期刊
NANO LETTERS
卷 22, 期 3, 页码 1257-1264出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c04420
关键词
selenide nanocrystals; electrochemical synthesis; ensemble effect; ligand effect; linear scaling relationship
类别
资金
- National Natural Science Foundation of China (NSFC) [22002088]
- National Research Foundation of Korea (NRF) [2015M3D3A1A01064929]
- Shanghai Sailing Program [20YF1420500]
- Oceanic Interdisciplinary Program of Shanghai Jiao Tong University [SL2020MS007]
- KISTI [KSC-2021-CRE-0321]
- China Postdoctoral Science Foundation [2020TQ0189, 2020M681293]
- National Research Foundation of Korea [2015M3D3A1A01064929] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Se-based nanoalloys are a promising class of metal chalcogenides with tunable crystalline and electronic structures, showing great potential in renewable energy conversion and utilization. By controlling the alloying component, a flexible control over the oxygen reduction reaction pathway has been achieved, and an optimized scaling relationship between oxygenated ORR intermediates has been discovered on certain nanocrystals.
Se-based nanoalloys as an emerging class of metal chalcogenide with tunable crystalline structure, component distribution, and electronic structure have attracted considerable interest in renewable energy conversion and utilization. In this Letter, we report a series of nanosized M-Se catalysts (M = Cu, Ni, Co) as prepared from laser ablation method and screen their electrocatalytic performance for onsite H2O2 generation from selective oxygen reduction reaction (ORR) in alkaline media. A flexible control on 2e(-)/4e(-) ORR pathway has been achieved by engineering the alloying component. Moreover, through a feedback loop between theory and experiment an optimized scaling relationship between oxygenated ORR intermediates has been discovered on cubic Cu7.2Se4 nanocrystals, that is, the ensemble effect of isolated Cu component destabilizes O* binding while the ligand effect of Se to Cu fine-tunes the binding strength of OOH*, leading to a superb H2O2 selectivity above 90% over a wide potential window even after 1400 potential cycles.
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