Review on cathode materials for CO2 methanation assisted by microbial electrolytic cell

doi:10.16085/j.issn.1000-6613.2021-1161

Abstract

Abstract:

Integrating microbial electrolysis cell (MEC) into anaerobic digestion for enhancing methane production (MEC-AD) is a new technology that has the potential to alleviate the energy crisis and greenhouse effect. With small input of electrical energy, it uses microorganisms as catalyst to decompose organic matter into electrons and protons at the anode while producing hydrogen and methane at the cathode. In recent years, MEC has made significant progress in reactor configuration, cathode material, electron transmission method and the composition of microbial community structure. Among them, high-efficiency and low-cost cathode catalysts, which attracts researchers' attention, is crucial in transforming the idea of MEC into practice. This article reviewed the working principle of MEC-AD in biomethanation and the development status of cathode catalyst including carbon-based cathodes, metal-based cathodes and composite cathodes. The methane yield, electrochemical characteristics, biocompatibility, electron transmission method and microbial community structure of different cathode systems were systematically introduced, compared and discussed according to their advantages and disadvantages. Potential future research directions were pointed out to provide the basis for the engineering application of the MEC-AD technology.

Key words: microbial electrolysis cell (MEC), anaerobic digestion, cathode materials, carbon dioxide, methane

摘要：

微生物电解池（microbial electrolysis cell，MEC）产甲烷技术是一种有望成为缓解能源危机与温室效应的重要新型途径。它以外界输入的较小电能为能量来源，以微生物为催化剂，在阳极通过分解有机物形成电子和质子；在阴极产生氢气和甲烷。近年来，MEC在反应器构型、阴极材料设计及电子转移途径、微生物群落结构组成等方面的研究取得了重要进展，寻找高效低价的阴极材料催化剂，实现MEC从概念到应用成为相关领域的研究热点。本文综述了MEC耦合厌氧消化系统产甲烷的工作原理和常见阴极材料的发展现状；分别对碳基阴极、金属基阴极及复合阴极的甲烷产率进行了阐述；系统介绍了不同阴极系统的电子传递方式、电化学特性、生物相容性、微生物群落结构组成等属性；讨论了各类电极的优缺点，并指出了今后的重点研究方向，以期为MEC耦合厌氧消化产甲烷技术的工程应用提供基础。

关键词: 微生物电解池, 厌氧消化, 阴极材料, 二氧化碳, 甲烷

CLC Number:

ZHENG Xiaomei, LIN Rujing, ZHOU Wenjing, XU Ling, ZHANG Hongning, ZHANG Xinying, XIE Li. Review on cathode materials for CO₂ methanation assisted by microbial electrolytic cell[J]. Chemical Industry and Engineering Progress, 2022, 41(5): 2476-2486.

郑小梅, 林茹晶, 周文静, 徐泠, 张洪宁, 张昕颖, 谢丽. 微生物电解池辅助CO₂甲烷化阴极材料的研究进展[J]. 化工进展, 2022, 41(5): 2476-2486.

Figures/Tables 4

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阴极材料	电极尺寸	反应器构型	接种培养物	基质	运行方式 /时间	温度/℃	阴极电势（vs. Ag/AgCl）/V	甲烷产率	CE/%	参考文献
活性炭颗粒	1.5g	单室	厌氧污泥（5.9g/L）	乙酸钠（3.2g/L）	批实验	10	0.90	31mg CH₄-COD/ g VSS	60	［30］
颗粒活性炭	8.45g	双室	污水处理厂厌氧污（12.9g/L）	CO₂	半连续流	30	0.58	65L/（m²·d）	66	［26］
石墨颗粒	27.6g	双室	污水处理厂厌氧污（12.9g/L）	CO₂	半连续流	30	0.9	62L/（m²·d）	67	［26］
颗粒活性炭	13.87g	双室	稳定MEC出水	乙酸钠（1.64g/L）	批实验	30	2.0~3.0	15.12m³/（m³·d）	71.76	［29］
碳毡	60cm²	单室	市政污泥池厌氧污泥（10g/L）	蜜糖（44.7g/L）	批实验	34	0.5	65.5mL/（L·d）	—	［31］
碳毡	60cm²	单室	市政污泥池厌氧污泥（10g/L）	蜜糖（44.7g/L）	批实验	34	1	127.5mL/（L·d）	—	［31］
碳布	4×10cm	单室	嗜热阳极MFC出水	乙酸钠（0.8g_COD/L）	批实验	55	0.8	1103mmol/ （m²·d）	—	［32］
碳纤维刷	Φ2.5cm×12cm	单室	发酵罐厌氧菌群接种物（17.083g/L）	葡萄糖（4g/L）	批实验	35	0.8	0.37L/g_COD	29	［33］
碳棒	Φ0.5×10cm	双室	厌氧污泥	CO₂	批实验	35	0.6~0.1	0.46mL/h	—	［34］
碳棒	Φ25×80mm	单室	污水处理厂厌氧污泥（43g/L）	活性污泥（41g/L）	批实验	37	0.6	2998.4mL	—	［35］
石墨毡	20cm²	三室	厌氧污泥（5.7g/L）	碳酸氢钠（5g/L）	批实验	—	0.8	0.0015L/（m²·d）	2.6	［36］
							1.1	7.2L/（m²·d）	20.3
							1.3	8.8L/（m²·d）	69.4

阴极材料	电极尺寸	反应器构型	接种培养物	基质	运行方式 /时间	温度/℃	阴极电势（vs. Ag/AgCl）/V	甲烷产率	CE/%	参考文献
活性炭颗粒	1.5g	单室	厌氧污泥（5.9g/L）	乙酸钠（3.2g/L）	批实验	10	0.90	31mg CH₄-COD/ g VSS	60	［30］
颗粒活性炭	8.45g	双室	污水处理厂厌氧污（12.9g/L）	CO₂	半连续流	30	0.58	65L/（m²·d）	66	［26］
石墨颗粒	27.6g	双室	污水处理厂厌氧污（12.9g/L）	CO₂	半连续流	30	0.9	62L/（m²·d）	67	［26］
颗粒活性炭	13.87g	双室	稳定MEC出水	乙酸钠（1.64g/L）	批实验	30	2.0~3.0	15.12m³/（m³·d）	71.76	［29］
碳毡	60cm²	单室	市政污泥池厌氧污泥（10g/L）	蜜糖（44.7g/L）	批实验	34	0.5	65.5mL/（L·d）	—	［31］
碳毡	60cm²	单室	市政污泥池厌氧污泥（10g/L）	蜜糖（44.7g/L）	批实验	34	1	127.5mL/（L·d）	—	［31］
碳布	4×10cm	单室	嗜热阳极MFC出水	乙酸钠（0.8g_COD/L）	批实验	55	0.8	1103mmol/ （m²·d）	—	［32］
碳纤维刷	Φ2.5cm×12cm	单室	发酵罐厌氧菌群接种物（17.083g/L）	葡萄糖（4g/L）	批实验	35	0.8	0.37L/g_COD	29	［33］
碳棒	Φ0.5×10cm	双室	厌氧污泥	CO₂	批实验	35	0.6~0.1	0.46mL/h	—	［34］
碳棒	Φ25×80mm	单室	污水处理厂厌氧污泥（43g/L）	活性污泥（41g/L）	批实验	37	0.6	2998.4mL	—	［35］
石墨毡	20cm²	三室	厌氧污泥（5.7g/L）	碳酸氢钠（5g/L）	批实验	—	0.8	0.0015L/（m²·d）	2.6	［36］
							1.1	7.2L/（m²·d）	20.3
							1.3	8.8L/（m²·d）	69.4

阴极材料	电极尺寸	反应器构型	接种培养物	基质	运行方式	温度/℃	阴极电势（vs. Ag/AgCl）/V	甲烷产率	CE/%	参考文献
不锈钢	22×7cm	双室	实验室稳定运行厌氧消化系统的厌氧污泥，64.2g/L	乙酸钠（7.3g/L）	批实验	25	0.4/1.0	1.08/1.18L/ （L·d）	—	［39］
热处理不锈钢毡	20cm²	三室	厌氧污泥，5.7g/L	碳酸氢钠（5g/L）	批实验	—	-0.8	0.02L/（m²·d）	2.4	［36］
							-1.1	1.0L/（m²·d）	32.9
							-1.3	7.2L/（m²·d）	60.8
不锈钢毡							-0.8	0.08L/（m²·d）	10.0
							-1.1	0.3L/（m²·d）	22.9
							-1.3	5.14L/（m²·d）	56.9
不锈钢	135cm²	单室	消化污泥+活性污泥， 5.2 gVSS/L	活性污泥（7.89g_COD/L）	批实验	22.5	1.2	25.6mL/d	—	［49］
不锈钢	10.0×7.6cm	单室	活性污泥	乙酸钠（10g/L）	批实验	25	1	225.5mL/g_COD	—	［50］
								272mL/g_COD
								360mL/g_COD
泡沫镍	Φ3cm×0.5mm	单室	实验室稳定运行的MEC出水，14g/L	废水活性污泥	批实验	35	0.8	145L/d	—	［41］

阴极材料	电极尺寸	反应器构型	接种培养物	基质	运行方式	温度/℃	阴极电势（vs. Ag/AgCl）/V	甲烷产率	CE/%	参考文献
不锈钢	22×7cm	双室	实验室稳定运行厌氧消化系统的厌氧污泥，64.2g/L	乙酸钠（7.3g/L）	批实验	25	0.4/1.0	1.08/1.18L/ （L·d）	—	［39］
热处理不锈钢毡	20cm²	三室	厌氧污泥，5.7g/L	碳酸氢钠（5g/L）	批实验	—	-0.8	0.02L/（m²·d）	2.4	［36］
							-1.1	1.0L/（m²·d）	32.9
							-1.3	7.2L/（m²·d）	60.8
不锈钢毡							-0.8	0.08L/（m²·d）	10.0
							-1.1	0.3L/（m²·d）	22.9
							-1.3	5.14L/（m²·d）	56.9
不锈钢	135cm²	单室	消化污泥+活性污泥， 5.2 gVSS/L	活性污泥（7.89g_COD/L）	批实验	22.5	1.2	25.6mL/d	—	［49］
不锈钢	10.0×7.6cm	单室	活性污泥	乙酸钠（10g/L）	批实验	25	1	225.5mL/g_COD	—	［50］
								272mL/g_COD
								360mL/g_COD
泡沫镍	Φ3cm×0.5mm	单室	实验室稳定运行的MEC出水，14g/L	废水活性污泥	批实验	35	0.8	145L/d	—	［41］

阴极材料	电极尺寸	反应器构型	接种培养物	基质	运行方式	温度/℃	阴极电势（vs. Ag/AgCl）/V	甲烷产率	CE/%	参考文献
Pt-碳毡	0.5mg/cm²	双室	厌氧污泥， 6.6gVss/L	乙酸钠	批实验	35	0.8	0.91m³/m³	71.7	［83］
Pt修饰碳布	Φ40mm； 0.5mg/cm²	单室	污水处理厂曝气池出水	1.5g/L 乙酸钠	批实验	20～25	0.8	91.8g/（m³·d）	102.7±4.5	［51］
Pt-石墨块	2cm×2cm×0.32cm	双室	市政污水处理厂二级消化厌氧消化泥	乙酸钠	批实验	30	0.6	250nmol/（m³·d）	100	［52］
Pt-碳布	Φ3cm； 0.5mg/cm²	单室	酸化处理后的二沉池厌氧消化污泥	—	批实验	20	0.8	0.0564m³/（m³·d）	—	［53］
Pt-碳布	0.5mg/cm²	单室	初沉池出水	1g/L乙酸钠	批实验	30	0.8	93L/（m³·d）	82	［55］
Pt-钛网	4cm×5cm	三室	初沉池出水	CO₂	批实验+ 连续流	22	1.2～1.5	CH₄含量98.1%	32.6	［84］
磁铁矿/ 沸石-碳布	2.5cm×4cm	单室	厌氧二级发酵罐厌氧污泥，16.883g/L	葡萄糖	批实验	35	0.8	238mL/（L·d）	52.3	［69］

Review on cathode materials for CO₂ methanation assisted by microbial electrolytic cell

微生物电解池辅助CO₂甲烷化阴极材料的研究进展

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