Electrochemical conversion of C1 molecules to sustainable fuels in solid oxide electrolysis cells

doi:10.1016/S1872-2067(21)63838-X

Abstract

Abstract:

Stimulated by increasing environmental awareness and renewable-energy utilization capabilities, fuel cell and electrolyzer technologies have emerged to play a unique role in energy storage, conversion, and utilization. In particular, solid oxide electrolysis cells (SOECs) are increasingly attracting the interest of researchers as a platform for the electrolysis and conversion of C1 molecules, such as carbon dioxide and methane. Compared to traditional catalysis methods, SOEC technology offers two major advantages: high energy efficiency and poisoning resistance, ensuring the long-term robustness of C1-to-fuels conversion. In this review, we focus on state-of-the-art technologies and introduce representative works on SOEC-based techniques for C1 molecule electrochemical conversion developed over the past several years, which can serve as a timely reference for designing suitable catalysts and cell processes for efficient and practical conversion of C1 molecules. The challenges and prospects are also discussed to suggest possible research directions for sustainable fuel production from C1 molecules by SOECs in the near future.

Key words: Solid oxide electrolysis cells, C1 molecules, Electrolysis, Methane conversion, CO₂ conversion

Ximeng Lv, Menghuan Chen, Zhaolong Xie, Linping Qian, Lijuan Zhang, Gengfeng Zheng. Electrochemical conversion of C1 molecules to sustainable fuels in solid oxide electrolysis cells[J]. Chinese Journal of Catalysis, 2022, 43(1): 92-103.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63838-X

https://www.cjcatal.com/EN/Y2022/V43/I1/92

Figures/Tables 7

Fig. 1. (a) Annual total CO2 emissions data since 1750 (by region); (b) Schematic for sustainable industrial chain toward C1-to-fuel process; (c) Research topics in SOEC-related studies since 2000; (d) Number of citations on SOEC-related publications. Inset: the number of SOEC-related papers published since 2000.

Fig. 2. (a) Model of MEA for a typical SOEC: the fuel electrode in red color, support layer in blue color, oxygen electrode in yellow color, and reaction barrier in green color. (b) Schematic of the triple-phase-boundary at cathode: the electronic conductor phase in yellow color, oxygen ion conductor phase in grey color, and gas phase in white color. (c) Schematic of charge transfer process in OC-SOEC and PC-SOEC (PCEC), respectively. (d) Comparison of the bulk conductivity of Ba7Nb4MoO20 (i.e., black dot-line in dry air and grey dot-line in Air/H2O) with other leading ionic conductors. (e) Perovskite oxide (ABO3) crystal structure. Figure (d) was reprinted with permission from Ref. [17] Copyright 2020 Springer Nature.

Table 1 Thermodynamic data for representative C1 chemical reactions in SOECs [27].

Reaction	ΔH°_298K (kJ·mol^-1)	ΔS°_298K (J·mol^-1·K^-1)
CO₂ = CO + 1/2O₂	283	86.5
2CO = C + CO₂	-173	-176
CO₂ + H₂O = CO + H₂ + O₂	569	250
CO + H₂O = CO₂ + H₂	2.83	76.8
CH₄ + H₂O = CO + 3H₂	206	338
CH₄ + CO₂ = 2CO + 2H₂	247	257
CH₄ + CO₂ = C₂H₄ + 2H₂O	-51.2	-40.9

Fig. 3. (a) The Arrhenius plots of the area specific resistance (EaASR) and polarization resistance (EaRp) from the (La0.75Sr0.25)0.97Cr0.5Mn0.5O3-δ/GDC cathode at open-circuit voltages over a range of operating temperatures in CO2/CO (70/30) atmosphere. EaR1 and EaR2 referred to high-frequency and low-frequency polarization resistances, respectively. (b) Temperature-programmed desorption (TPD) curves of CO2 on (La0.2Sr0.8)0.95Ti0.65-xMn0.35CuxO3-δ surface, measured in the temperature range of 200 to 950 °C; (c) I-V curves of (La0.2Sr0.8)0.95Ti0.65-xMn0.35CuxO3-δ-based SOECs at 800 °C; (d) Measured outlet pCO (balance CO2) and cell overpotential corrected for iRΩ at increasing applied current densities. The dashed vertical line was the thermodynamic threshold of carbon deposition via the Boudouard reaction. Inset: Typical electrolysis current-voltage curve measured on a cell with ceria negative electrode; (e) Selected data in (d), now shown as a function of time at two of the final operating points (fixed current densities: 0.35 A·cm-2 for the ceria cell and 0.5 A·cm-2 for the Ni-YSZ cell). (f) Illustrations of the two cell types and post-test cross-sectional scanning electron microscopy images at the gas outlet near the negative electrode/electrolyte interfaces, where carbon was deposited in the Ni-YSZ electrode and caused interface delamination. Fig. (a) was reprinted with permission from Ref. [37]. Copyright 2012 The electrochemical society (IOP Publishing). Figs. (b,c) were reprinted with permission from Ref. [42]. Copyright 2020 Elsevier. Figs. (d,e,f) were reprinted with permission from Ref. [48]. Copyright 2019 Springer Nature.

Table 2 Representative materials researches on SOEC-based CO2 electrolysis in 2020.

Cell configuration	Performance	Ref.
Anode: La_0.8Sr_0.2MnO_3-_δ, Cathode: (La_0.2Sr_0.8)_0.95Ti_0.65-_xMn_0.35Cu_xO_3-_δ Electrolyte: LSGM	2.33 A·cm^-2 at 1.8 V (1073 K) Feed stock: CO₂	[42]
Anode: (La_0.60Sr_0.40)_0.95Co_0.20Fe_0.80O_3-_δ-GDC Cathode: Fe/MnO_x on (Pr,Ba)₂Mn_2-_yFe_yO₅₊_δ Electrolyte: YSZ	0.638 A·cm^-2 at 1.6 V (1123 K) Feed stock: CO₂	[44]
Anode: Sr₂Fe_1.3Co_0.2Mo_0.5O_6-_δ Cathode: Sr₂Fe_1.3Co_0.2Mo_0.5O_6-_δ Electrolyte: LSGM	2.12 A·cm^-2 at 1.4 V (1123 K) Feed stock: CO₂-CO (1:1)	[45]
Anode: NiO-YSZ Cathode: LaCo_0.6Ni_0.4O_3-_δ-GDC Electrolyte: YSZ	2.316 A·cm^-2 at 2.0 V (1073 K) Feed stock: CO₂	[46]
Anode: Sm_1-_xCa_xFe_1-_yCu_yO_3-_δ Cathode: La_0.8Sr_0.2MnO_3-_δ-GDC Electrolyte: SSZ	1.20 A·cm^-2 at 1.5 V (1073 K) Feed stock: CO₂	[47]

Fig. 4. (a) Schematic of a sustainable fuels generator consist of a SOEC stack and a Fischer-Tropsch synthesis reactor. (b) Polarization curves for H2O electrolysis, H2O/CO2 co-electrolysis versus CO2 electrolysis with mean area specific resistance values. (c) Oxygen evolution from powdered ferrite perovskite catalyst during heat treatment under helium. (d) I-V curve of a La0.7Sr0.3MnO3-YSZ (anode)/YSZ/La0.7Sr0.2Ni0.1Co0.1Fe0.8O3 (cathode) cell under 40% CO2 and different H2O concentrations on the cathode side at 1073 K in SOEC mode. (e) Cell voltage and Faradaic efficiency during a long-term co-electrolysis test with a La0.7Sr0.3MnO3-YSZ (anode)/YSZ/La0.7Sr0.2Ni0.1Co0.1Fe0.8O3 (cathode) cell at 1073 K using a cathode feed of 40% CO2 + 10% H2O/He. (f) Electrochemical performance of La0.7Sr0.3Fe0.9Ni0.1O3-δ-GDC/LSGM/PrBa0.8Ca0.2Co2O5+δ-GDC cells for H2O-CO2 co-electrolysis. Inset: Long-term stability of co-electrolysis cells measured at a current density of 1 A·cm-2 with 20 vol% H2O-CO2 and 1073 K. (g) Relationships between surface oxophilicity and electrolysis performance. (h) Free energy diagrams for CO2 electrolysis on the monometallic Fe(110) clean surface, and surfaces pre-covered by O* with various coverages at 1073 K, standard pressure, and an applied potential of 1.3 V. (i) Plot comparing the energy barriers for CO2 dissociation and O diffusion as a function of oxygen surface coverage on Fe(110). Fig. (b) was reprinted with permission from Ref. [51]. Copyright 2009 Elsevier. Figs. (c,d,e) were reprinted with permission from Ref. [52]. Copyright 2019 Elsevier. Fig. (f) was reprinted with permission from Ref. [8]. Copyright 2021 Elsevier. Figs. (g,h,i) were reprinted with permission from Ref. [54]. Copyright 2020 American chemical society.

Fig. 5. (a) Schematic of utilization of CH4 as fuel in SOFCs. (b) I-V curves for CH4/CO2 co-electrolysis in different anodes. (c) Electrochemical oxidation of CH4 in conjunction with CO2 electrolysis, and the product analysis in the anode. 1: Sr2Fe1.5Mo0.5O6-δ (SFMO), 2: 0.025Fe-SFMO, 3: 0.050Fe-SFMO, 4: 0.075Fe-SFMO, 5: 0.100Fe-SFMO. (d) Long-term performance of the 0.075Fe-SFMO-SDC electrode for CH4 oxidation with CO2 electrolysis at 1123 K. (e) Development over time of reported stack test duration since 2009. (f) Degradation rates of reported SOEC stacks since 2009. (g) SOEC plant production capacities from 2015 to 2022. Fig. (b) was reprinted with permission from Ref. [59]. Copyright 2018 American Association for the Advancement of Science (AAAS). Figs. (c,d) were reprinted with permission from Ref. [60], according to Creative Commons Attribution 4.0 International License. Figs. (e,f,g) were reprinted with permission from Ref. [3]. Copyright 2020 AAAS.

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