Overview and prospect of studies on electrochemical reduction of carbon dioxide electrolyzers

doi:10.19799/j.cnki.2095-4239.2020.0167

Abstract

Abstract:

The electrochemical reduction of carbon dioxide can deal with the mismatch between the demand and the supply of renewable energy, such as solar energy, converting excess electrical energy into chemical storage with a high added value while reducing carbon dioxide emissions, and alleviating environmental pressure. H-type electrolytic cells have mostly been adopted in early research, and this is far from the industrial application of the carbon dioxide electrochemical reduction technology. H-cells are susceptible to mass transfer limitations and often have low current density. This study no longer focuses on the research and development of cathode catalysts, but on studies using a continuous carbon dioxide electrochemical reduction reactor. We introduce herein several types of reactor structure commonly used in the current research and discuss the components, operating conditions, possible optimization methods (e.g., novel gas diffusion electrode structure), failure mechanism of the electrolyzer, and possible repair methods. A direct comparison of the performances of the cathode catalyst would be impossible due to the difference in structure, composition, and operating parameters of the electrolyzers used in each study; therefore, the reference electrode should be a necessary part of a CO₂ electrolyzer. The possible optimization methods of the carbon dioxide electrolyzer are as follows: ① preparation technology of the catalyst layer slurry and binder selection; ② preparation technology of the gas diffusion electrode and substrate selection; ③ development of a highly efficient and long-term stable polymer electrolyte membrane; and ④ optimization of the operating parameters.

Key words: carbon dioxide, electrochemical reduction, electrolytic reactor, failure mechanism

CLC Number:

O 646

Yueyuan GU, Jucai WEI, Jindong LI, Luyang WANG, Xu WU. Overview and prospect of studies on electrochemical reduction of carbon dioxide electrolyzers[J]. Energy Storage Science and Technology, 2020, 9(6): 1691-1701.

Figures/Tables 7

Fig.1

Table 1

Specifications and main results of continuous-flow CO2 electrolyzers"

setup	membrane	current collector	catalysts		reference electrode	feeding	electrolyte composition		main results	Ref.
setup	membrane	current collector	cathode	anode	reference electrode	feeding	cathode	anode	main results	Ref.
(a)	Nafion^? 117	Al	Ag 10mg/1.5 cm²	Pt 10mg/1.5 cm²	Home-made Ag/Ag⁺	CO₂ 2.5 sccm solution 0.5 mL/min	18% EMIM BF₄	100 mM H₂SO₄	1.5～2.5 V, CO FE>96% for at least 7 hours	[32]
(d)	none	Al	Ag 0.75 mg/cm²	Pt/C 4.25 mg/cm²	External Ag/AgCl	CO₂ 7 sccm solution 0.5mL/min	1 mol/L KCl		-1.56 V vs Ag/AgCl Air-brushed , CO FE (95±5)%; hand-painted, CO FE (83±14)%	[27]
(d)	none	Al and graphite	Ag 0.9 mg/cm²	Pt 1.0 mg/cm²	none	CO₂ diluted by N₂ 7 sccm solution 0.4 mL/min	1 mol/L KCl		3 V, 10%～100% v/v CO₂, CO FE>80%	[43]
(b)	BPM	gold-coated graphite	Ag BiO_x	NiFeO_x	none	-	0.5 mol/L KHCO₃saturated with CO₂	0.1 mol/L KOH	50 mA/cm², CO FE>60%	[35]
(d)	none	Stainless steel	Ag (2±0.1) mg/cm²	IrO₂ (2±0.1) mg/cm²	Ag/AgCl (inlet)	CO₂ 17 sccm solution 0.5 mL/min	3 mol/L KOH		2.75 V, 342.8 mA/cm² CO (101.2%)	[44]
(a)	AEM	-	Ag	IrO₂	none	CO₂ 10 sccm	50% EMIMCI	0.5 mol/L H₂SO₄	50 mA/cm², CO FE 97.08% pH adjusted to 6.6, 25 mA/cm², CO FE 99.1%	[7]
(d)	none	Al	Ag 0.75 mg/cm²	Pt/C 4.25 mg/cm²	External Ag/AgCl	CO₂ 7 sccm solution 0.5mL/min	1 mol/L KCl		-1.62 V vs Ag/AgCl (cell potential 3V), CO FE ～98%, partial current density ～90mA/cm²	[31]
(d)	none	Al	CN/MWCNT 2.39 mg/cm²	Pt/C 4.25 mg/cm²	External Ag/AgCl	CO₂ 7 sccm solution 0.5mL/min	1 mol/L KCl		-1.68 V vs Ag/AgCl (cell potential 3V), CO FE ～93%, partial current density ～86 mA/cm²	[31]
(c)	CEM	Ti	Ag or Cu (5mg/cm²)	IrO₂ (2mg/cm²)	Ag/AgCl	CO₂ 4.5 sccm	0.5 mol/L K₂SO₄		Cu, -0.8 V vs. RHE, CO FE ～75% Ag, -0.8 V vs. RHE, CO FE ～80%	[13]
(d)	none	Al	MWNT/PyPBI/Au 0.34 mg/cm²	Pt /C 4.25 mg/cm²	Ag/AgCl (outlet)	CO₂ 7 sccm solution 0.5 mL/min	1 mol/L KCl		-1.4 V vs Ag/AgCl, CO FE 92%	[30]
(d)	none	stainless steel	MWNT/PyPBI/Au (1±0.1) mg/cm²	IrO₂ (4.25±0.25) mg/cm²	Ag/AgCl (inlet)	CO₂ 17 sccm solution 0.5mL/min	2 mol/L KOH		-0.22 V vs RHE (cell potential-1.7 V) CO FE 98.3%	[29]
(b)	CEM	titanium	Cu	IrO₂	none	both 100 sccm	CO₂	humidified N₂（25、50、75%）	relative humidity 72.5%, 30 ^oC, 6 V Hydrocarbons FE 0.12%; relative humidity 73.7 %, 70 ^oC, 2.4 V hydrocarbons FE 0.11%	[11]
(a)	AEM	Stainless steel	Cu 1.0 mg/cm²	IrO₂ 1.0 mg/cm²	Ag/AgCl (outlet)	CO₂ 7 sccm; solution 0.5 mL/min（-2～-3.5 V）0.1 mL/min (-1.6～-2 V)	1 mol/L KOH	1 mol/L KOH	-0.58 V vs. RHE, C₂H₄ and C₂H₅OH FE 46%, partial current density ～200 mA/cm²	[48]
(c)	Nafion^?117	-	Cu₂O 1 mg/cm²	Ti	Ag/AgCl	CO₂ 10～40 mL/min solution 1～3 mL/min	0.5 mol/L KHCO₃	0.5 mol/L KHCO₃	10 mA/cm²CH₃OH FE 42.3%, r_T=83.2 μmol/(m²·s^-1)	[56]
(c)	Nafion^?117	-	Cu₂O/ZnO 1mg/cm²	Ti	Ag/AgCl	CO₂ 10～40 mL/min solution 1～3 mL/min	0.5 mol/L KHCO₃	0.5 mol/L KHCO₃	10 mA/cm²CH₃OH FE 27.5%, r_T=50.8 μmol/(m²·s^-1)	[56]
(b)	PBI	carbon paper	Cu-CNF 0.5 mg/cm²	IrO₂ 0.5 mg/cm²	-	CO₂ 0.5 NmL/min N₂ 6 NmL/min	CO₂	N₂ 1 mol/L H₃PO₄saturator	110 ℃, -0.8 mA/cm², acetaldehyde FE 85%, r>24 nmol/(h·cm^-2); 110 ℃, -1.6 mA/cm², acetaldehyde FE 70%, r>55nmol/(h·cm^-2)	[12]
(b)	Nafion115 AAEM	-	1 mg/cm² Cu/CNTs Pt/C Pd/C	Pt/C	none	both 20 mL/min	humidified CO₂ (100%)	humidified H₂(100%)	40 ℃, 3V, CO, r=8.88 μmol/(h·cm^-2), r=0.75 μmol/(h·cm^-2), r=7.59 μmol/(h·cm^-2)	[10]
(c)	Nafion^?117	-	Sn 1.5 mg/cm²	DSA	Ag/AgCl	CO₂ 0.57 mL/(min·cm^-2)	0.45 mol/L KHCO₃ + 0.5 mol/L KCl	1 mol/L KOH	40 mA/cm², cell potential 3.21 V, Formate FE 70.5%	[57]
(b)	BPM	-	Sn	Ir-MMO	none	solution 10 mL/min	pressured CO₂ 0.5mol/L KHCO₃	pressured N₂ 1mol/L KOH	3.5 V, 40 bar, ～30 mA/cm², HCOOH FE ～90% 4 V, 50 bar, ～100 mA/cm², HCOOH FE ～65%	[51]
(b)	CEM	-	Sn	Ir-MMO	none	solution 10 mL/min	pressured CO₂ 1mol/L KHCO₃	pressured N₂ 0.5mol/L H₂SO₄	3.5 V, 40 bar, ～50 mA/cm², HCOOH FE ～90% 3.5 V, 50 bar, ～60 mA/cm², HCOOH FE ～80%	[51]
(d)	none	graphite	Ru–Pd/C 2 mg/cm²	Pt/C 2 mg/cm²	Ag/AgCl (outlet)	CO₂ 5sccm solution 0.5 mL/min	0.5 mol/L KHCO₃		3.25 V, HCOOH FE～ 16%, EE～ 7%	[45]
(d)	none	graphite	Sn 5 mg/cm²	Pt/C 2 mg/cm²	Ag/AgCl (outlet)	CO₂ 5sccm solution 0.5 mL/min	0.5 mol/L KCl+1mol/L HCl (pH=4)		3V, ～100 mA/cm² HCOOH FE 89%, EE 45%	[45]
(b)	Nafion117	-	1mg/cm² Pt/C Pt-Ru/C	Pt/C 1mg/cm²	DHE	Both 50 sccm	N₂or CO₂ (fully humidified)	H₂ (fully humidified)	80 ℃ ,0.06 V vs. DHE CH₃OH FE 35% CH₃OH FE 75%	[8]
(b)	Nafion^?115	titanium	PtRu/C metal 0.5 mg/cm²	IrRuO_x 0.4 mg/cm²	none	CO₂ 50 mL/min solution 4 mL/min	humidified CO₂	H₂O	40 ℃, 1.25V, CH₃OH r=0.9 μmol/(g·h^-1) 95 ℃, 1.25V, CH₃OH r=56 μmol/(g·h^-1)	[58]
(b)	Nafion 115	gold-plated graphite (anode)	Indium	Pt/C	none	-	1mol/L NaHCO₃	10%（w/v）NaOH	40 mA/cm², HCOOH FE ～77%	[59]
(b)	AEM	gold-plated graphite (anode)	Indium	Pt/C	none	-	1mol/L NaHCO₃	1 mol/L NaHCO₃	40 mA/cm², HCOOH FE 80%	[59]
(b)	Nafion117	-	Pb	DSA	Ag/AgCl	CO₂ 200 mL/min solution 1.44 mL /(min·cm^-2)	0.45 mol/L KHCO₃ + 0.5 mol/L KCl	1 mol/L KOH	10.5 mA/cm², HCOOH FE 57%	[33]
(b)	Nafion	-	N-doped graphene 0.3～0.5 mg/cm²	Pt 0.3 mg/cm²	DHE	CO₂ 45 sccm H₂ 50 sccm	CO₂	H₂	-0.58 V vs RHE, ～1.8 mA/cm², CO FE ～85% for at least 5 h	[60]
(b)	AEM	Ti	Ni-NG 0.5 mg/cm²	IrO₂ 0.5 mg/cm²	none	CO₂ 50 sccm solution 2 mL/min	humidified CO₂	0.1 mol/L KHCO₃	2.78V, ～ 50 mA/cm², CO FE >90%, for at least 8 h, 3.81 mmol/h	[61]
(b)	PSMIM AEM	Ti	Ni-NG 1.25 mg/cm²	IrO₂ 1.25 mg/cm²	none	CO₂ 50 or 500 sccm solution 2 or 10 mL/min for different area	humidified CO₂	0.1 mol/L KHCO₃	2×2 cm², 2.46V, ～80 mA/cm², CO FE～100% for 20h10×10 cm², 2.8V, ～8A, CO FE >90% for 6h, r=3.34 L/h	[47]

Table 1

Fig.2

Fig.3

Fig.4

Fig.5

Fig.6

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