Oxygen vacancies endow atomic cobalt-palladium oxide clusters with outstanding oxygen reduction reaction activity

Thomas Yang, Dinesh Bhalothia, Hong Wei Chang, Che Yan, Amisha Beniwal, You Xun Chang, Shun Chi Wu, Po Chun Chen, Kuan Wen Wang, Sheng Dai, Tsan Yao Chen

研究成果: 雜誌貢獻期刊論文同行評審

2 引文 斯高帕斯(Scopus)

摘要

Considering the technological importance of fuel cells, developing highly efficacious, durable, and Platinum (Pt)-free catalysts are crucial. In this work, we propose a novel nanocatalyst (NC) comprising oxygen vacancies (OV) enriched atomic CoPdOx clusters (CoPdOxV) anchored Pd nanoparticles (NP)s on cobalt-oxide support (denoted as CPCo). As-prepared CPCo NC with an additional 3 wt% of Co decoration (denoted as CPCo-3) delivers an exceptionally high mass activity (MA) of 4394 mAmgCo−1 at 0.85 V vs RHE and 426 mAmgCo−1 at 0.90 V vs RHE in alkaline oxygen reduction reaction (ORR) (0.1 M KOH), which surpasses the commercial J.M.-Pt/C (20 wt%) catalyst by 65-times. More importantly, the CPCo-3 NC exhibits outstanding durability in an accelerated durability test (ADT) with a progressively increased MA by 40 % (6,140 mAmgCo−1) as that of the initial condition after 20 k cycles. Through in-depth physical characterization, electrochemical analysis, and in-situ X-ray absorption spectroscopy (XAS), we demonstrated the conceptual framework of potential synergism between the CoPdOxV and neighbouring metallic Pd-sites. In this event, the surface-anchored CoPdOxV species coupling with OV promotes the O2 splitting, while the neighbouring Pd-sites simultaneously trigger the Oads relocation (i.e. OH desorption) step. In addition, the cobalt oxide support underneath assists the electron injection to surface Pd-sites. This work not only marks a step ahead for designing high-performance transition metal oxide catalysts for fuel cells but also uncovers the material's aspects of cobalt that shall spark motivation for the other catalytic applications.

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文章編號140289
期刊Chemical Engineering Journal
454
DOIs
出版狀態已出版 - 15 2月 2023

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