气候变化领域集成服务门户(CCPortal): High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells

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DOI	10.1039/d0ee03351k
	High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells
	Li Y.; Pillai H.S.; Wang T.; Hwang S.; Zhao Y.; Qiao Z.; Mu Q.; Karakalos S.; Chen M.; Yang J.; Su D.; Xin H.; Yan Y.; Wu G.
发表日期	2021
ISSN	17545692
起始页码	1449
结束页码	1460
卷号	14 期号:3
英文摘要	Low-temperature direct ammonia fuel cells (DAFCs) use carbon-neutral ammonia as a fuel, which has attracted increasing attention recently due to ammonia's low source-to-tank energy cost, easy transport and storage, and wide availability. However, current DAFC technologies are greatly limited by the kinetically sluggish ammonia oxidation reaction (AOR) at the anode. Herein, we report an AOR catalyst, in which ternary PtIrZn nanoparticles with an average size of 2.3 ± 0.2 nm were highly dispersed on a binary composite support comprising cerium oxide (CeO2) and zeolitic imidazolate framework-8 (ZIF-8)-derived carbon (PtIrZn/CeO2-ZIF-8) through a sonochemical-assisted synthesis method. The PtIrZn alloy, with the aid of abundant OHad provided by CeO2 and uniform particle dispersibility contributed by porous ZIF-8 carbon (surface area: ∼600 m2 g-1), has shown highly efficient catalytic activity for the AOR in alkaline media, superior to that of commercial PtIr/C. The rotating disk electrode (RDE) results indicate a lower onset potential (0.35 vs. 0.43 V), relative to the reversible hydrogen electrode at room temperature, and a decreased activation energy (∼36.7 vs. 50.8 kJ mol-1) relative to the PtIr/C catalyst. Notably, the PtIrZn/CeO2-ZIF-8 catalyst was assembled with a high-performance hydroxide anion-exchange membrane to fabricate an alkaline DAFC, reaching a peak power density of 91 mW cm-2. Unlike in aqueous electrolytes, supports play a critical role in improving uniform ionomer distribution and mass transport in the anode. PtIrZn nanoparticles on silicon dioxide (SiO2) integrated with carboxyl-functionalized carbon nanotubes (CNT-COOH) were further studied as the anode in a DAFC. A significantly enhanced peak power density of 314 mW cm-2 was achieved. Density functional theory calculations elucidated that Zn atoms in the PtIr alloy can reduce the theoretical limiting potential of ∗NH2 dehydrogenation to ∗NH by ∼0.1 V, which can be attributed to a Zn-modulated upshift of the Pt-Ir d-band that facilitates the N-H bond breakage. © 2021 The Royal Society of Chemistry.
英文关键词	Activation energy; Alkaline fuel cells; Ammonia; Anodes; Binary alloys; Carbon nanotubes; Catalyst activity; Cerium oxide; Density functional theory; Fuel storage; Ion exchange membranes; Nanoparticles; Silica; Silicon oxides; SiO2 nanoparticles; Synthesis (chemical); Temperature; Ternary alloys; Uranium alloys; Anion exchange membrane; Aqueous electrolyte; Carboxyl-functionalized; Direct ammonia fuel cells; Peak power densities; Reversible hydrogen electrodes; Rotating disk electrodes; Zeolitic imidazolate framework-8; Direct alcohol fuel cells (DAFC); ammonia; catalyst; fuel cell; membrane; performance assessment
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190746
作者单位	Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, United States; School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China; Department of Chemical Engineering, Virginia Polytechnic Institute, State University, Blacksburg, VA 24061, United States; Department of Chemical and Biomolecular Engineering, Center for Catalytic Science and Technology, University of Delaware, Newark, DE 19716, United States; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, United States; Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208, United States
推荐引用方式 GB/T 7714	Li Y.,Pillai H.S.,Wang T.,et al. High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells[J],2021,14(3).
APA	Li Y..,Pillai H.S..,Wang T..,Hwang S..,Zhao Y..,...&Wu G..(2021).High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells.Energy & Environmental Science,14(3).
MLA	Li Y.,et al."High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells".Energy & Environmental Science 14.3(2021).