Yao Wang , Meng Zheng , Yunrui Li , Lidan Zhu , Haoran Li , Qishun Wang , Hui Zhao , Jiawei Zhang , Yuming Dong , Yongfa Zhu
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引用次数: 0
摘要
在乙醇氧化反应过程中，构建所需的长程双位点以增强 C-C 键的清除能力和 CO 的溶解能力对进一步的应用具有重要意义。本文提出了在铂基高指数面（NiOx/Pt）上支撑原子分散的 NiOx 簇的概念，以构建 O 桥接的铂镍双位点。引人注目的是，所获得的 NiOx/Pt 双基点的比活度是商用 Pt/C 的 4.97 倍（0.35 mA cm-2），而且具有出色的一氧化碳耐受性和耐久性。先进的电化学原位表征显示，NiOx/Pt 比 Pt-Ni 双位点更能加速脱羟基和 C-C 键的裂解。理论计算表明，原子分散的氧化镍物种可以降低中间产物的吸附/反应能垒。这种方法为通过设计原子分散氧化物位点来调节表面协同位点提供了一种可行的方法。
Atomically dispersed NiOx cluster on high-index Pt facets boost ethanol electrooxidation through long-range synergistic sites
Constructing the desired long-range dual sites to enhance the C–C bond-cleavage and CO-tolerate ability during ethanol oxidation reaction is of importance for further applications. Herein, the concept of holding atomically dispersed NiOx cluster supported on Pt-based high-index facets (NiOx/Pt) is proposed to build O-bridged Pt–Ni dual sites. Strikingly, the obtained NiOx/Pt dual sites show 4.97 times specific activity higher than that of commercial Pt/C (0.35 mA cm−2), as well as outstanding CO-tolerance and durability. The advanced electrochemical in-situ characterizations reveal that the NiOx/Pt can accelerate rapid dehydroxylation and C–C bond-cleavage over the Pt–Ni dual sites. Theoretical calculations disclose that the atomically dispersed NiOx species can lower the adsorption/reaction energy barriers of intermediates. This tactic provides a promising methodology on regulating the surface synergistic sites via engineering atomically dispersed oxide site.
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