Cooperative Active Sites on Ag 2 Pt 3 TiS 6 for Enhanced Low-Temperature Ammonia Fuel Cell Electrocatalysis.

Autor: Wu T; Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Republic of Singapore.; Centre for Hydrogen Innovations, National University of Singapore, Singapore, 117580, Republic of Singapore., Dhaka K; Faculty of Chemistry, Theoretical Inorganic Chemistry, University of Duisburg-Essen, Universitätsstraße 5, 45141, Essen, Germany., Luo M; Nanchang Key Laboratory of Photoelectric Conversion and Energy Storage Materials, Nanchang Institute of Technology, Nanchang, 330099, China., Wang B; Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Republic of Singapore., Wang M; Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Republic of Singapore.; Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Innovis #08-03, Singapore, 138634, Republic of Singapore., Xi S; Institute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR), 1 Pesek Road, Singapore, 627833, Republic of Singapore., Zhang M; Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Innovis #08-03, Singapore, 138634, Republic of Singapore., Huang F; State Key Lab of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China., Exner KS; Faculty of Chemistry, Theoretical Inorganic Chemistry, University of Duisburg-Essen, Universitätsstraße 5, 45141, Essen, Germany.; Cluster of Excellence RESOLV, 44801, Bochum, Germany.; Center for Nanointegration (CENIDE) Duisburg-Essen, 47057, Duisburg, Germany., Lum Y; Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Republic of Singapore.; Centre for Hydrogen Innovations, National University of Singapore, Singapore, 117580, Republic of Singapore.; Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Innovis #08-03, Singapore, 138634, Republic of Singapore.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Nov 26, pp. e202418691. Date of Electronic Publication: 2024 Nov 26.
DOI: 10.1002/anie.202418691
Abstrakt: Ammonia has attracted considerable interest as a hydrogen carrier that can help decarbonize global energy networks. Key to realizing this is the development of low temperature ammonia fuel cells for the on-demand generation of electricity. However, the efficiency of such systems is significantly impaired by the sluggish ammonia oxidation reaction (AOR) and oxygen reduction reaction (ORR). Here, we report the design of a bifunctional Ag 2 Pt 3 TiS 6 electrocatalyst that facilitates both reactions at mass activities exceeding that of commercial Pt/C. Through comprehensive density functional theory calculations, we identify that active site motifs composed of Pt and Ti atoms work cooperatively to catalyze ORR and AOR. Notably, in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) experiments indicate a decreased propensity for *NO x formation and hence an increased resistance toward catalyst poisoning for AOR. Employing Ag 2 Pt 3 TiS 6 as both the cathode and anode, we constructed a low temperature ammonia fuel cell with a high peak power density of 8.71 mW cm -2 and low Pt loading of 0.45 mg cm -2 . Our findings demonstrate a pathway towards the rational design of effective electrocatalysts with multi-element active sites that work cooperatively.
(© 2024 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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