固态氧化物电解池中碳一分子电化学转化为可再生燃料

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

催化学报 ›› 2022, Vol. 43 ›› Issue (1): 92-103.DOI: 10.1016/S1872-2067(21)63838-X

固态氧化物电解池中碳一分子电化学转化为可再生燃料

吕希蒙, 陈锰寰, 谢朝龙, 钱林平, 张丽娟, 郑耿锋^*()

复旦大学先进材料实验室, 化学与材料学院, 化学系, 上海市分子催化和功能材料重点实验室, 上海200438

收稿日期:2021-04-10 接受日期:2021-04-23 出版日期:2022-01-18 发布日期:2021-05-18
通讯作者: 郑耿锋
基金资助:
国家重点研究和发展项目(2018YFA0209401);国家重点研究和发展项目(2017YFA0206901);国家科学基金(22025502);国家科学基金(21975051);国家科学基金(21773036);上海市科学技术委员会资助项目(19XD1420400);上海市教育委员会资助项目(2019-01-07-00-07-E00045)

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

Ximeng Lv, Menghuan Chen, Zhaolong Xie, Linping Qian, Lijuan Zhang, Gengfeng Zheng^*()

Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, China

Received:2021-04-10 Accepted:2021-04-23 Online:2022-01-18 Published:2021-05-18
Contact: Gengfeng Zheng
About author:* E-mail: gfzheng@fudan.edu.cn
Supported by:
National Key Research and Development Program of China(2018YFA0209401);National Key Research and Development Program of China(2017YFA0206901);National Science Foundation of China(22025502);National Science Foundation of China(21975051);National Science Foundation of China(21773036);Science and Technology Commission of Shanghai Municipality(19XD1420400);Shanghai Municipal Education Commission(2019-01-07-00-07-E00045)

摘要/Abstract

摘要：

近年来, 随着社会环保意识的迅速提高以及对可再生能源利用能力的大幅增强, 以燃料电池和电解池为代表的电化学技术已经逐渐在能源的存储、转化和利用方面发挥着不可或缺的独特作用. 其中, 固态氧化物电解池经过多年的发展, 在装置成本和工作效率上取得了长足的进步, 在储能转化方面具有重要的潜力. 与此同时, 伴随着《巴黎协定》签订以来各国的“碳中和”路线图逐渐出台, 利用相对廉价易得的可再生电能, 将二氧化碳(CO₂)和甲烷(CH₄)等碳一(C1)分子电解转化为高附加值的可再生燃料(如水煤气、乙烯等), 对于碳中和目标的实现具有重要的意义. 因此, C1分子电化学转化的研究成为了当下重点关注的研究领域, 许多重要的研究成果和技术进步在过去几年中不断涌现. 固态氧化物电解池作为一种代表性的C1分子电解和转化平台, 也日渐引起相关领域研究人员的关注和兴趣. 与传统的C1分子催化转化方法相比, 基于固态氧化物电解池的电解转化技术具有两个重要优点: 高能量转换效率与体系抗中毒能力. 这两个特性作为体系稳健性的基石, 保障了C1分子转化为可再生燃料的反应过程的长期可持续性.
本文首先简要回顾了固态氧化物电解池的前沿技术与发展, 并从电解池系统分类、反应体系的特征和反应体系发展的前景与挑战这三个方面, 简要介绍了近年来基于固态氧化物电解池体系的C1分子电化学转化的代表性工作. CO₂与CH₄作为廉价易得的C1分子的代表, 其转化因其反应分子惰性及反应过程不可控性而广受研究者关注, 本文重点关注了在固态氧化物电解池中CO₂, CO₂/H₂O和CH₄三个体系的电化学反应过程和近期研究进展, 希望可为相关研究人员未来设计更合适的催化剂和构建更优的电解池结构提供有益的参考. 本文还针对目前固态氧化物电解池体系在C1分子转化领域所面临的挑战, 提出了未来的一些可能的研究方向, 以期助力研究者在不远的将来实现C1分子电解生产可再生燃料的实用化.

关键词: 固态氧化物电解池, 碳一分子, 电解, 甲烷转化, 二氧化碳转化

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

吕希蒙, 陈锰寰, 谢朝龙, 钱林平, 张丽娟, 郑耿锋. 固态氧化物电解池中碳一分子电化学转化为可再生燃料[J]. 催化学报, 2022, 43(1): 92-103.

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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图/表 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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固态氧化物电解池中碳一分子电化学转化为可再生燃料

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

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