微生物电合成技术转化二氧化碳研究进展

doi:10.12211/2096-8280.2023-107

合成生物学 ›› 2024, Vol. 5 ›› Issue (5): 1142-1168.DOI: 10.12211/2096-8280.2023-107

微生物电合成技术转化二氧化碳研究进展

陈雨¹^,², 张康¹^,², 邱以婧¹^,², 程彩云¹^,², 殷晶晶¹^,², 宋天顺¹^,², 谢婧婧¹^,²

^1.南京工业大学材料化学工程国家重点实验室，江苏南京 211816
^2.南京工业大学生物与制药工程学院，江苏南京 211816

收稿日期:2023-12-15 修回日期:2024-04-16 出版日期:2024-10-31 发布日期:2024-11-20
通讯作者: 宋天顺,谢婧婧
作者简介:陈雨（1999—），男，硕士研究生。研究方向为微生物电合成还原CO2。 E-mail：925157378@qq.com
宋天顺（1981—），男，学科教授，硕士生导师。研究方向为微生物技术在废弃物资源化方面的应用。 E-mail：tshsong@njtech.edu.cn
谢婧婧（1981—），女，教授，博士生导师。研究方向为高效生物催化剂在化学品的绿色制造中的应用。 E-mail：xiej@njtech.edu.cn
基金资助:
国家重点研发计划(2018YFA0901300);国家自然科学基金(22078149);江苏省自然科学基金(BK20220002)

Progress of microbial electrosynthesis for conversion of CO₂

Yu CHEN¹^,², Kang ZHANG¹^,², Yijing QIU¹^,², Caiyun CHENG¹^,², Jingjing YIN¹^,², Tianshun SONG¹^,², Jingjing XIE¹^,²

^1.State Key Laboratory of Materials-Oriented Chemical Engineering，Nanjing Tech University，Nanjing 211816，Jiangsu，China
^2.College of Biotechnology and Pharmaceutical Engineering，Nanjing Tech University，Nanjing 211816，Jiangsu，China

Received:2023-12-15 Revised:2024-04-16 Online:2024-10-31 Published:2024-11-20
Contact: Tianshun SONG, Jingjing XIE

摘要/Abstract

摘要：

为了实现碳中和绿色经济，人们利用生物炼制技术对二氧化碳（CO₂）进行转化利用。其中，微生物电合成（MES）是通过电能驱动生物催化剂将CO₂转化为化学品的新兴技术。目前MES仍存在微生物固碳效率低、电子传递机制未明确、产品合成速率低、反应器元件适用性差等问题，这成为其规模化应用的限制因素。本文基于阴极微生物获得电子的途径，系统综述了电极、H₂、甲酸、CO以及其他电子供体在MES系统内的电子供给机制。通过合成生物学改造电活性微生物的导电纳米线，优化微生物相关氢化酶、甲酸脱氢酶和CO脱氢酶的表达是提高电子传递效率的有效方法。进一步通过阴极修饰，强化微生物-电极间电子传递速率、提高生物相容性，提供更多的还原力有利于高附加值产物的生成。除了增强阴极的电子传递效率，构建具有高效气液固传质和电子传递的反应器、降低阳极电解水电位和调控微生物活性等也被证明是提高MES性能的重要策略。未来需要进一步解析微生物电子传递机制，利用合成生物群落的方式强化MES的性能，并构建更加高效的电极界面，兼顾电子传递速率、底物传质和生物相容性。反应装置放大方面，可通过多种方式的结合来提升电子传递和气体传质，并将产物的分离也融合在一起，推动该技术的进一步发展，为“双碳”目标的实现提供新思路。

关键词: 微生物电合成, CO₂转化, 电子传递机制, 化学品, 合成生物学

Abstract:

In order to achieve carbon neutrality and green economy, people use biorefinery technology to transform and utilize CO₂. Microbial electrosynthesis (MES) is an emerging technology that converts CO₂ into chemicals by electrically driven biocatalysts. Currently, the low efficiency of microbial carbon sequestration, an incomplete understanding of electron transfer mechanisms, low synthesis rate, and poor applicability of reactor components have been the limiting factors for the large-scale application of MES. In this paper, the mechanisms of electron supply in the MES system, including through electrodes and electron donors such as H₂, formic acid, CO, and other molecules, are systematically reviewed based on how cathodic microorganisms obtain electrons. It is an effective method to improve electron transport efficiency by modifying conductive nanowires of electroactive microorganisms and optimizing the expression of microbially associated hydrogenase, formate dehydrogenase and CO dehydrogenase using synthetic biology techniques. Additionally, cathode modification aimed at improving electron transfer rates between microbes and electrodes, enhancing the biocompatibility, and providing more reducing power can facilitate the generation of value-added products. In addition to enhancing the electron transfer efficiency of the cathode, the construction of a reactor with high efficiency of gas-liquid-solid mass transfer and electron transfer, the reduction of anode potential for water electrolysis, and the regulation of microbial activity are also important strategies to enhance MES performance. In the future, it is necessary to further elucidate the mechanism of microbial electron transport and strengthen the performance of MES by means of synthetic biological communities, and by designing a more efficient electrode interface that balances electron transfer rate, substrate mass transfer and biocompatibility. In terms of the scaling-up of reaction devices, electron transfer and gas mass transfer can be improved through the combination of various methods, and integrating product separation processes can promote the further development of the technology and provide new ideas for the realization of the “Carbon Peak and Carbon Neutrality” goal.

Key words: microbial electrosynthesis, CO₂ conversion, electron transfer mechanisms, chemicals, synthetic biology

中图分类号:

Q816

陈雨, 张康, 邱以婧, 程彩云, 殷晶晶, 宋天顺, 谢婧婧. 微生物电合成技术转化二氧化碳研究进展[J]. 合成生物学, 2024, 5(5): 1142-1168.

Yu CHEN, Kang ZHANG, Yijing QIU, Caiyun CHENG, Jingjing YIN, Tianshun SONG, Jingjing XIE. Progress of microbial electrosynthesis for conversion of CO₂[J]. Synthetic Biology Journal, 2024, 5(5): 1142-1168.

图/表 10

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电子供体方式	基本原理	优势	缺点
电极	通过纳米导线和细胞色素蛋白与电极的物理接触实现电子传递	无需电子穿梭体，电子利用率高	电子传递距离短
H₂	通过微生物体内的氢化酶将H₂氧化以实现电子的释放传递	电子穿梭体来源简单，生物相容性好	氢气溶解度低，电子利用率低
甲酸	通过甲酸脱氢酶氧化释放电子，或直接被同化间接提供电子	甲酸溶解度高，生物相容性好	对微生物具有低毒性，大量的积累会影响pH
CO	通过一氧化碳脱氢酶氧化释放电子，或直接被同化间接提供电子	既可以作为电子供体又可以作为底物	对微生物体内的酶具有毒性，溶解度低
有机/人工	微生物相关代谢途径提供额外还原力的氧化还原反应	有利于碳链延长，获取高附加值产物	有机电子需要不断外源添加，部分人工电子介体对微生物有毒害作用

电子供体方式	基本原理	优势	缺点
电极	通过纳米导线和细胞色素蛋白与电极的物理接触实现电子传递	无需电子穿梭体，电子利用率高	电子传递距离短
H₂	通过微生物体内的氢化酶将H₂氧化以实现电子的释放传递	电子穿梭体来源简单，生物相容性好	氢气溶解度低，电子利用率低
甲酸	通过甲酸脱氢酶氧化释放电子，或直接被同化间接提供电子	甲酸溶解度高，生物相容性好	对微生物具有低毒性，大量的积累会影响pH
CO	通过一氧化碳脱氢酶氧化释放电子，或直接被同化间接提供电子	既可以作为电子供体又可以作为底物	对微生物体内的酶具有毒性，溶解度低
有机/人工	微生物相关代谢途径提供额外还原力的氧化还原反应	有利于碳链延长，获取高附加值产物	有机电子需要不断外源添加，部分人工电子介体对微生物有毒害作用

Electron donor	Inoculum	Cathode	Potentiostatic control (Ag/AgCl)	Average production rate	Reference
electrodes	mixed culture	rGO-Biofilm	-1.05 V	Acetate:0.17 g/(L·d)	[51]
electrodes	mixed culture	3D graphere-nickel foam	-1.05 V	Acetate:0.186 g/(L·d)	[52]
electrodes	mixed culture	CNT-MXene@Sponge	-0.8 V	Butyrate: 0.156 g/(L·d)	[53]
electrodes	mixed culture	Graphite particle	-0.79 V	Acetate:0.525 g/(L·d)	[54]
electrodes	mixed culture	EPD-3D	10 mA/m²	Acetate:0.685 g/(m²·d)	[55]
electrodes	Sporomusaovata	nickel nanowires anchored to graphite	-0.6 V	Acetate: 17.04 g/(m²·d)	[56]
electrodes	Sporomusaovata	Functionalization with chitosan	-0.6 V	Acetate: 13.74 g/(m²·d)	[57]
H₂	Sporomusaovata	PANI-modified GDEs	-1.0 V	Acetate: 0.554 g/(L·d) Butyrate: 0.0122 g/(L·d)	[76]
H₂	mixed culture	Mo₂C	-1.05 V	Acetate: 0.19 g/(L·d)	[58]
H₂	mixed culture	MoS₂	-1.05 V	Acetate: 0.2 g/(L·d)	[77]
H₂	mixed culture	Pr0.5BSCF-CF	-1.05 V	Acetate: 0.24 g/(L·d)	[78]
H₂	R.eutropha	Co-P	2 V	PHB: 0.14 g/(L·d)	[79]
H₂	C.ljungdahlii	Graphene oxide and Shewanella oneidensis MR-1	-1.05 V	Acetate: 0.18 g/(L·d) Butyrate: 0.07 g/(L·d)	[80]
H₂	Serratiamarcescens Q1	WO₃/MoO₃/g-C₃N₄	-1.3 V	Acetate: 0.19 g/(L·d)	[81]
H₂	Serratiamarcescens Q1	Ag₃PO₄/g-C₃N₄	-1.3 V	Acetate: 0.32 g/(L·d)	[82]
H₂	Serratiamarcescens Q1	MnFe₂O₄/g-C₃N₄	-1.3 V	Acetate: 0.51 g/(L·d)	[83]
H₂	mixed culture	CuO/g-C₃N₄	-1.05 V	Acetate: 0.16 g/(L·d)	[85]
H₂	mixed culture	CuO/g-C₃N₄/rGO	-0.9 V	Acetate: 0.27 g/(L·d)	[86]
H₂	mixed culture	α-Fe₂O₃/g-C₃N₄	-0.9 V	Acetate: 0.33 g/(L·d)	[87]
formate	mixed culture	Sn	-1.3 V	Acetate: 0.32 g/(L·d)	[96]
formate	R.eutropha	Sn-GDE	-1.75 V	PHB: 0.276 g/(L·d)	[97]
formate	mixed culture	Bi₂O₃	-1.23 V	Acetate: 0.269 g/(L·d)	[98]
CO	C.ljungdahlii	cobalt phthalocyanine	-1.2 V	Acetate: 1.4 g/(L·d) Ethanol: 0.87 g/(L·d)	[105]
ethanol	mixed culture	CF	10 mA/m²	Butyrate: 0.17 g/(L·d) Caproate: 2.41 g/(L·d)	[106]
ethanol / lactate	mixed culture	CF	-1.05 V	Butyrate: 0.92 g/(L·d) Caproate: 0.23 g/(L·d)	[107]
glucose	mixed culture	CF	-1.0 V	Acetate: 0.1 g/(L·d) Butyrate: 0.036 g/(L·d) Caproate: 0.012 g/(L·d)	[108]
formate / ethanol	mixed culture	CF	-1.0 V	Butyrate: 0.06 g/(L·d) Caproate: 0.06 g/(L·d)	[88]
ethanol	mixed culture	CF	5 A/m²	Caproate: 0.33 g/(L·d)	[109]
NR	mixed culture	CF	-1.1 V	Acetate: 0.1g/L/day Butyrate: 0.036 g/(L·d)	[111]
Prussian blue	mixed culture	PB-CF	-1.05 V	Acetate: 0.2 g/(L·d)	[112]

Electron donor	Inoculum	Cathode	Potentiostatic control (Ag/AgCl)	Average production rate	Reference
electrodes	mixed culture	rGO-Biofilm	-1.05 V	Acetate:0.17 g/(L·d)	[51]
electrodes	mixed culture	3D graphere-nickel foam	-1.05 V	Acetate:0.186 g/(L·d)	[52]
electrodes	mixed culture	CNT-MXene@Sponge	-0.8 V	Butyrate: 0.156 g/(L·d)	[53]
electrodes	mixed culture	Graphite particle	-0.79 V	Acetate:0.525 g/(L·d)	[54]
electrodes	mixed culture	EPD-3D	10 mA/m²	Acetate:0.685 g/(m²·d)	[55]
electrodes	Sporomusaovata	nickel nanowires anchored to graphite	-0.6 V	Acetate: 17.04 g/(m²·d)	[56]
electrodes	Sporomusaovata	Functionalization with chitosan	-0.6 V	Acetate: 13.74 g/(m²·d)	[57]
H₂	Sporomusaovata	PANI-modified GDEs	-1.0 V	Acetate: 0.554 g/(L·d) Butyrate: 0.0122 g/(L·d)	[76]
H₂	mixed culture	Mo₂C	-1.05 V	Acetate: 0.19 g/(L·d)	[58]
H₂	mixed culture	MoS₂	-1.05 V	Acetate: 0.2 g/(L·d)	[77]
H₂	mixed culture	Pr0.5BSCF-CF	-1.05 V	Acetate: 0.24 g/(L·d)	[78]
H₂	R.eutropha	Co-P	2 V	PHB: 0.14 g/(L·d)	[79]
H₂	C.ljungdahlii	Graphene oxide and Shewanella oneidensis MR-1	-1.05 V	Acetate: 0.18 g/(L·d) Butyrate: 0.07 g/(L·d)	[80]
H₂	Serratiamarcescens Q1	WO₃/MoO₃/g-C₃N₄	-1.3 V	Acetate: 0.19 g/(L·d)	[81]
H₂	Serratiamarcescens Q1	Ag₃PO₄/g-C₃N₄	-1.3 V	Acetate: 0.32 g/(L·d)	[82]
H₂	Serratiamarcescens Q1	MnFe₂O₄/g-C₃N₄	-1.3 V	Acetate: 0.51 g/(L·d)	[83]
H₂	mixed culture	CuO/g-C₃N₄	-1.05 V	Acetate: 0.16 g/(L·d)	[85]
H₂	mixed culture	CuO/g-C₃N₄/rGO	-0.9 V	Acetate: 0.27 g/(L·d)	[86]
H₂	mixed culture	α-Fe₂O₃/g-C₃N₄	-0.9 V	Acetate: 0.33 g/(L·d)	[87]
formate	mixed culture	Sn	-1.3 V	Acetate: 0.32 g/(L·d)	[96]
formate	R.eutropha	Sn-GDE	-1.75 V	PHB: 0.276 g/(L·d)	[97]
formate	mixed culture	Bi₂O₃	-1.23 V	Acetate: 0.269 g/(L·d)	[98]
CO	C.ljungdahlii	cobalt phthalocyanine	-1.2 V	Acetate: 1.4 g/(L·d) Ethanol: 0.87 g/(L·d)	[105]
ethanol	mixed culture	CF	10 mA/m²	Butyrate: 0.17 g/(L·d) Caproate: 2.41 g/(L·d)	[106]
ethanol / lactate	mixed culture	CF	-1.05 V	Butyrate: 0.92 g/(L·d) Caproate: 0.23 g/(L·d)	[107]
glucose	mixed culture	CF	-1.0 V	Acetate: 0.1 g/(L·d) Butyrate: 0.036 g/(L·d) Caproate: 0.012 g/(L·d)	[108]
formate / ethanol	mixed culture	CF	-1.0 V	Butyrate: 0.06 g/(L·d) Caproate: 0.06 g/(L·d)	[88]
ethanol	mixed culture	CF	5 A/m²	Caproate: 0.33 g/(L·d)	[109]
NR	mixed culture	CF	-1.1 V	Acetate: 0.1g/L/day Butyrate: 0.036 g/(L·d)	[111]
Prussian blue	mixed culture	PB-CF	-1.05 V	Acetate: 0.2 g/(L·d)	[112]

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微生物电合成技术转化二氧化碳研究进展

Progress of microbial electrosynthesis for conversion of CO₂

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微生物电合成技术转化二氧化碳研究进展

Progress of microbial electrosynthesis for conversion of CO2

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Progress of microbial electrosynthesis for conversion of CO₂