High‐Performance and Durable Fuel Cells using Co/Sr‐Free Fluorite‐Based Mixed Conducting (Pr,Ce)O 2‐δ Cathode

Seo, Han Gil; Kim, Dong Hwan; Seo, Jongsu; Jeong, Seung Jin; Kim, Jinwook; Tuller, Harry L.; Son, Ji‐Won; Jung, WooChul

doi:10.1002/aenm.202202101

High‐Performance and Durable Fuel Cells using Co/Sr‐Free Fluorite‐Based Mixed Conducting (Pr,Ce)O _2‐δ Cathode

Journal Article · Thu Sep 08 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202101· OSTI ID:1894722

^[1]; Kim, Dong Hwan ^[2]; Seo, Jongsu ^[3]; Jeong, Seung Jin ^[3]; Kim, Jinwook ^[3]; Tuller, Harry L. ^[4]; Son, Ji‐Won ^[5]; ^[3]

Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of Korea, Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
Energy Materials Research Center Korea Institute of Science and Technology (KIST) Seoul 02792 Republic of Korea, Department of Mechanical Engineering Korea University Seoul 02841 Republic of Korea
Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of Korea
Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
Energy Materials Research Center Korea Institute of Science and Technology (KIST) Seoul 02792 Republic of Korea, Graduate School of Energy and Environment (KU‐KIST GREEN SCHOOL) Korea University Seoul 02841 Republic of Korea

Abstract

A major challenge to overcome in demonstrating solid oxide fuel cells (SOFCs) to be suitable as efficient and environmentally friendly energy conversion devices capable of addressing pressing clean energy and environmental needs is to surmount chemical and thermo‐mechanical instabilities in their operational phase. To date, perovskite‐based mixed conducting cathodes, which include inherent Co and Sr elements for enhanced reactivity and conductivity, have been intensively studied. These Co/Sr‐based oxides, however, exhibit severe thermochemical expansion and suffer from Sr surface segregation, ultimately degrading the electrode performance. Here, high‐performance and durable SOFCs are demonstrated by employing a Co/Sr‐free fluorite‐based mixed conducting (Pr,Ce)O _2‐δ (PCO) cathode eminently compatible with fluorite‐based solid electrolytes. The nanocolumnar PCO electrode developed in this study provides not only a remarkable low level of electrode resistance (e.g., ≈0.05 Ω cm ² at 600 °C) but also exceptional long‐term stability (e.g., a degradation rate 15 times slower compared to the state‐of‐the‐art La _0.6 Sr _0.4 CoO _3‐δ perovskite). The competitive peak power densities of an anode‐supported single cell with the PCO cathode are also successively achieved, recording a value of 0.92 W cm ⁻² at 600 °C. These findings herald the development of new Co/Sr‐free electrodes for SOFCs at intermediate temperatures.

View Journal Article

Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: Korea Institute of Energy Technology Evaluation and Planning (KETEP); National Research Foundation of Korea (NRF); USDOE; USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: FE0031668

OSTI ID:: 1894722

Alternate ID(s):: OSTI ID: 1898686
OSTI ID: 1908557
OSTI ID: 23204479

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 43 Vol. 12; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (64)

Microstructures of CGO and YSZ Thin Films by Pulsed Laser Deposition Infortuna, A.; Harvey, A. S.; Gauckler, L. J. Advanced Functional Materials, Vol. 18, Issue 1 https://doi.org/10.1002/adfm.200700136	journal	December 2007
High-Performance Micro-Solid Oxide Fuel Cells Fabricated on Nanoporous Anodic Aluminum Oxide Templates Kwon, Chang-Woo; Son, Ji-Won; Lee, Jong-Ho Advanced Functional Materials, Vol. 21, Issue 6 https://doi.org/10.1002/adfm.201002137	journal	February 2011
Non-stoichiometry in Oxide Thin Films: A Chemical Capacitance Study of the Praseodymium-Cerium Oxide System Chen, Di; Bishop, Sean R.; Tuller, Harry L. Advanced Functional Materials, Vol. 23, Issue 17 https://doi.org/10.1002/adfm.201202104	journal	November 2012
A New Model Describing Solid Oxide Fuel Cell Cathode Kinetics: Model Thin Film SrTi1-xFexO3-δ Mixed Conducting Oxides-a Case Study Jung, WooChul; Tuller, Harry L. Advanced Energy Materials, Vol. 1, Issue 6 https://doi.org/10.1002/aenm.201100164	journal	September 2011
A Highly Efficient and Robust Nanofiber Cathode for Solid Oxide Fuel Cells Chen, Yu; Bu, Yunfei; Zhang, Yanxiang Advanced Energy Materials, Vol. 7, Issue 6 https://doi.org/10.1002/aenm.201601890	journal	November 2016
Exceptionally Enhanced Electrode Activity of (Pr,Ce)O ₂₋ _δ -Based Cathodes for Thin-Film Solid Oxide Fuel Cells Seo, Han Gil; Choi, Yoonseok; Jung, WooChul Advanced Energy Materials, Vol. 8, Issue 19 https://doi.org/10.1002/aenm.201703647	journal	March 2018
Electronic conductivity of Ce _0.8 Gd _{0.2− x} Pr _x O _{2− δ} and influence of added CoO: Electronic conductivity of Ce _0.8 Gd _{0.2− x} Pr _x O _{2− δ} Schmale, Kerstin; Grünebaum, Mariano; Janssen, Martin physica status solidi (b), Vol. 248, Issue 2 https://doi.org/10.1002/pssb.201046365	journal	October 2010
Praseodymium-cerium oxide thin film cathodes: Study of oxygen reduction reaction kinetics Chen, Di; Bishop, Sean R.; Tuller, Harry L. Journal of Electroceramics, Vol. 28, Issue 1 https://doi.org/10.1007/s10832-011-9678-z	journal	January 2012
Efficient and Stable Ideal Bandgap Perovskite Solar Cell Achieved by a Small Amount of Tin Substituted Methylammonium Lead Iodide Yin, Yongqi; Fu, Sufang; Zhou, Sheng Electronic Materials Letters, Vol. 16, Issue 3 https://doi.org/10.1007/s13391-020-00206-3	journal	February 2020
Protonic ceramic electrolysis cells for fuel production: a brief review Ji, Ho-Il; Lee, Jong-Ho; Son, Ji-Won Journal of the Korean Ceramic Society, Vol. 57, Issue 5 https://doi.org/10.1007/s43207-020-00059-4	journal	May 2020
PrBa0.5Sr0.5Co1.5Fe0.5O5+δ composite cathode in protonic ceramic fuel cells Im, Seunghyeok; Lee, Jong-Ho; Ji, Ho-Il Journal of the Korean Ceramic Society, Vol. 58, Issue 3 https://doi.org/10.1007/s43207-021-00109-5	journal	February 2021
Thermal expansion of Gd-doped ceria and reduced ceria Hayashi, H. Solid State Ionics, Vol. 132, Issue 3-4 https://doi.org/10.1016/S0167-2738(00)00646-9	journal	July 2000
Sm0.5Sr0.5CoO3 cathodes for low-temperature SOFCs Xia, C. Solid State Ionics, Vol. 149, Issue 1-2 https://doi.org/10.1016/S0167-2738(02)00131-5	journal	July 2002
Nanostructured cathode thin films with vertically-aligned nanopores for thin film SOFC and their characteristics Yoon, Jongsik; Araujo, Roy; Grunbaum, Nicolás Applied Surface Science, Vol. 254, Issue 1 https://doi.org/10.1016/j.apsusc.2007.07.053	journal	October 2007
A Highly Efficient Multi-phase Catalyst Dramatically Enhances the Rate of Oxygen Reduction Chen, Yu; Choi, YongMan; Yoo, Seonyoung Joule, Vol. 2, Issue 5 https://doi.org/10.1016/j.joule.2018.02.008	journal	May 2018
Sr Segregation in Perovskite Oxides: Why It Happens and How It Exists Koo, Bonjae; Kim, Kyeounghak; Kim, Jun Kyu Joule, Vol. 2, Issue 8 https://doi.org/10.1016/j.joule.2018.07.016	journal	August 2018
Thin films for micro solid oxide fuel cells Beckel, D.; Bieberle-Hütter, A.; Harvey, A. Journal of Power Sources, Vol. 173, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.04.070	journal	November 2007
Review on microfabricated micro-solid oxide fuel cell membranes Evans, Anna; Bieberle-Hütter, Anja; Rupp, Jennifer L. M. Journal of Power Sources, Vol. 194, Issue 1 https://doi.org/10.1016/j.jpowsour.2009.03.048	journal	October 2009
Co-free, iron perovskites as cathode materials for intermediate-temperature solid oxide fuel cells Hou, Shu-en; Alonso, José Antonio; Goodenough, John B. Journal of Power Sources, Vol. 195, Issue 1 https://doi.org/10.1016/j.jpowsour.2009.07.017	journal	January 2010
Novel SrCo1−yNbyO3−δ cathodes for intermediate-temperature solid oxide fuel cells Wang, Fang; Zhou, Qingjun; He, Tianmin Journal of Power Sources, Vol. 195, Issue 12 https://doi.org/10.1016/j.jpowsour.2009.12.081	journal	June 2010
Nanoscaled La0.6Sr0.4CoO3−δ as intermediate temperature solid oxide fuel cell cathode: Microstructure and electrochemical performance Hayd, Jan; Dieterle, Levin; Guntow, Uwe Journal of Power Sources, Vol. 196, Issue 17 https://doi.org/10.1016/j.jpowsour.2010.11.147	journal	September 2011
Optimization of current collection to reduce the lateral conduction loss of thin-film-processed cathodes Noh, Ho-Sung; Hwang, Jaeyeon; Yoon, Kyungjoong Journal of Power Sources, Vol. 230 https://doi.org/10.1016/j.jpowsour.2012.12.059	journal	May 2013
Praseodymium and gadolinium doped ceria as a cathode material for low temperature solid oxide fuel cells Chockalingam, Rajalekshmi; Ganguli, Ashok Kumar; Basu, Suddhasatwa Journal of Power Sources, Vol. 250 https://doi.org/10.1016/j.jpowsour.2013.10.105	journal	March 2014
Ca and In co-doped BaFeO 3−δ as a cobalt-free cathode material for intermediate-temperature solid oxide fuel cells Wang, Jian; Lam, Kwun Yu; Saccoccio, Mattia Journal of Power Sources, Vol. 324 https://doi.org/10.1016/j.jpowsour.2016.05.089	journal	August 2016
Thermal expansion coefficient of yttria stabilized zirconia for various yttria contents Hayashi, H.; Saitou, T.; Maruyama, N. Solid State Ionics, Vol. 176, Issue 5-6 https://doi.org/10.1016/j.ssi.2004.08.021	journal	February 2005
Mixed conductivity, thermal expansion, and oxygen permeability of Ce(Pr,Zr)O Fagg, D.; Kharton, V.; Shaula, A. Solid State Ionics, Vol. 176, Issue 19-22 https://doi.org/10.1016/j.ssi.2005.04.023	journal	June 2005
Electrochemical performance of LSCF based thin film cathodes prepared by spray pyrolysis Beckel, D.; Muecke, U.; Gyger, T. Solid State Ionics, Vol. 178, Issue 5-6 https://doi.org/10.1016/j.ssi.2007.01.019	journal	March 2007
Characteristics of ABO3 and A2BO4 (ASm, Sr; BCo, Fe, Ni) samarium oxide system as cathode materials for intermediate temperature-operating solid oxide fuel cell Baek, Seung-Wook; Kim, Jung Hyun; Bae, Joongmyeon Solid State Ionics, Vol. 179, Issue 27-32 https://doi.org/10.1016/j.ssi.2007.12.010	journal	September 2008
Oxygen nonstoichiometry and exchange kinetics of Ba0.5Sr0.5Co0.8Fe0.2O3−δ Bucher, Edith; Egger, Andreas; Ried, Peter Solid State Ionics, Vol. 179, Issue 21-26 https://doi.org/10.1016/j.ssi.2008.01.089	journal	September 2008
Long-term stability of the oxygen exchange properties of (La,Sr)1−z(Co,Fe)O3−δ in dry and wet atmospheres Bucher, Edith; Sitte, Werner Solid State Ionics, Vol. 192, Issue 1 https://doi.org/10.1016/j.ssi.2010.01.006	journal	June 2011
Comparison of oxygen exchange kinetics of the IT-SOFC cathode materials La0.5Sr0.5CoO3−δ and La0.6Sr0.4CoO3−δ Egger, Andreas; Bucher, Edith; Yang, Min Solid State Ionics, Vol. 225 https://doi.org/10.1016/j.ssi.2012.02.050	journal	October 2012
Optically derived energy band gap states of Pr in ceria Kim, Jae Jin; Bishop, Sean R.; Thompson, Nicholas Solid State Ionics, Vol. 225 https://doi.org/10.1016/j.ssi.2012.03.047	journal	October 2012
Impact of defect chemistry on cathode performance: A case study of Pr-doped ceria Lenser, Christian; Gunkel, Felix; Sohn, Yoo Jung Solid State Ionics, Vol. 314 https://doi.org/10.1016/j.ssi.2017.09.023	journal	January 2018
Improving the Si Impurity Tolerance of Pr _0.1 Ce _0.9 O _2−δ SOFC Electrodes with Reactive Surface Additives Zhao, Liang; Perry, Nicola H.; Daio, Takeshi Chemistry of Materials, Vol. 27, Issue 8 https://doi.org/10.1021/acs.chemmater.5b00501	journal	April 2015
All-Sputtered, Superior Power Density Thin-Film Solid Oxide Fuel Cells with a Novel Nanofibrous Ceramic Cathode Lee, Yoon Ho; Ren, Haowen; Wu, Erik A. Nano Letters, Vol. 20, Issue 5 https://doi.org/10.1021/acs.nanolett.9b02344	journal	March 2020
Chemical Heterogeneities on La _0.6 Sr _0.4 CoO _3−δ Thin Films—Correlations to Cathode Surface Activity and Stability Cai, Zhuhua; Kubicek, Markus; Fleig, Jürgen Chemistry of Materials, Vol. 24, Issue 6 https://doi.org/10.1021/cm203501u	journal	March 2012
Factors Governing Oxygen Reduction in Solid Oxide Fuel Cell Cathodes ^† Adler, Stuart B. Chemical Reviews, Vol. 104, Issue 10 https://doi.org/10.1021/cr020724o	journal	October 2004
Materials for fuel-cell technologies Steele, Brian C. H.; Heinzel, Angelika Nature, Vol. 414, Issue 6861, p. 345-352 https://doi.org/10.1038/35104620	journal	November 2001
A high-performance cathode for the next generation of solid-oxide fuel cells Shao, Zongping; Haile, Sossina M. Nature, Vol. 431, Issue 7005, p. 170-173 https://doi.org/10.1038/nature02863	journal	September 2004
Improved chemical and electrochemical stability of perovskite oxides with less reducible cations at the surface Tsvetkov, Nikolai; Lu, Qiyang; Sun, Lixin Nature Materials, Vol. 15, Issue 9 https://doi.org/10.1038/nmat4659	journal	June 2016
Scalable nanostructured membranes for solid-oxide fuel cells Tsuchiya, Masaru; Lai, Bo-Kuai; Ramanathan, Shriram Nature Nanotechnology, Vol. 6, Issue 5 https://doi.org/10.1038/nnano.2011.43	journal	April 2011
In situ click chemistry generation of cyclooxygenase-2 inhibitors Bhardwaj, Atul; Kaur, Jatinder; Wuest, Melinda Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-016-0009-6	journal	February 2017
Thermal-expansion offset for high-performance fuel cell cathodes Zhang, Yuan; Chen, Bin; Guan, Daqin Nature, Vol. 591, Issue 7849 https://doi.org/10.1038/s41586-021-03264-1	journal	March 2021
Constructing a pathway for mixed ion and electron transfer reactions for O2 incorporation in Pr0.1Ce0.9O2−x Chen, Di; Guan, Zixuan; Zhang, Dawei Nature Catalysis, Vol. 3, Issue 2 https://doi.org/10.1038/s41929-019-0401-9	journal	January 2020
Acidity of surface-infiltrated binary oxides as a sensitive descriptor of oxygen exchange kinetics in mixed conducting oxides Nicollet, Clement; Toparli, Cigdem; Harrington, George F. Nature Catalysis, Vol. 3, Issue 11 https://doi.org/10.1038/s41929-020-00520-x	journal	October 2020
Investigation of surface Sr segregation in model thin film solid oxidefuel cell perovskite electrodes Jung, WooChul; Tuller, Harry L. Energy Environ. Sci., Vol. 5, Issue 1 https://doi.org/10.1039/C1EE02762J	journal	January 2012
An electrical conductivity relaxation study of oxygen transport in samarium doped ceria Gopal, Chirranjeevi Balaji; Haile, Sossina M. J. Mater. Chem. A, Vol. 2, Issue 7 https://doi.org/10.1039/C3TA13404K	journal	January 2014
The effect of calcium doping on the improvement of performance and durability in a layered perovskite cathode for intermediate-temperature solid oxide fuel cells Choi, Sihyuk; Park, Seonhye; Shin, Jeeyoung Journal of Materials Chemistry A, Vol. 3, Issue 11 https://doi.org/10.1039/C4TA05684A	journal	January 2015
Zr and Y co-doped perovskite as a stable, high performance cathode for solid oxide fuel cells operating below 500 °C Duan, Chuancheng; Hook, David; Chen, Yachao Energy & Environmental Science, Vol. 10, Issue 1 https://doi.org/10.1039/C6EE01915C	journal	January 2017
Enhanced oxygen exchange of perovskite oxide surfaces through strain-driven chemical stabilization Koo, Bonjae; Kwon, Hyunguk; Kim, YeonJu Energy & Environmental Science, Vol. 11, Issue 1 https://doi.org/10.1039/C7EE00770A	journal	January 2018
Cobalt-substituted SrTi _0.3 Fe _0.7 O _3−δ : a stable high-performance oxygen electrode material for intermediate-temperature solid oxide electrochemical cells Zhang, Shan-Lin; Wang, Hongqian; Lu, Matthew Y. Energy & Environmental Science, Vol. 11, Issue 7 https://doi.org/10.1039/C8EE00449H	journal	January 2018
A highly active, CO ₂ -tolerant electrode for the oxygen reduction reaction Chen, Yu; Yoo, Seonyoung; Choi, YongMan Energy & Environmental Science, Vol. 11, Issue 9 https://doi.org/10.1039/C8EE01140K	journal	January 2018
Oxygen exchange kinetics on systematically doped ceria: a pulsed isotope exchange study Schaube, Maximilian; Merkle, Rotraut; Maier, Joachim Journal of Materials Chemistry A, Vol. 7, Issue 38 https://doi.org/10.1039/C9TA05908C	journal	January 2019
Integrated Cr and S poisoning of a La _0.6 Sr _0.4 Co _0.2 Fe _0.8 O _3−δ (LSCF) cathode for solid oxide fuel cells Wang, Cheng Cheng; Gholizadeh, Mortaza; Hou, Bingxue RSC Advances, Vol. 11, Issue 1 https://doi.org/10.1039/D0RA09239H	journal	January 2021
Cathodic electrochemical deposition: a new strategy to enhance the activity and stability of silver cathodes for thin-film solid oxide fuel cells Kim, Hyunseung; Seo, Han Gil; Choi, Yoonseok Journal of Materials Chemistry A, Vol. 8, Issue 29 https://doi.org/10.1039/D0TA02439B	journal	January 2020
Isovalent doping: a new strategy to suppress surface Sr segregation of the perovskite O₂-electrode for solid oxide fuel cells Koo, Bonjae; Seo, Jongsu; Kim, Jun Kyu Journal of Materials Chemistry A, Vol. 8, Issue 27 https://doi.org/10.1039/D0TA02870C	journal	January 2020
Silica: ubiquitous poison of metal oxide interfaces Staerz, Anna; Seo, Han Gil; Defferriere, Thomas Journal of Materials Chemistry A, Vol. 10, Issue 6 https://doi.org/10.1039/D1TA08469K	journal	January 2022
Electrical conductivity and defect equilibria of Pr0.1Ce0.9O2−δ Bishop, Sean R.; Stefanik, Todd S.; Tuller, Harry L. Physical Chemistry Chemical Physics, Vol. 13, Issue 21 https://doi.org/10.1039/c0cp02920c	journal	January 2011
Proton conductivity of columnar ceria thin-films grown by chemical vapor deposition Oh, Tae-Sik; Boyd, David A.; Goodwin, David G. Physical Chemistry Chemical Physics, Vol. 15, Issue 7 https://doi.org/10.1039/c2cp43036c	journal	January 2013
A promising cathode for intermediate temperature protonic ceramic fuel cells: BaCo_0.4Fe_0.4Zr_0.2O_3−δ Shang, Meng; Tong, Jianhua; O'Hayre, Ryan RSC Advances, Vol. 3, Issue 36, p. 15769-15775 https://doi.org/10.1039/c3ra41828f	journal	January 2013
Recent Advances in Materials for Fuel Cells Brandon, N. P.; Skinner, S.; Steele, B. C. H. Annual Review of Materials Research, Vol. 33, Issue 1 https://doi.org/10.1146/annurev.matsci.33.022802.094122	journal	August 2003
Structural Stability and Oxygen Permeation Properties of Sr[sub 3−x]La[sub x]Fe[sub 2−y]Co[sub y]O[sub 7−δ] (0≤x≤0.3 and 0≤y≤1.0) Prado, F.; Armstrong, T.; Caneiro, A. Journal of The Electrochemical Society, Vol. 148, Issue 4 https://doi.org/10.1149/1.1354605	journal	January 2001
Physical and Electrochemical Characteristics of Pulsed Laser Deposited La_0.6Sr_0.4CoO_3−δ-Ce_0.9Gd_0.1O_2−δNanocomposites as a Function of the Mixing Ratio Park, Jung-Hoon; Hong, Wan-Shick; Yoon, Kyung Joong Journal of The Electrochemical Society, Vol. 161, Issue 1 https://doi.org/10.1149/2.019401jes	journal	October 2013
MEMS-based thin-film solid-oxide fuel cells An, Jihwan; Shim, Joon Hyung; Kim, Young-Beom MRS Bulletin, Vol. 39, Issue 9 https://doi.org/10.1557/mrs.2014.171	journal	September 2014

Similar Records

Robust highly durable solid oxide fuel cell cathodes – Improved materials compatibility & self-regulating surface chemistry

Technical Report · Thu Mar 02 23:00:00 EST 2023 · OSTI ID:1960547

Related Subjects

30 DIRECT ENERGY CONVERSION
36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
cathode
power density
praseodymia ceria
solid oxide fuel cell
thin film

High‐Performance and Durable Fuel Cells using Co/Sr‐Free Fluorite‐Based Mixed Conducting (Pr,Ce)O 2‐δ Cathode

Citation Formats

References (64)

Similar Records

Related Subjects

High‐Performance and Durable Fuel Cells using Co/Sr‐Free Fluorite‐Based Mixed Conducting (Pr,Ce)O _2‐δ Cathode