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Creating metal-carbide interactions to boost ammonia oxidation activity for low-temperature direct ammonia fuel cells
被引:27
作者:
Fang, Huihuang
[1
,2
]
Liao, Chen
[1
]
Ying, Yiran
[3
]
Cheng, Jinxing
[1
]
Wang, Qiuxiang
[4
]
Huang, Haitao
[3
]
Luo, Yu
[1
,2
]
Jiang, Lilong
[1
,2
]
机构:
[1] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst NERC CF, Sch Chem Engn, Fuzhou 350002, Peoples R China
[2] Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China
[3] Hong Kong Polytech Univ, Res Inst Smart Energy, Dept Appl Phys, Hung Hom,Kowloon, Hong Kong, Peoples R China
[4] Huaqiao Univ, Instrumental Anal Ctr, Xiamen 361021, Peoples R China
基金:
中国国家自然科学基金;
国家重点研发计划;
关键词:
Ammonia oxidation;
Tungsten carbide;
Metal -support interaction;
Direct ammonia fuel cell;
TUNGSTEN CARBIDE;
BIMETALLIC CLUSTERS;
HYDROGEN OXIDATION;
PLATINUM;
IR;
CATALYSTS;
ELECTROCATALYSTS;
ELECTROOXIDATION;
CARBON;
DFT;
D O I:
10.1016/j.jcat.2022.11.028
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:
Low-temperature direct ammonia fuel cell (DAFC) can easily transform the chemical energy into green in-commission power, yet remains great challenging due to kinetically sluggish ammonia oxidation reaction (AOR). The interface engineering is a promising strategy to take advantage of synergistic proficiencies and electronic properties, which was widely applied in heterogeneous catalysis but rarely studied in AOR. Herein, non-oxide-based metal-metal carbide interfaces were employed to construct excellent AOR catalysts. The as-built Pt/WC and PtIr/WC catalysts with the excellent peak current densities of 96.5 and 61.7 A gPGM -1 , respectively, which are over 3.5-fold and 2.7-fold than those of carbon-supported catalysts. Both experimental and theoretical studies reveal that the charge transfer between PtIr NPs and WC regulates the work function and d-band center of catalysts and further alters adsorption energies of intermediates. The WC also plays an important role for water dissociation and hydroxyl group activation. Based on the understanding, maximizing active interfaces by dispersing PtIr-WC composites onto CNTs (PtIr-WC/CNT) achieves a compelling peak power density of 140.0 mW cm-2 at 80 degrees C in a DAFC test, which is at the top of previously reported catalysts at similar conditions. Our study provides a way to design highly-active catalysts for AOR and DAFC by interface engineering.(c) 2022 Elsevier Inc. All rights reserved.
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页码:129 / 139
页数:11
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