Interfacial oxygen atom modification of a PdSn alloy to boost oxygen reduction in zinc-air batteries

Modifying the surface of a catalyst with heteroatoms can regulate the interfacial atomic valence state and adjust the charge distribution, which is promising for obtaining desirable platinum carbon catalyst (Pt/C)-matched oxygen reduction reaction (ORR) catalytic performance. Here, we developed an e...

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Veröffentlicht in:Journal of colloid and interface science 2024-04, Vol.659, p.257-266
Hauptverfasser: Li, Zongge, Chen, Jiabao, Guo, Yajie, Zheng, Fuxian, Qu, Konggang, Wang, Lei, Li, Rui, Xiong, Shenglin, Kang, Wenjun, Li, Haibo
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Sprache:eng
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Zusammenfassung:Modifying the surface of a catalyst with heteroatoms can regulate the interfacial atomic valence state and adjust the charge distribution, which is promising for obtaining desirable platinum carbon catalyst (Pt/C)-matched oxygen reduction reaction (ORR) catalytic performance. Here, we developed an efficient method to access O-rich crystalline interfacial-exposed palladium-tin alloy (111) crystal surfaces [Pd Sn (111)] for highly efficient ORR via direct reduction of Pd/Sn metal salt species that are well dispersed in a nitrogen, phosphorus-doped carbonaceous (NPC) substrate. In addition to the other materials, preembedded Pd/Sn metal salt species in NPC control the release of metal sources upon reduction in the liquid phase, resulting in the grafting of an as-prepared PdSn alloy with many merits, such as efficient electron conduction, short-range crystallinity and increased crystal interface exposure. The presence of a considerable quantity of oxygen atoms at the interface of small-sized PdSn alloys on NPC substrates has been methodically verified by powder X-ray diffraction, high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. The PdSn-O sample exhibited excellent ORR activity, achieving an onset potential of ∼0.99 V and a half-wave potential of ∼0.88 V at 1600 rpm in O -saturated 1.0 M KOH. Density functional theory simulations of pure Pd, Pd-O, the PdSn alloy and PdSn-O suggest that interfacial oxygen atom modification is responsible for the significantly improved ORR activity. The assembled zinc-air battery provides a high specific power of 218.9 mW cm and a specific capacity of 810.6 mAh g . Our approach has the potential to stimulate the preparation of O-rich crystalline interfacial-exposed alloy compounds for other energy conversion applications.
ISSN:0021-9797
1095-7103
DOI:10.1016/j.jcis.2023.12.168