In situ formed catalysts for active, durable, and thermally stable ammonia protonic ceramic fuel cells at 550 °C

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

doi:10.1039/d4ee00219a

Title: In situ formed catalysts for active, durable, and thermally stable ammonia protonic ceramic fuel cells at 550 °C

Journal Article · 10 April 2024 · Energy & Environmental Science

DOI: https://doi.org/10.1039/d4ee00219a · OSTI ID:2372819

Zhang, Hua ^[1]; Xu, Kang ^[1]; Xu, Yangsen ^[1]; He, Fan ^[1]; Zhu, Feng ^[1];

^[2];

^[3];

^[1]

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

Ammonia protonic ceramic fuel cells (NH₃-PCFCs) are promising and attractive energy-conversion devices owing to their high energy density, zero-carbon emission, and safety. The development of NH₃-PCFCs, however, depends largely on the insufficient activity and poor durability of typical Ni-based anodes for ammonia decomposition, especially at low temperatures such as 550 °C. Herein, we report a self-assembled heterostructured Ru_0.95Cu_0.05Ni_x (RCN) catalyst obtained through an in situ reaction between the surface-decorated Ru_0.95Cu_0.05 nanoparticles and the Ni grain in the anode under typical processing conditions. At 550 °C, Ni–BaZr_0.1Ce_0.7Y_0.1Yb_0.1O₃ anode-supported PCFCs with RCN catalysts exhibit a high peak power density of 0.732 W cm^-2 and a significantly enhanced durability of 100 h in NH₃. Moreover, the cells demonstrate improved thermal stability compared with the bare cell during a 31-cycle thermal cycling test in NH₃ between 550 and 700 °C. In conclusion, the enhanced performance is likely attributed to the synergistic effects of Ru and Cu in RCN for NH₃ decomposition, resulting in a more vital interaction of NH₃ than that of the bare anode surfaces, as confirmed by NH₃ thermal conversion, electrochemical performance, and theoretical simulations.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); National Natural Science Foundation of China (NSFC); Natural Science Foundation of Guangdong Province; Innovative R&D Team of Guangdong; National Science and Technology Council (NSTC)

Grant/Contract Number:: SC0012704

OSTI ID:: 2372819

Report Number(s):: BNL--225711-2024-JAAM

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 10 Vol. 17; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (60)

Advanced Materials for Thin‐Film Solid Oxide Fuel Cells: Recent Progress and Challenges in Boosting the Device Performance at Low Temperatures Zhang, Jun; Ricote, Sandrine; Hendriksen, Peter Vang Advanced Functional Materials, Vol. 32, Issue 22 https://doi.org/10.1002/adfm.202111205	journal	March 2022
Towards the Next Generation of Solid Oxide Fuel Cells Operating Below 600 °C with Chemically Stable Proton-Conducting Electrolytes Fabbri, Emiliana; Bi, Lei; Pergolesi, Daniele Advanced Materials, Vol. 24, Issue 2 https://doi.org/10.1002/adma.201103102	journal	September 2011
Cation‐Vacancy‐Enriched Nickel Phosphide for Efficient Electrosynthesis of Hydrogen Peroxides Zhou, Zheng; Kong, Yuan; Tan, Hao Advanced Materials, Vol. 34, Issue 16 https://doi.org/10.1002/adma.202106541	journal	March 2022
Self‐Construction of Efficient Interfaces Ensures High‐Performance Direct Ammonia Protonic Ceramic Fuel Cells He, Fan; Hou, Mingyang; Du, Zhiwei Advanced Materials, Vol. 35, Issue 42 https://doi.org/10.1002/adma.202304957	journal	September 2023
A New Pd Doped Proton Conducting Perovskite Oxide with Multiple Functionalities for Efficient and Stable Power Generation from Ammonia at Reduced Temperatures He, Fan; Gao, Qinning; Liu, Zuoqing Advanced Energy Materials, Vol. 11, Issue 19 https://doi.org/10.1002/aenm.202003916	journal	March 2021
In Situ Observation of Cu-Ni Alloy Nanoparticle Formation by X-Ray Diffraction, X-Ray Absorption Spectroscopy, and Transmission Electron Microscopy: Influence of Cu/Ni Ratio Wu, Qiongxiao; Duchstein, Linus D. L.; Chiarello, Gian Luca ChemCatChem, Vol. 6, Issue 1 https://doi.org/10.1002/cctc.201300628	journal	December 2013
Triple-Conducting Layered Perovskites as Cathode Materials for Proton-Conducting Solid Oxide Fuel Cells Kim, Junyoung; Sengodan, Sivaprakash; Kwon, Goeun ChemSusChem, Vol. 7, Issue 10 https://doi.org/10.1002/cssc.201402351	journal	August 2014
High-Efficiency Direct Ammonia Fuel Cells Based on BaZr _0.1 Ce _0.7 Y _0.2 O ₃₋ _δ /Pd Oxide-Metal Junctions Aoki, Yoshitaka; Yamaguchi, Tomoyuki; Kobayashi, Shohei Global Challenges, Vol. 2, Issue 1 https://doi.org/10.1002/gch2.201700088	journal	December 2017
Realizing Simultaneous Detrimental Reactions Suppression and Multiple Benefits Generation from Nickel Doping toward Improved Protonic Ceramic Fuel Cell Performance Song, Yufei; Chen, Jiaming; Yang, Meiting Small, Vol. 18, Issue 16 https://doi.org/10.1002/smll.202200450	journal	March 2022
Visiting the roles of Sr‐ or Ca‐ doping on the oxygen reduction reaction activity and stability of a perovskite cathode for proton conducting solid oxide fuel cells Hu, Tong; Xu, Yangsen; Xu, Kang SusMat, Vol. 3, Issue 1 https://doi.org/10.1002/sus2.101	journal	January 2023
Atomic and Molecular Adsorption on Cu(111) Xu, Lang; Lin, Joshua; Bai, Yunhai Topics in Catalysis, Vol. 61, Issue 9-11 https://doi.org/10.1007/s11244-018-0943-0	journal	May 2018
Ammonia as a fuel in solid oxide fuel cells Wojcik, Adam; Middleton, Hugh; Damopoulos, Ioannis Journal of Power Sources, Vol. 118, Issue 1-2 https://doi.org/10.1016/S0378-7753(03)00083-1	journal	May 2003
Alloyed Ni-Fe nanoparticles as catalysts for NH3 decomposition Simonsen, Søren Bredmose; Chakraborty, Debasish; Chorkendorff, Ib Applied Catalysis A: General, Vol. 447-448 https://doi.org/10.1016/j.apcata.2012.08.045	journal	December 2012
Low-temperature ammonia decomposition catalysts for hydrogen generation Mukherjee, Shreya; Devaguptapu, Surya V.; Sviripa, Anna Applied Catalysis B: Environmental, Vol. 226 https://doi.org/10.1016/j.apcatb.2017.12.039	journal	June 2018
A high-performance and durable direct NH3 tubular protonic ceramic fuel cell integrated with an internal catalyst layer Pan, Yuxin; Zhang, Hua; Xu, Kang Applied Catalysis B: Environmental, Vol. 306 https://doi.org/10.1016/j.apcatb.2022.121071	journal	June 2022
Efficient and durable ammonia power generation by symmetric flat-tube solid oxide fuel cells Wang, Yuanhui; Gu, Yuchen; Zhang, Hua Applied Energy, Vol. 270 https://doi.org/10.1016/j.apenergy.2020.115185	journal	July 2020
RuCu bimetallic catalyst on N-doped mesoporous carbon for high-performance CO2 methanation Sun, Haoyue; Tang, Rui; Zhang, Xingmo Carbon Capture Science & Technology, Vol. 6 https://doi.org/10.1016/j.ccst.2023.100100	journal	March 2023
Effect of Ni diffusion into BaZr0.1Ce0.7Y0.1Yb0.1O3− electrolyte during high temperature co-sintering in anode-supported solid oxide fuel cells Shimada, Hiroyuki; Yamaguchi, Toshiaki; Sumi, Hirofumi Ceramics International, Vol. 44, Issue 3 https://doi.org/10.1016/j.ceramint.2017.11.081	journal	February 2018
Coordination engineering in single-site catalysts: General principles, characterizations, and recent advances Wang, Haozhu; Yang, Tao; Wang, Jingyang Chem, Vol. 10, Issue 1 https://doi.org/10.1016/j.chempr.2023.08.014	journal	January 2024
Thermodynamic analysis of 100% system fuel utilization solid oxide fuel cell (SOFC) system fueled with ammonia Selvam, Kalimuthu; Komatsu, Yosuke; Sciazko, Anna Energy Conversion and Management, Vol. 249 https://doi.org/10.1016/j.enconman.2021.114839	journal	December 2021
Thermodynamic analysis of SOFC (solid oxide fuel cell)–Stirling hybrid plants using alternative fuels Rokni, Masoud Energy, Vol. 61 https://doi.org/10.1016/j.energy.2013.06.001	journal	November 2013
Ammonia as a green energy carrier: Electrochemical synthesis and direct ammonia fuel cell - a comprehensive review Wang, Bin; Li, Tao; Gong, Feng Fuel Processing Technology, Vol. 235 https://doi.org/10.1016/j.fuproc.2022.107380	journal	October 2022
Proton-conducting fuel cells operating on hydrogen, ammonia and hydrazine at intermediate temperatures Lin, Ye; Ran, Ran; Guo, Youmin International Journal of Hydrogen Energy, Vol. 35, Issue 7 https://doi.org/10.1016/j.ijhydene.2009.04.019	journal	April 2010
Energy and exergy analyses of a combined ammonia-fed solid oxide fuel cell system for vehicular applications Baniasadi, Ehsan; Dincer, Ibrahim International Journal of Hydrogen Energy, Vol. 36, Issue 17 https://doi.org/10.1016/j.ijhydene.2011.04.234	journal	August 2011
Formulation of ammonia decomposition rate in Ni-YSZ anode of solid oxide fuel cells Kishimoto, Masashi; Furukawa, Naoto; Kume, Tatsuya International Journal of Hydrogen Energy, Vol. 42, Issue 4 https://doi.org/10.1016/j.ijhydene.2016.11.183	journal	January 2017
Catalytic ammonia decomposition for hydrogen production on Ni, Ru and Ni Ru supported on CeO2 Lucentini, Ilaria; Casanovas, Albert; Llorca, Jordi International Journal of Hydrogen Energy, Vol. 44, Issue 25 https://doi.org/10.1016/j.ijhydene.2019.01.154	journal	May 2019
Ruthenium catalyst supported on Ba modified ZrO2 for ammonia decomposition to COx-free hydrogen Wang, Ziqing; Qu, Yingmin; Shen, Xiaolong International Journal of Hydrogen Energy, Vol. 44, Issue 14 https://doi.org/10.1016/j.ijhydene.2019.01.235	journal	March 2019
A comprehensive investigation of direct ammonia-fueled thin-film solid-oxide fuel cells: Performance, limitation, and prospects Oh, Seongkook; Oh, Min Jun; Hong, Jongsup iScience, Vol. 25, Issue 9 https://doi.org/10.1016/j.isci.2022.105009	journal	September 2022
An intermediate temperature direct ammonia fuel cell using a proton conducting electrolyte Maffei, N.; Pelletier, L.; Charland, J. Journal of Power Sources, Vol. 140, Issue 2 https://doi.org/10.1016/j.jpowsour.2004.08.020	journal	February 2005
An ammonia fuel cell using a mixed ionic and electronic conducting electrolyte Maffei, N.; Pelletier, L.; Charland, J. P. Journal of Power Sources, Vol. 162, Issue 1 https://doi.org/10.1016/j.jpowsour.2006.06.056	journal	November 2006
Comparative study on the performance of a SDC-based SOFC fueled by ammonia and hydrogen Meng, Guangyao; Jiang, Cairong; Ma, Jianjun Journal of Power Sources, Vol. 173, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.05.002	journal	November 2007
A high performance direct ammonia fuel cell using a mixed ionic and electronic conducting anode Maffei, N.; Pelletier, L.; McFarlan, A. Journal of Power Sources, Vol. 175, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.09.040	journal	January 2008
Comparative study on ammonia oxidation over Ni-based cermet anodes for solid oxide fuel cells Molouk, Ahmed Fathi Salem; Yang, Jun; Okanishi, Takeou Journal of Power Sources, Vol. 305 https://doi.org/10.1016/j.jpowsour.2015.11.085	journal	February 2016
Development of Ni–Ba(Zr,Y)O3 cermet anodes for direct ammonia-fueled solid oxide fuel cells Miyazaki, Kazunari; Okanishi, Takeou; Muroyama, Hiroki Journal of Power Sources, Vol. 365 https://doi.org/10.1016/j.jpowsour.2017.08.085	journal	October 2017
Ammonia decomposition on Fe(110), Co(111) and Ni(111) surfaces: A density functional theory study Duan, Xuezhi; Ji, Jian; Qian, Gang Journal of Molecular Catalysis A: Chemical, Vol. 357 https://doi.org/10.1016/j.molcata.2012.01.023	journal	May 2012
Advances and challenges in developing protonic ceramic cells Kim, Donguk; Lee, Tae Kyeong; Han, Seungwoo Materials Today Energy, Vol. 36 https://doi.org/10.1016/j.mtener.2023.101365	journal	August 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
Enhanced n-pentanol sensing performance by RuCu alloy nanoparticles decorated SnO2 nanoclusters Wang, Chenchang; Bai, Jihao; Wang, Hongtao Sensors and Actuators B: Chemical, Vol. 351 https://doi.org/10.1016/j.snb.2021.130900	journal	January 2022
On the use of NiO as sintering additive for BaCe0,9Y0,1O3−α Costa, R.; Grünbaum, N.; Berger, M. -H. Solid State Ionics, Vol. 180, Issue 11-13 https://doi.org/10.1016/j.ssi.2009.02.018	journal	June 2009
Enhancement of anode activity at Ni/Sm-doped CeO2 cermet anodes by Mo addition in NH3-fueled solid oxide fuel cells Hashinokuchi, Michihiro; Yokochi, Ryuji; Akimoto, Wataru Solid State Ionics, Vol. 285 https://doi.org/10.1016/j.ssi.2015.07.021	journal	February 2016
First-principles calculations of ammonia decomposition on Ni(110) surface Duan, Xuezhi; Qian, Gang; Fan, Chen Surface Science, Vol. 606, Issue 3-4 https://doi.org/10.1016/j.susc.2011.11.030	journal	February 2012
Atomic and molecular adsorption on Ni(111) Bai, Yunhai; Kirvassilis, Demetrios; Xu, Lang Surface Science, Vol. 679 https://doi.org/10.1016/j.susc.2018.08.004	journal	January 2019
Review on Ru-Based and Ni-Based Catalysts for Ammonia Decomposition: Research Status, Reaction Mechanism, and Perspectives Su, Tianxu; Guan, Bin; Zhou, Jiefei Energy & Fuels, Vol. 37, Issue 12 https://doi.org/10.1021/acs.energyfuels.3c00804	journal	May 2023
Electrochemical and Catalytic Properties of Ni/BaCe _0.75 Y _0.25 O _3−δ Anode for Direct Ammonia-Fueled Solid Oxide Fuel Cells Yang, Jun; Molouk, Ahmed Fathi Salem; Okanishi, Takeou ACS Applied Materials & Interfaces, Vol. 7, Issue 13 https://doi.org/10.1021/acsami.5b01048	journal	March 2015
An Active and Robust Air Electrode for Reversible Protonic Ceramic Electrochemical Cells Zhou, Yucun; Liu, Enzuo; Chen, Yu ACS Energy Letters https://doi.org/10.1021/acsenergylett.1c00432	journal	March 2021
A Priori Catalytic Activity Correlations: The Difficult Case of Hydrogen Production from Ammonia Ganley, J. C.; Thomas, F. S.; Seebauer, E. G. Catalysis Letters, Vol. 96, Issue 3/4 https://doi.org/10.1023/B:CATL.0000030108.50691.d4	journal	July 2004
Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts Liu, Yangyang; Li, Can; Tan, Chunhui Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-38129-w	journal	April 2023
Direct methane protonic ceramic fuel cells with self-assembled Ni-Rh bimetallic catalyst Hong, Kyungpyo; Choi, Mingi; Bae, Yonggyun Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-43388-8	journal	November 2023
Lowering the operating temperature of protonic ceramic electrochemical cells to <450 °C Liu, Fan; Deng, Hao; Diercks, David Nature Energy, Vol. 8, Issue 10 https://doi.org/10.1038/s41560-023-01350-4	journal	September 2023
Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst Chen, Feng-Yang; Wu, Zhen-Yu; Gupta, Srishti Nature Nanotechnology, Vol. 17, Issue 7 https://doi.org/10.1038/s41565-022-01121-4	journal	May 2022
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
Ammonia-fed reversible protonic ceramic fuel cells with Ru-based catalyst Zhu, Liangzhu; Cadigan, Chris; Duan, Chuancheng Communications Chemistry, Vol. 4, Issue 1 https://doi.org/10.1038/s42004-021-00559-2	journal	August 2021
A perspective on low-temperature solid oxide fuel cells Gao, Zhan; Mogni, Liliana V.; Miller, Elizabeth C. Energy & Environmental Science, Vol. 9, Issue 5 https://doi.org/10.1039/C5EE03858H	journal	January 2016
Impact of the ammonia decomposition reaction over an anode on direct ammonia-fueled protonic ceramic fuel cells Miyazaki, Kazunari; Muroyama, Hiroki; Matsui, Toshiaki Sustainable Energy & Fuels, Vol. 4, Issue 10 https://doi.org/10.1039/D0SE00841A	journal	January 2020
An efficient and durable anode for ammonia protonic ceramic fuel cells Zhang, Hua; Zhou, Yucun; Pei, Kai Energy & Environmental Science, Vol. 15, Issue 1 https://doi.org/10.1039/D1EE02158C	journal	January 2022
Hydrogen generation via ammonia decomposition on highly efficient and stable Ru-free catalysts: approaching complete conversion at 450 °C Tabassum, Hassina; Mukherjee, Shreya; Chen, Junjie Energy & Environmental Science, Vol. 15, Issue 10 https://doi.org/10.1039/D1EE03730G	journal	January 2022
Ammonia for hydrogen storage: challenges and opportunities Klerke, Asbjørn; Christensen, Claus Hviid; Nørskov, Jens K. Journal of Materials Chemistry, Vol. 18, Issue 20 https://doi.org/10.1039/b720020j	journal	January 2008
Protonic ceramic materials for clean and sustainable energy: advantages and challenges Tian, Hanchen; Luo, Zheyu; Song, Yufei International Materials Reviews, Vol. 68, Issue 3 https://doi.org/10.1080/09506608.2022.2068399	journal	May 2022
Enhanced Sulfur and Coking Tolerance of a Mixed Ion Conductor for SOFCs: BaZr_0.1Ce_0.7Y_0.2–xYb_xO_3–δ Yang, L.; Wang, S.; Blinn, K. Science, Vol. 326, Issue 5949, p. 126-129 https://doi.org/10.1126/science.1174811	journal	October 2009
Direct ammonia fueled solid oxide fuel cells: A comprehensive review on challenges, opportunities and future outlooks Asmare, Molla; Ilbas, Mustafa International Journal of Energy Technology https://doi.org/10.32438/IJET.203011	journal	July 2020

Similar Records

An efficient and durable anode for ammonia protonic ceramic fuel cells

Journal Article · 2021 · Energy & Environmental Science · OSTI ID:1838162

Zhang, Hua; Zhou, Yucun; Pei, Kai; +8 more

A high-performance and durable direct NH₃ tubular protonic ceramic fuel cell integrated with an internal catalyst layer

Journal Article · 2022 · Applied Catalysis. B, Environmental · OSTI ID:1869254

Pan, Yuxin; Zhang, Hua; Xu, Kang; +7 more

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

Journal Article · 2024 · Applied Catalysis. B, Environmental · OSTI ID:2500290

Xu, Kang; Zhang, Hua; Xu, Yangsen; +5 more

Related Subjects

30 DIRECT ENERGY CONVERSION
Ammonia protonic ceramic fuel cells
Durability
Hetero-structured catalysts
In-situ formation

Title: In situ formed catalysts for active, durable, and thermally stable ammonia protonic ceramic fuel cells at 550 °C

Citation Formats

References (60)

Similar Records

Related Subjects