.1000-6613.2024-1073

摘要/Abstract

摘要：

微生物电合成系统是以微生物作为生物催化剂，利用可再生能源将二氧化碳（CO₂）还原为有机化合物的可持续发展技术，可以帮助缓解大气温室气体并实现低碳循环生物经济和工业CO₂生物转化过程。本文介绍了微生物电合成系统中阴极与微生物之间的电子传递机制，包括直接电子传递和间接电子传递，其中氢气（H₂）介导的间接电子传递为研究最多的电子传递过程。本文还介绍了微生物电合成系统中阴极电化学产氢和生物产氢过程的发生机制，阐述了H₂的产生和利用以及在CO₂的还原过程中不同微生物之间的相互依存和协作机制。本文还围绕H₂介导的间接电子传递过程提出促进阴极析氢反应、投加外源介质和优化反应器设计等强化措施以促进H₂的产生和CO₂的还原过程。本文为提升微生物电合成系统的电子传递效率和目标产物产率提供了理论依据和技术支撑。

关键词: 微生物电合成, 直接电子传递, 间接电子传递, 氢介导, 二氧化碳

Abstract:

Microbial electrosynthesis system is a sustainable technology that uses microorganisms as biocatalysts to reduce carbon dioxide (CO₂) to organic compounds using renewable energy sources, which can help to mitigate atmospheric greenhouse gases and realize a low-carbon recycling bio-economy and industrial CO₂ bioconversion process. This paper describes the electron transfer mechanisms between the cathode and microorganisms in microbial electrosynthesis system, including direct and indirect electron transfer, of which hydrogen (H₂) mediated indirect electron transfer is the most studied electron transfer process. This paper also introduces the occurrence mechanisms of cathodic pure electrochemical hydrogen evolution reaction and biological hydrogen production in microbial electrosynthesis system, and elaborates on the interdependence and collaboration mechanisms between different microorganisms in the process of H₂ production and utilization and CO₂ reduction. The paper also focuses on the H₂ mediated indirect electron transfer process and proposes enhanced measures such as promoting the cathodic hydrogen evolution reaction, adding exogenous media and optimizing the reactor design in order to promote hydrogen production and CO₂ reduction process. This review provides theoretical basis and technological support for improving the electron transfer efficiency and target product yield of microbial electrosynthesis system.

Key words: microbial electrosynthesis, direct electron transfer, indirect electron transfer, hydrogen mediated, carbon dioxide

中图分类号:

Q936

陈高祥, 王荣昌, 蒋佳承. 微生物电合成系统阴极电子传递机制和氢介导强化措施[J]. 化工进展, 2024, 43(S1): 504-516.

CHEN Gaoxiang, WANG Rongchang, JIANG Jiacheng. Mechanism of cathodic electron transfer and hydrogen–mediated enhanced measures in microbial electrosynthesis system[J]. Chemical Industry and Engineering Progress, 2024, 43(S1): 504-516.

图/表 3

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项目	强化措施	阴极电位/电流密度/电压	产物产率	库仑效率	参考文献
阴极析氢	NiMo合金修饰的硅基底	10A/m²	4.60×10^–3mmol/h 乙酸	98.6%	[101]
	NiMo合金修饰的硅基底	10A/m²	9.16×10^–3mmol/h 甲烷	98.2%	[101]
	Ni泡沫修饰的碳毡	-0.89V(vs. SHE)	2.00g/(L·d)乙酸	—	[48]
	Mo₂C修饰的碳毡	-1.05V(vs. Ag/AgCl)	(0.15±0.01)g/(L·d)乙酸	50.0% ± 0.3%	[102]
	Pt纳米颗粒/rGO修饰的碳毡	-0.90V(vs. Ag/AgCl)	26.20g/(m²·d)乙酸	—	[103]
	Sporomusa ovata生物打印的钛网	-0.80V(vs. Ag/AgCl)	(0.34±0.12)g/(L·d)乙酸	55.0% ± 20.1%	[104]
	800℃煅烧ZIF-67修饰的碳毡	-1.05V(vs. Ag/AgCl)	0.19g/(L·d)乙酸	—	[105]
	不锈钢金属网修饰的碳毡	1.00V	(163.00±13.50)mmol/(m²·d)甲烷	—	[106]
	阴极室增设析氢钛网阴极	-0.90V(vs. Ag/AgCl)	0.68~0.70g/(L·d)乙酸	66.0% ± 12.0%	[107]
投加介质	全氟化碳纳米乳液	-1.02V(vs. SHE)	1.1mmol/h乙酸	100%	[108]
	多孔聚氨酯颗粒	133A/m²	1.48g/(L·d)乙酸	最大38.0%	[109]
	SiO₂纳米颗粒	39A/m²	2.14g/(L·d)乙酸	36.0%	[98]
	Fe₃O₄纳米颗粒	—	—	—	[110]
反应器设计	电解氢移动床生物膜反应器	111A/m²	1.42L/(L·d )甲烷	—	[42]
	电产氢气泡柱反应器	156A/m²	1.15g/(L·d)乙酸	最大92.0%	[111]
	反应器内部引入导流筒	337A/m²	3.10g/(L·d)乙酸	53.0%	[112]
	设计圆柱形碳毡电极	-1.50V(vs. Ag/AgCl)	12.88mmol /L乙酸	88.0%	[113]
	增设顶空气体循环装置	-0.90V(vs. Ag/AgCl)	0.68~0.70g/(L·d)乙酸	66.0%±12.0%	[107]

项目	强化措施	阴极电位/电流密度/电压	产物产率	库仑效率	参考文献
阴极析氢	NiMo合金修饰的硅基底	10A/m²	4.60×10^–3mmol/h 乙酸	98.6%	[101]
	NiMo合金修饰的硅基底	10A/m²	9.16×10^–3mmol/h 甲烷	98.2%	[101]
	Ni泡沫修饰的碳毡	-0.89V(vs. SHE)	2.00g/(L·d)乙酸	—	[48]
	Mo₂C修饰的碳毡	-1.05V(vs. Ag/AgCl)	(0.15±0.01)g/(L·d)乙酸	50.0% ± 0.3%	[102]
	Pt纳米颗粒/rGO修饰的碳毡	-0.90V(vs. Ag/AgCl)	26.20g/(m²·d)乙酸	—	[103]
	Sporomusa ovata生物打印的钛网	-0.80V(vs. Ag/AgCl)	(0.34±0.12)g/(L·d)乙酸	55.0% ± 20.1%	[104]
	800℃煅烧ZIF-67修饰的碳毡	-1.05V(vs. Ag/AgCl)	0.19g/(L·d)乙酸	—	[105]
	不锈钢金属网修饰的碳毡	1.00V	(163.00±13.50)mmol/(m²·d)甲烷	—	[106]
	阴极室增设析氢钛网阴极	-0.90V(vs. Ag/AgCl)	0.68~0.70g/(L·d)乙酸	66.0% ± 12.0%	[107]
投加介质	全氟化碳纳米乳液	-1.02V(vs. SHE)	1.1mmol/h乙酸	100%	[108]
	多孔聚氨酯颗粒	133A/m²	1.48g/(L·d)乙酸	最大38.0%	[109]
	SiO₂纳米颗粒	39A/m²	2.14g/(L·d)乙酸	36.0%	[98]
	Fe₃O₄纳米颗粒	—	—	—	[110]
反应器设计	电解氢移动床生物膜反应器	111A/m²	1.42L/(L·d )甲烷	—	[42]
	电产氢气泡柱反应器	156A/m²	1.15g/(L·d)乙酸	最大92.0%	[111]
	反应器内部引入导流筒	337A/m²	3.10g/(L·d)乙酸	53.0%	[112]
	设计圆柱形碳毡电极	-1.50V(vs. Ag/AgCl)	12.88mmol /L乙酸	88.0%	[113]
	增设顶空气体循环装置	-0.90V(vs. Ag/AgCl)	0.68~0.70g/(L·d)乙酸	66.0%±12.0%	[107]

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