Electrochemical reduction of CO2 coupled with oxidative conversion of biomass

doi:10.16085/j.issn.1000-6613.2023-0725

Abstract

Abstract:

The large-scale use of fossil energy significantly increased CO₂ emissions. It is of great importance to decrease the dependence on fossil energy and reduce carbon emission by developing renewable energy such as biomass energy combined with the conversion and utilization of CO₂. Electroreduction driven by renewable electricity is an effective way for CO₂ conversion and utilization. In this paper, new routes for biomass utilization, electrochemical conversion of CO₂ coupled with biomass oxidative conversion were reviewed. The latest development of catalysts, reaction systems and reaction mechanisms for electrochemical reduction of CO₂, as well as new oxidative conversion technologies of biomass and its derived alcohols and aldehydes on anodes were introduced. By coupling biomass oxidative conversion with CO₂electrochemical reduction, high-value chemicals can be produced with significant reduction of the net CO₂ emission. Therefore, this paper can provide new ideas for the conversion of biomass and CO₂.

Key words: carbon dioxide, biomass, electrochemical conversion, biofuel, high-value chemicals

摘要：

化石能源的大规模使用使得大气中CO₂的含量不断增加。发展生物质能源等可再生能源，结合CO₂的转化利用对降低化石能源的依赖和减少碳排放具有重要的意义。利用可再生电能驱动CO₂的电化学还原生成燃料和化学品是CO₂转化利用的一个有效途径。本文对CO₂电化学转化以及耦合生物质氧化转化新路线的主要研究进展进行了综述。重点介绍了CO₂电化学还原的催化剂、反应系统、反应机制等方面的最新进展，以及阳极耦合生物质及其衍生醇类、醛类等氧化转化的新技术。可再生电能驱动的生物质氧化转化与CO₂电还原相耦合不仅可以获得高值化学品，而且可以显著减少CO₂的净排放。因此，本文可为生物质和CO₂转化提供新的思路。

关键词: 二氧化碳, 生物质, 电化学转化, 生物燃料, 高值化学品

CLC Number:

O646

YAN Zhe, LIU Chang, WANG Fengxu, ZHOU Hongwang, LIU Xi, ZHAO Xuebing. Electrochemical reduction of CO₂ coupled with oxidative conversion of biomass[J]. Chemical Industry and Engineering Progress, 2024, 43(6): 3310-3321.

闫哲, 刘畅, 王丰旭, 周宏旺, 刘樨, 赵雪冰. 耦合生物质氧化转化的CO₂电化学还原[J]. 化工进展, 2024, 43(6): 3310-3321.

Figures/Tables 9

还原反应方程式	标准电势/V
CO₂+e^- $→$ $C O 2 - ·$	-1.90
CO₂+2H⁺+2e^- $→$ CO+ H₂O	-0.53
CO₂+H₂O+2e^- $→$ CO+2OH^-	-1.35
CO₂+2H⁺+2e^- $→$ HCOOH	-0.61
CO₂+H₂O+2e^- $→$ HCOO^-+OH^-	-1.49
CO₂+4H⁺+4e^- $→$ HCHO+H₂O	-0.48
CO₂+3H₂O+4e^- $→$ HCHO+4OH^-	-1.31
CO₂+6H⁺+6e^- $→$ CH₃OH+H₂O	-0.38
CO₂+5H₂O+6e^- $→$ CH₃OH+6OH^-	-1.23
CO₂+8H⁺+8e^- $→$ CH₄+2H₂O	-0.24
CO₂+6H₂O+8e^- $→$ CH₄+8OH^-	-1.07
CO₂+4H⁺+4e^- $→$ C+2H₂O	-2.00
CO₂+2H₂O+4e^- $→$ C+4OH^-	-1.04
2CO₂+12H⁺+12e^- $→$ C₂H₄+4H₂O	-0.34
2CO₂+8H₂O+12e^- $→$ C₂H₄+12OH^-	-1.17
2CO₂+14H⁺+14e^- $→$ C₂H₆+4H₂O	-0.27
2CO₂+2H⁺+2e^- $→$ H₂C₂O₄	-0.91
2CO₂+2e^- $→$ C₂ $O 4 2 -$	-1.00
2CO₂+12H⁺+12e^- $→$ C₂H₅OH+3H₂O	-0.33
2CO₂+9H₂O+12e^- $→$ C₂H₅OH+12OH^-	-1.16
3CO₂+18H⁺+18e^- $→$ C₃H₇OH+5H₂O	-0.32
2H⁺+2e^- $→$ H₂	-0.42

还原反应方程式	标准电势/V
CO₂+e^- $→$ $C O 2 - ·$	-1.90
CO₂+2H⁺+2e^- $→$ CO+ H₂O	-0.53
CO₂+H₂O+2e^- $→$ CO+2OH^-	-1.35
CO₂+2H⁺+2e^- $→$ HCOOH	-0.61
CO₂+H₂O+2e^- $→$ HCOO^-+OH^-	-1.49
CO₂+4H⁺+4e^- $→$ HCHO+H₂O	-0.48
CO₂+3H₂O+4e^- $→$ HCHO+4OH^-	-1.31
CO₂+6H⁺+6e^- $→$ CH₃OH+H₂O	-0.38
CO₂+5H₂O+6e^- $→$ CH₃OH+6OH^-	-1.23
CO₂+8H⁺+8e^- $→$ CH₄+2H₂O	-0.24
CO₂+6H₂O+8e^- $→$ CH₄+8OH^-	-1.07
CO₂+4H⁺+4e^- $→$ C+2H₂O	-2.00
CO₂+2H₂O+4e^- $→$ C+4OH^-	-1.04
2CO₂+12H⁺+12e^- $→$ C₂H₄+4H₂O	-0.34
2CO₂+8H₂O+12e^- $→$ C₂H₄+12OH^-	-1.17
2CO₂+14H⁺+14e^- $→$ C₂H₆+4H₂O	-0.27
2CO₂+2H⁺+2e^- $→$ H₂C₂O₄	-0.91
2CO₂+2e^- $→$ C₂ $O 4 2 -$	-1.00
2CO₂+12H⁺+12e^- $→$ C₂H₅OH+3H₂O	-0.33
2CO₂+9H₂O+12e^- $→$ C₂H₅OH+12OH^-	-1.16
3CO₂+18H⁺+18e^- $→$ C₃H₇OH+5H₂O	-0.32
2H⁺+2e^- $→$ H₂	-0.42

产物	催化剂	法拉第效率/%	过电势/V	电流密度/mA·cm^-2	电解液
HCOOH	Pb	97.4	-1.19	5.0	0.1mol/L KHCO₃
	Sn	88.4	-1.04	5.0	0.1mol/L KHCO₃
	Pd/C	99	-0.15	2.4~7.0	2.8mol/L KHCO₃
	Pd₇₀Pt₃₀/C	90	-0.36	4.0~7.5	0.2mol/L PO₄^3–
CO	Au	87.1	-0.64	5	0.1mol/L KHCO₃
	Au NPs	97	-0.58	3.49 ± 0.61	0.1mol/L KHCO₃
	OD-Au	>96	-0.25	2~4	0.5mol/L NaHCO₃
	Ag	94	-0.99	约5	0.1mol/L KHCO₃
CH₄	铜箔	40.4	-1.34	约7	0.1mol/L KHCO₃
CH₄	Cu(210)	64	-1.29	5	0.1mol/L KHCO₃
C₂H₄	铜箔	26.0	-1.13	1~2	0.1mol/L KHCO₃
	Cu	60	-0.98	约15	0.1mol/L KHCO₃
	卤化铜	60.5~79.5	-2.11	46.1~39.2	3mol/L KBr
	石墨/碳 NPs/Cu/PTFE	70	-0.63	75~100	7mol/L KOH
CH₃OH	Cu₂O	38	-0.43	1~2	0.5mol/L KHCO₃
CH₃OH	Mo	84	-0.33	0.12	0.2mol/L Na₂SO₄
C₂H₅OH	铜箔	9.8	-1.14	约0.6	0.1mol/L KHCO₃
	Cu₂O	9~16	-1.08	30~35	0.1mol/L KHCO₃
	CuO	36.1	—	约11.7	0.2mol/L KI
	Cu/CNS	63	-1.29	2	0.1mol/L KHCO₃

阴极CO₂电化学还原反应			电流密度 /mA·cm^-2	阳极反应		电压 /V
催化剂	生成产物	法拉第效率/%	电流密度 /mA·cm^-2	催化剂	反应底物	电压 /V
Ag GDL	CO	100.9	2.29	Pt	甘油	0.9
Ag GDL	CO	98.85	4.55	Pt	葡萄糖	1.2
Sn GDL	HCOOH	85.5	82.52	Pt	甘油	2.3
Sn GDL	HCOOH	86.39	52.46	Pt	葡萄糖	1.4

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Electrochemical reduction of CO₂ coupled with oxidative conversion of biomass

耦合生物质氧化转化的CO₂电化学还原

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