Ultrastable and Phosphoric Acid-Resistant PtRhCu@Pt Oxygen Reduction Electrocatalyst for High-Temperature Polymer Electrolyte Fuel Cells

被引:7
作者
An, Zhao [1 ,2 ,3 ]
Li, Huanqiao [1 ,2 ]
Zhang, Xiaoming [1 ,2 ]
Xia, Zhangxun [1 ,2 ]
Zhang, Hong [1 ,2 ,3 ]
Chu, Wenling [4 ]
Yu, Shansheng [5 ]
Wang, Suli [1 ,2 ]
Sun, Gongquan [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Div Fuel Cells & Battery, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Key Lab Fuel Cell & Hybrid Power Sources, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[5] Jilin Univ, Dept Mat Sci, Changchun 130012, Peoples R China
基金
中国国家自然科学基金;
关键词
HT-PEMFCs; oxygen reduction reaction; phosphoricacid resistance electrocatalysts; core-shell; self-healing; stability; DEGRADATION MECHANISMS; ALLOY NANOPARTICLES; ADSORPTION; CATALYSTS; PERFORMANCE;
D O I
10.1021/acscatal.3c04488
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
With much enhanced fuel flexibility to overcome the shortcomings of hydrogen production and storage, high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) are still facing challenges of activity loss of oxygen reduction electrocatalyst under the working circumstance of phosphoric acid (PA) electrolyte. Dissolution and leaching of metal component of PtM (M = Cu, Co, Ni<middle dot><middle dot><middle dot>) electrocatalysts is one of the key factors that degrade their initial resistance toward PA and hinder the accessing of activity and durability simultaneously. Here, we report an ultradurable PtRhCu@Pt/C electrocatalyst with a high mass activity of 0.90 A mg(Pt)(-1), which only decreased by 14.4% after 30K ADT cycles in the half-cell and reaches the DOE at 2025 target (<30 mV at 0.8 A cm(-2)) with 27 mV voltage loss at 0.8 A cm(-2) in the single-cell. After adding 0.1 M PA into the electrolyte, the half-wave potential of PtRhCu@Pt/C is negatively shifted by only 52 mV, much lower than that of commercial Pt/C (90 mV). Moreover, the HT-PEMFC assembled by this catalyst delivers a preeminent peak power density of 529 and 977 mW cm(-2) under H-2-air and H-2-O-2 conditions, respectively. Experiments and theoretical calculations reveal that the ligand effect arising from the sublayer Cu is attributed to the ability of PA resistance, while the self-healing behavior and the synergy between the PtRhCu core and the Pt shell ensures high stability.
引用
收藏
页码:2572 / 2581
页数:10
相关论文
共 59 条
[31]   Preparation, characterization and degradation mechanisms of PtCu alloy nanoparticles for automotive fuel cells [J].
Marcu, A. ;
Toth, G. ;
Srivastava, R. ;
Strasser, P. .
JOURNAL OF POWER SOURCES, 2012, 208 :288-295
[32]   SPECIAL POINTS FOR BRILLOUIN-ZONE INTEGRATIONS [J].
CHADI, DJ .
PHYSICAL REVIEW B, 1977, 16 (04) :1746-1747
[33]   Origin of the overpotential for oxygen reduction at a fuel-cell cathode [J].
Norskov, JK ;
Rossmeisl, J ;
Logadottir, A ;
Lindqvist, L ;
Kitchin, JR ;
Bligaard, T ;
Jónsson, H .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (46) :17886-17892
[34]   A review of accelerated stress tests dedicated to proton exchange membrane fuel cells-Part I: Fuel cell component level [J].
Pahon, E. ;
Hissel, D. ;
Yousfi-Steiner, N. .
JOURNAL OF POWER SOURCES, 2022, 546
[35]   Transition metal alloying effect on the phosphoric acid adsorption strength of Pt nanoparticles: an experimental and density functional theory study [J].
Park, Hee-Young ;
Lim, Dong-Hee ;
Yoo, Sung Jong ;
Kim, Hyoung-Juhn ;
Henkensmeier, Dirk ;
Kim, Jin Young ;
Ham, Hyung Chul ;
Jang, Jong Hyun .
SCIENTIFIC REPORTS, 2017, 7
[36]   Generalized gradient approximation for the exchange-correlation hole of a many-electron system [J].
Perdew, JP ;
Burke, K ;
Wang, Y .
PHYSICAL REVIEW B, 1996, 54 (23) :16533-16539
[37]   A review of high-temperature proton exchange membrane fuel cell (HT-PEMFC) system [J].
Rosli, R. E. ;
Sulong, A. B. ;
Daud, W. R. W. ;
Zullzifley, M. A. ;
Husaini, T. ;
Rosli, M. I. ;
Majlan, E. H. ;
Haque, M. A. .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2017, 42 (14) :9293-9314
[38]   Surface electronic structure and reactivity of transition and noble metals [J].
Ruban, A ;
Hammer, B ;
Stoltze, P ;
Skriver, HL ;
Norskov, JK .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1997, 115 (03) :421-429
[39]   First-principles simulation: ideas, illustrations and the CASTEP code [J].
Segall, MD ;
Lindan, PJD ;
Probert, MJ ;
Pickard, CJ ;
Hasnip, PJ ;
Clark, SJ ;
Payne, MC .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2002, 14 (11) :2717-2744
[40]   An opinion on catalyst degradation mechanisms during catalyst support focused accelerated stress test (AST) for proton exchange membrane fuel cells (PEMFCs) [J].
Sharma, Raghunandan ;
Andersen, Shuang Ma .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 239 :636-643