一体化电极电催化二氧化碳还原研究进展

doi:10.3866/PKU.WHXB202101028

Abstract

Abstract:

The electrocatalytic carbon dioxide reduction reaction (E-CO₂RR) has attracted attention in recent years for its ability to effectively alleviate the environmental problems caused by the rapid increase of CO₂ in the atmosphere and transform CO₂ into high value-added fuels or chemicals (e.g., CO, HCOOH, CH₄, CH₃OH, C₂H₄, C₂H₅OH, etc.) under mild conditions. In addition, clean energy sources, such as solar and wind energy, can provide electrical energy for the electrochemical CO₂ conversion technology used in large-scale industrial applications. One limitation of the E-CO₂RR is that CO₂ is a thermodynamically stable linear molecule with a slow kinetic reaction rate. In addition, the E-CO₂RR involves complex processes, such as gas diffusion and multi-electron transfer, making its selectivity problematic. Therefore, constructing highly efficient and stable catalytic electrodes has become a core research topic in the field of E-CO₂RR. Unfortunately, the traditional method of coating electrodes with binders (e.g., Nafion, polyvinylidene fluoride, and polytetrafluoroethylene) usually results in a low utilization ratio of active sites due to the easy aggregation of the catalysts themselves. This could result in the severe embedding of active sites and limited mass transfer. Moreover, the dissolution of the catalyst layer during the electrocatalytic process also reduces the activity and stability of the electrodes, making it difficult to reuse. Therefore, it is necessary to regulate the electrode reaction interface to improve the utilization ratio of active sites. The integrated electrodes, where the catalyst is grown directly on the current collector, can avoid the use of binders to facilitate the exposure of active sites and transfer of electrons. The integrated structure can also enhance the bonding strength between the active material and current collector and improve the cycling stability of the electrodes. Meanwhile, the micro-environment (e.g., pH, concentration of CO₂, and intermediates) at the three-phase interface can be effectively controlled on the integrated electrodes, which can enhance the performance of the E-CO₂RR. In recent years, encouraging progress has been achieved in the study of the E-CO₂RR. However, current reviews of the E-CO₂RR mainly focus on the regulation of the intrinsic activity of catalysts; discussions and reviews from the perspective of the electrodes are rarely reported. This article reviews the latest research of the integrated electrodes for the E-CO₂RR with a focus on the application of different types of integrated electrodes (e.g., metal, alloy, metal oxide, metal sulfide/phosphide, and metal single atom). It also analyzes the effects of morphology, surface, and interface regulation on the electrocatalytic performance of the E-CO₂RR. Finally, it highlights the challenges that still exist in this field and discusses the future development of the integrated electrodes.

Key words: Integrated electrode, Electrocatalysis, Carbon dioxide reduction reaction, Structural design, Interface regulation

Yuke Song, Wenfu Xie, Mingfei Shao. Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction[J]. Acta Phys. -Chim. Sin. 2022, 38(6), 2101028. doi: 10.3866/PKU.WHXB202101028

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References 145

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Catalyst	Product	Electrolyte	Potential/(V vs. RHE)	FE/%	j/(mA·cm^-2)	Stability/h	Ref.
Zn	CO	1.0 mol·L^-1 KOH	-0.62	91.6	-200 (flow cell)	18	40
Hierarchical CoS₂ nanocages	CO	0.5 mol·L^-1 KHCO₃	-0.6	85.7	-3.3	-	46
Au₃Cu	CO	0.1 mol·L^-1 KHCO₃	-0.7	98.12	-12.77	80	72
NiSA/PCFM	CO	0.5 mol·L^-1 KHCO₃	-1.0	88	-350.4 (flow cell)	120	108
Ag-deposited Ti GDE	CO	1.0 mol·L^-1 KHCO₃	-	67.3	-	-	111
NSHCF900	CO	0.5 mol·L^-1 KHCO₃	-0.7	94	-109.5	36	112
Bi nanodendrite	HCOO^-/HCOOH	0.5 mol·L^-1 NaHCO₃	-1.8 (vs. SCE)	96.4	-15.2	10	42
mPd/TNTAs	HCOO^-/HCOOH	0.5 mol·L^-1 NaHCO₃	-0.1	88±2	–	4	57
Bi nanoflaks@Cu film	HCOO^-/HCOOH	0.1 mol·L^-1 KHCO₃	-0.6	100	-	10	62
V_O-SnO_x/CF-40	HCOO^-/HCOOH	0.1 mol·L^-1 KHCO₃	-1.0	86	-34.9	8	78
NiSn-APC	HCOO^-/HCOOH	0.5 mol·L^-1 KHCO₃	-0.82	86.1	-43.7	23	110
CuS-NW@NF	CH₄	0.1 mol·L^-1 KHCO₃	-1.1	73±5	-	60	99
Oxide-derived Cu	CH₄	0.1 mol·L^-1 CsHCO₃	-1.2	62	-29	-	113
Plasma-Cu	C₂H₄	0.1 mol·L^-1 NaHCO₃	-0.9	60	-	1	114
Cu₂O films	C₂H₄	0.1 mol·L^-1 KHCO₃	-0.99	39	-11.7	-	115
Porous copper foil	C₂H₄	0.1 mol·L^-1 KHCO₃	-1.3	35	-57	1.4	116
FeP NA/TM	CH₃OH	0.5 mol·L^-1 KHCO₃	-0.2	80.2	-	36	100
CuSAs/TCNFs	CH₃OH	0.1 mol·L^-1 KHCO₃	-0.9	44	-90	50	117
Zn dendrites	CH₃OH	0.5 mol·L^-1 KHCO₃	-0.2	10.5	-26	-	118
AgCu wire	C₂H₅OH	1.0 mol·L^-1 KOH	-0.68	30	-267 (flow cell)	-	22
HMMP Cu₅Zn₈	C₂H₅OH	0.1 mol·L^-1 KHCO₃	-0.8	46.6	-3.6	11	47
Cu nanocrystals	n-propanol	0.1 mol·L^-1 NaHCO₃	-0.95	14	-12	6	119
Cu nanowire arrays	n-propanol	0.1 mol·L^-1 KHCO₃	-1.1	75	-	5	120

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Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction

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