Realizing efficient operations of Ni-cermet-based fuel cells on hydrocarbons via an in situ self-assembled metal/oxide nano-heterostructured catalyst

Xu, Kang; Zhang, Hua; Xu, Yangsen; Zhu, Feng; He, Fan; Sasaki, Kotaro; Choi, YongMan; Chen, Yu

doi:10.1016/j.apcatb.2024.124208

Title: Realizing efficient operations of Ni-cermet-based fuel cells on hydrocarbons via an in situ self-assembled metal/oxide nano-heterostructured catalyst

Journal Article · 15 May 2024 · Applied Catalysis. B, Environmental

DOI: https://doi.org/10.1016/j.apcatb.2024.124208 · OSTI ID:2500290

Xu, Kang ^[1]; Zhang, Hua ^[1]; Xu, Yangsen ^[1]; Zhu, Feng ^[1]; He, Fan ^[1]; Sasaki, Kotaro ^[2]; Choi, YongMan ^[3]; Chen, Yu ^[1]

South China University of Technology (SCUT), Guangzhou (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
National Yang Ming Chiao Tung University, Tainan (Taiwan)

Operating Ni-cermet-based fuel cells on hydrocarbons is charming by largely hindered by poor coking tolerance and severe deterioration. Here, in this study, we report an effective metal/oxide nano-heterostructured catalyst with a nominal composition of Pr_0.95Ru_0.05O_2-δ (PRO), which is in situ self-assembled to a Pr_0.95Ru_0.05-xO_2-δ oxide frame coated with Ru metallic nanoparticles (denoted as Ru/PRO) under the operation condition. When applied to the Ni-cermet (Ni-YSZ) anodes, the cells achieve decent peak power densities of 1.784 and 1.870 W cm^-2 on CH₄ and C₃H₈ with only 3% H₂O at 750 °C, respectively. Moreover, the cells with Ru/PRO-coated anode demonstrate excellent durability when operated on CH₄ for ~ 220 h and C₃H₈ for ~115 h. It is demonstrated that the Ru/PRO generates hydroxyl species that react with carbon species, followed by the formation of COH intermediates on Ni anode surfaces for removing the coking, as confirmed by experiments and computations.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Fundamental Research Funds for the Central Universities; National Natural Science Foundation of China (NSFC); National Science and Technology Council (NSTC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2500290

Report Number(s):: BNL--226463-2025-JAAM

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 355; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (63)

An Efficient Steam‐Induced Heterostructured Air Electrode for Protonic Ceramic Electrochemical Cells Xu, Kang; Zhang, Hua; Xu, Yangsen Advanced Functional Materials, Vol. 32, Issue 23 https://doi.org/10.1002/adfm.202110998	journal	February 2022
Recent Progress in the Development of Anode Materials for Solid Oxide Fuel Cells Cowin, Peter I.; Petit, Christophe T. G.; Lan, Rong Advanced Energy Materials, Vol. 1, Issue 3 https://doi.org/10.1002/aenm.201100108	journal	April 2011
Optimizing the preparation of Ni‐Ce‐Pr catalysts for efficient hydrogen production by n ‐dodecane steam reforming Xiao, Zhourong; Zhang, Xiangwen; Wang, Li International Journal of Energy Research, Vol. 44, Issue 3 https://doi.org/10.1002/er.5029	journal	December 2019
Electrochemical properties of Sr-doped layered perovskite as a promising anode material for direct hydrocarbon SOFCs Choi, Sihyuk Journal of the Korean Ceramic Society, Vol. 57, Issue 4 https://doi.org/10.1007/s43207-020-00045-w	journal	April 2020
A new model explaining carbon filament growth on nickel, iron, and Ni$z.sbnd;Cu alloy catalysts Alstrup, I. Journal of Catalysis, Vol. 109, Issue 2 https://doi.org/10.1016/0021-9517(88)90207-2	journal	February 1988
Ni doped La 0.6 Sr 0.4 FeO 3- δ symmetrical electrode for solid oxide fuel cells Ma, Zhaohui; Sun, Chunwen; Ma, Chao Chinese Journal of Catalysis, Vol. 37, Issue 8 https://doi.org/10.1016/S1872-2067(15)61116-0	journal	August 2016
Optimizing cathode materials for intermediate-temperature solid oxide fuel cells (SOFCs): Oxygen reduction on nanostructured lanthanum nickelate oxides Carneiro, Juliana Silva Alves; Brocca, Roger Antunes; Lucena, Max Laylson Ribeiro Sampaio Applied Catalysis B: Environmental, Vol. 200 https://doi.org/10.1016/j.apcatb.2016.06.073	journal	January 2017
Weakening the metal-support strong interaction to enhance catalytic performances of alumina supported Ni-based catalysts for producing hydrogen Lu, Jichang; Lei, Yanqiu; Wan, Gengping Applied Catalysis B: Environmental, Vol. 263 https://doi.org/10.1016/j.apcatb.2019.118177	journal	April 2020
Ru/Nb co-doped perovskite anode: Achieving good coking resistance in hydrocarbon fuels via core-shell nanocatalysts exsolution Qin, Mingxia; Xiao, Yu; Yang, Hongyu Applied Catalysis B: Environmental, Vol. 299 https://doi.org/10.1016/j.apcatb.2021.120613	journal	December 2021
(La0.8Sr0.2)0.98MnO3-δ-Zr0.92Y0.16O2-δ:PrOx for oxygen electrode supported solid oxide cells Yang, Tianrang; Kollasch, Shannon L.; Grimes, Jerren Applied Catalysis B: Environmental, Vol. 306 https://doi.org/10.1016/j.apcatb.2022.121114	journal	June 2022
Promoted methane activation on doped ceria via occupation of Pr(4f) states Salcedo, Agustín; Iglesias, Ignacio; Mariño, Fernando Applied Surface Science, Vol. 458 https://doi.org/10.1016/j.apsusc.2018.07.090	journal	November 2018
Three-dimensionally ordered macroporous Pr6O11 and Tb4O7 with mesoporous walls: Preparation, characterization, and catalytic activity for CO oxidation Zhang, Yujuan; Deng, Jiguang; Zhang, Han Catalysis Today, Vol. 245 https://doi.org/10.1016/j.cattod.2014.09.017	journal	May 2015
Solid oxide fuel cells fueled by simulated biogas: Comparison of anode modification by infiltration and reforming catalytic layer Lyu, Zewei; Wang, Yige; Zhang, Yongliang Chemical Engineering Journal, Vol. 393 https://doi.org/10.1016/j.cej.2020.124755	journal	August 2020
A rational design of highly active and coke-resistant anode for methanol-fueled solid oxide fuel cells with Sn doped Ni-Ce0.8Sm0.2O2−δ Gan, Tian; Song, Hexuan; Fan, Xinqiang Chemical Engineering Journal, Vol. 455 https://doi.org/10.1016/j.cej.2022.140692	journal	January 2023
Cobalt-free perovskite Ba1-xNdxFeO3-δ air electrode materials for reversible solid oxide cells Kim, You-Dong; Yang, Ja-Yoon; Saqib, Muhammad Ceramics International, Vol. 47, Issue 6 https://doi.org/10.1016/j.ceramint.2020.11.149	journal	March 2021
A finger-like anode with infiltrated Ni0.1Ce0.9O2-δ catalyst using new phase inversion combined tape-casting technology for optimized dry reforming of methane Sha, Yuhang; Ling, Yihan; Yang, Yang Ceramics International, Vol. 49, Issue 17 https://doi.org/10.1016/j.ceramint.2023.06.195	journal	September 2023
High-performance Ni in-situ exsolved Ba(Ce0.9Y0.1)0.8Ni0.2O3-δ/Gd0.1Ce0.9O1.95 composite anode for SOFC with long-term stability in methane fuel Liu, Yanya; Jia, Lichao; Li, Jin Composites Part B: Engineering, Vol. 193 https://doi.org/10.1016/j.compositesb.2020.108033	journal	July 2020
An oxygen reduction reaction active and durable SOFC cathode/electrolyte interface achieved via a cost-effective spray-coating Xu, Kang; Pei, Kai; Zhao, Bote International Journal of Hydrogen Energy, Vol. 46, Issue 63 https://doi.org/10.1016/j.ijhydene.2021.06.224	journal	September 2021
Synergistic effect study of EuBa0.98Co2O5+-Ce0.8Sm0.2O1.9 composite cathodes for intermediate-temperature solid oxide fuel cells Li, Shuli; Zhang, Likun; Xia, Tian Journal of Alloys and Compounds, Vol. 771 https://doi.org/10.1016/j.jallcom.2018.08.300	journal	January 2019
Enhanced coking resistance of a Ni cermet anode by a chromates protective layer Chang, Hong; Chen, Huili; Yang, Guangming Journal of Energy Chemistry, Vol. 37 https://doi.org/10.1016/j.jechem.2018.12.007	journal	October 2019
Process-intensified protonic ceramic fuel cells for power generation, chemical production, and greenhouse gas mitigation Liu, Fan; Deng, Hao; Ding, Hanping Joule, Vol. 7, Issue 6 https://doi.org/10.1016/j.joule.2023.05.009	journal	June 2023
Nb-doped double perovskite Sr2CoFeO6−δ as an efficient and prospective electrode for quasi-symmetrical solid oxide fuel cells Shi, Chenchen; Liu, Yue; Wang, Biao Materials Letters, Vol. 350 https://doi.org/10.1016/j.matlet.2023.134892	journal	November 2023
Multi-functionalities enabled fivefold applications of LaCo0.6Ni0.4O3−δ in intermediate temperature symmetrical solid oxide fuel/electrolysis cells Duan, Nanqi; Yang, Jiajun; Gao, Minrui Nano Energy, Vol. 77 https://doi.org/10.1016/j.nanoen.2020.105207	journal	November 2020
Rapid fabrication of lanthanum strontium cobalt ferrite (LSCF) with suppression of LSCF/YSZ chemical side reaction via flash light sintering for SOFCs Lim, Yonghyun; Park, Junghum; Lee, Hojae Nano Energy, Vol. 90 https://doi.org/10.1016/j.nanoen.2021.106524	journal	December 2021
In situ/operando regulation of the reaction activities on hetero-structured electrodes for solid oxide cells Hu, Tong; He, Fan; Liu, Meilin Progress in Materials Science, Vol. 133 https://doi.org/10.1016/j.pmatsci.2022.101050	journal	March 2023
Self-hydrating of a ceria-based catalyst enables efficient operation of solid oxide fuel cells on liquid fuels Xu, Kang; Zhang, Hua; Deng, Wanqing Science Bulletin, Vol. 68, Issue 21 https://doi.org/10.1016/j.scib.2023.09.012	journal	November 2023
High performance and stability of PrBa0.5Sr0.5Fe2O5+δ symmetrical electrode for intermediate temperature solid oxide fuel cells Wen, Chengyi; Chen, Kai; Guo, Dong Solid State Ionics, Vol. 386 https://doi.org/10.1016/j.ssi.2022.116048	journal	November 2022
Self-Regenerating Co–Fe Nanoparticles on Perovskite Oxides as a Hydrocarbon Fuel Oxidation Catalyst in Solid Oxide Fuel Cells Lai, Ke-Yu; Manthiram, Arumugam Chemistry of Materials, Vol. 30, Issue 8 https://doi.org/10.1021/acs.chemmater.7b04569	journal	March 2018
High-Entropy Alloys FeCoNiCuX (X = Al, Mo)-Ce_0.8Sm_0.2O₂ as High-Performance Solid Oxide Fuel Cell Anodes Chen, Dezhi; Huan, Yu; Ma, Guanjun ACS Applied Energy Materials, Vol. 6, Issue 2 https://doi.org/10.1021/acsaem.2c03655	journal	January 2023
Synergistically Promoting Coking Resistance of a La_0.4Sr_0.4Ti_0.85Ni_0.15O_3−δ Anode by Ru-Doping-Induced Active Twin Defects and Highly Dispersed Ni Nanoparticles Tang, Yawei; Wang, Haocong; Wang, Ruichen ACS Applied Materials & Interfaces, Vol. 14, Issue 38 https://doi.org/10.1021/acsami.2c15337	journal	September 2022
Robust Direct Hydrocarbon Solid Oxide Fuel Cells with Exsolved Anode Nanocatalysts Wang, Tengpeng; Wang, Runze; Xie, Xiaoyu ACS Applied Materials & Interfaces, Vol. 14, Issue 51 https://doi.org/10.1021/acsami.2c16284	journal	December 2022
A-Site Ordered Double Perovskite with in Situ Exsolved Core–Shell Nanoparticles as Anode for Solid Oxide Fuel Cells Hou, Nianjun; Yao, Tongtong; Li, Ping ACS Applied Materials & Interfaces, Vol. 11, Issue 7 https://doi.org/10.1021/acsami.8b19928	journal	January 2019
Reaction Pathway for Coke-Free Methane Steam Reforming on a Ni/CeO ₂ Catalyst: Active Sites and the Role of Metal–Support Interactions Salcedo, Agustín; Lustemberg, Pablo G.; Rui, Ning ACS Catalysis, Vol. 11, Issue 13 https://doi.org/10.1021/acscatal.1c01604	journal	June 2021
High-Performance Co-production of Electricity and Light Olefins Enabled by Exsolved NiFe Alloy Nanoparticles from a Double-Perovskite Oxide Anode in Solid Oxide-Ion-Conducting Fuel Cells Tan, Ting; Wang, Ziming; Huang, Kevin ACS Nano, Vol. 17, Issue 14 https://doi.org/10.1021/acsnano.3c03956	journal	July 2023
In Situ Exsolved NiFe/(NiFe)O_x Core–Shell-Structured Nanocatalysts on Perovskite Anode with Enhanced Coking Resistance Yang, Hongyu; La, Ming; Wang, Ziming ACS Sustainable Chemistry & Engineering, Vol. 10, Issue 38 https://doi.org/10.1021/acssuschemeng.2c01024	journal	September 2022
Catalytic Conversion of Carbon Dioxide to Methane on Ruthenium–Cobalt Bimetallic Nanocatalysts and Correlation between Surface Chemistry of Catalysts under Reaction Conditions and Catalytic Performances Zhu, Yuan; Zhang, Shiran; Ye, Yingchun ACS Catalysis, Vol. 2, Issue 11 https://doi.org/10.1021/cs3005242	journal	September 2012
Doped CeO ₂ –LaFeO ₃ Composite Oxide as an Active Anode for Direct Hydrocarbon-Type Solid Oxide Fuel Cells Shin, Tae Ho; Ida, Shintaro; Ishihara, Tatsumi Journal of the American Chemical Society, Vol. 133, Issue 48 https://doi.org/10.1021/ja206278f	journal	December 2011
Oxidation of H ₂ , CH ₄ , and CO Molecules at the Interface between Nickel and Yttria-Stabilized Zirconia: A Theoretical Study Based on DFT Shishkin, M.; Ziegler, T. The Journal of Physical Chemistry C, Vol. 113, Issue 52 https://doi.org/10.1021/jp905615c	journal	December 2009
Direct oxidation of hydrocarbons in a solid-oxide fuel cell Park, Seungdoo; Vohs, John M.; Gorte, Raymond J. Nature, Vol. 404, Issue 6775 https://doi.org/10.1038/35005040	journal	March 2000
Disruption of extended defects in solid oxide fuel cell anodes for methane oxidation Ruiz-Morales, Juan Carlos; Canales-Vázquez, Jesús; Savaniu, Cristian Nature, Vol. 439, Issue 7076 https://doi.org/10.1038/nature04438	journal	February 2006
Promotion of water-mediated carbon removal by nanostructured barium oxide/nickel interfaces in solid oxide fuel cells Yang, Lei; Choi, YongMan; Qin, Wentao Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1359	journal	June 2011
Layered oxygen-deficient double perovskite as an efficient and stable anode for direct hydrocarbon solid oxide fuel cells Sengodan, Sivaprakash; Choi, Sihyuk; Jun, Areum Nature Materials, Vol. 14, Issue 2 https://doi.org/10.1038/nmat4166	journal	December 2014
A redox-stable efficient anode for solid-oxide fuel cells Tao, Shanwen; Irvine, John T. S. Nature Materials, Vol. 2, Issue 5 https://doi.org/10.1038/nmat871	journal	March 2003
Electrochemical conversion of methane to ethylene in a solid oxide electrolyzer Zhu, Changli; Hou, Shisheng; Hu, Xiuli Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09083-3	journal	March 2019
A robust fuel cell operated on nearly dry methane at 500 °C enabled by synergistic thermal catalysis and electrocatalysis Chen, Yu; deGlee, Ben; Tang, Yu Nature Energy, Vol. 3, Issue 12 https://doi.org/10.1038/s41560-018-0262-5	journal	October 2018
Highly durable, coking and sulfur tolerant, fuel-flexible protonic ceramic fuel cells Duan, Chuancheng; Kee, Robert J.; Zhu, Huayang Nature, Vol. 557, Issue 7704 https://doi.org/10.1038/s41586-018-0082-6	journal	May 2018
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
Carbon-tolerant Ni-based cermet anodes modified by proton conducting yttrium- and ytterbium-doped barium cerates for direct methane solid oxide fuel cells Li, Meng; Hua, Bin; Luo, Jing-li Journal of Materials Chemistry A, Vol. 3, Issue 43 https://doi.org/10.1039/C5TA06488K	journal	January 2015
Demonstration of high performance in a perovskite oxide supported solid oxide fuel cell based on La and Ca co-doped SrTiO ₃ Lu, Lanying; Ni, Chengsheng; Cassidy, Mark Journal of Materials Chemistry A, Vol. 4, Issue 30 https://doi.org/10.1039/C6TA04074H	journal	January 2016
Direct application of cobaltite-based perovskite cathodes on the yttria-stabilized zirconia electrolyte for intermediate temperature solid oxide fuel cells Chen, Kongfa; Li, Na; Ai, Na Journal of Materials Chemistry A, Vol. 4, Issue 45 https://doi.org/10.1039/C6TA07067A	journal	January 2016
Smart utilization of cobaltite-based double perovskite cathodes on barrier-layer-free zirconia electrolyte of solid oxide fuel cells Li, Meng; Chen, Kongfa; Hua, Bin Journal of Materials Chemistry A, Vol. 4, Issue 48 https://doi.org/10.1039/C6TA08396J	journal	January 2016
Corn-cob like nanofibres as cathode catalysts for an effective microstructure design in solid oxide fuel cells Jeon, Yukwon; Myung, Jae-ha; Hyun, Sang-hoon Journal of Materials Chemistry A, Vol. 5, Issue 8 https://doi.org/10.1039/C6TA08692F	journal	January 2017
Highly active and stable Er_0.4Bi_1.6O₃ decorated La_0.76Sr_0.19MnO_3+δ nanostructured oxygen electrodes for reversible solid oxide cells Ai, Na; Li, Na; He, Shuai Journal of Materials Chemistry A, Vol. 5, Issue 24 https://doi.org/10.1039/C7TA02950K	journal	January 2017
Ce-doped La _0.7 Sr _0.3 Fe _0.9 Ni _0.1 O _3−δ as symmetrical electrodes for high performance direct hydrocarbon solid oxide fuel cells Bian, Liuzhen; Duan, Chuancheng; Wang, Lijun Journal of Materials Chemistry A, Vol. 5, Issue 29 https://doi.org/10.1039/C7TA03001K	journal	January 2017
Bismuth-doped La_1.75Sr_0.25NiO_4+δ as a novel cathode material for solid oxide fuel cells Zhu, Zhesheng; Li, Mei; Xia, Changrong Journal of Materials Chemistry A, Vol. 5, Issue 27 https://doi.org/10.1039/C7TA03381H	journal	January 2017
Enhanced sinterability and electrochemical performance of solid oxide fuel cellsviaa roll calendering process Kim, Junseok; Ahn, Junsung; Shin, Jisu Journal of Materials Chemistry A, Vol. 7, Issue 16 https://doi.org/10.1039/C9TA01818B	journal	January 2019
Enhancement of Ni–(Y ₂ O ₃ ) _0.08 (ZrO ₂ ) _0.92 fuel electrode performance by infiltration of Ce _0.8 Gd _0.2 O _2−δ nanoparticles Park, Beom-Kyeong; Scipioni, Roberto; Cox, Dalton Journal of Materials Chemistry A, Vol. 8, Issue 7 https://doi.org/10.1039/C9TA12316D	journal	January 2020
Advanced oxygen-electrode-supported solid oxide electrochemical cells with Sr(Ti,Fe)O _3−δ -based fuel electrodes for electricity generation and hydrogen production Zhang, Shan-Lin; Wang, Hongqian; Yang, Tianrang Journal of Materials Chemistry A, Vol. 8, Issue 48 https://doi.org/10.1039/D0TA06678H	journal	January 2020
In situ observation of highly oxidized Ru species in Ru/CeO₂ catalyst under propane oxidation Bezkrovnyi, Oleksii; Vorokhta, Mykhailo; Pawlyta, Mirosława Journal of Materials Chemistry A, Vol. 10, Issue 31 https://doi.org/10.1039/D2TA02330J	journal	January 2022
Boosting the performance of reversible solid oxide electrochemical cells with a novel hybrid oxygen electrode, Pr_1.39Ba_0.14Sr_0.53Co_1.48Fe_0.76O_6−δ-Ba_0.66Sr_0.34CoO_3−δ Fang, Liyang; Liu, Fan; Diercks, David Journal of Materials Chemistry A, Vol. 11, Issue 39 https://doi.org/10.1039/D3TA03629D	journal	January 2023
An Octane-Fueled Solid Oxide Fuel Cell Zhan, Z. Science, Vol. 308, Issue 5723 https://doi.org/10.1126/science.1109213	journal	May 2005
Double Perovskites as Anode Materials for Solid-Oxide Fuel Cells Huang, Y. -H. Science, Vol. 312, Issue 5771 https://doi.org/10.1126/science.1125877	journal	April 2006
Quantifying Percolated Triple Phase Boundary Density and Its Effects on Anodic Polarization in Ni-Infiltrated Ni/YSZ SOFC Anodes Rix, Jillian G.; Mo, Boshan; Nikiforov, Alexey Y. Journal of The Electrochemical Society, Vol. 168, Issue 11 https://doi.org/10.1149/1945-7111/ac3599	journal	November 2021

Similar Records

An efficient construction of nano-interfaces for excellent coking tolerance of cermet anodes

Journal Article · 2024 · Materials Today · OSTI ID:2473068

Xu, Kang; Zhang, Hua; Xu, Yangsen; +6 more

A robust fuel cell operated on nearly dry methane at 500 °C enabled by synergistic thermal catalysis and electrocatalysis

Journal Article · 2018 · Nature Energy · OSTI ID:1877397

Chen, Yu; deGlee, Ben; Tang, Yu; +11 more

Catalytic and electrocatalytic performance of Sr(Ti_0.3Fe_0.7Ru_0.07)O_3-δ for applications in solid oxide fuel cells supplied with ethanol steam reforming mixtures

Journal Article · 2022 · Journal of Power Sources · OSTI ID:1906721

Donazzi, Alessandro; Schmauss, Travis A.; Barnett, Scott A.

Related Subjects

30 DIRECT ENERGY CONVERSION
Coking tolerance
Nano-heterostructure
Ni-cermet anodes
Solid oxide fuel cells
catalysts

Title: Realizing efficient operations of Ni-cermet-based fuel cells on hydrocarbons via an in situ self-assembled metal/oxide nano-heterostructured catalyst

Citation Formats

References (63)

Similar Records

Related Subjects