Ying Yang, Xuebo Cao, Lin Huang, Quankun Li, Li Gu, Zheng Yan, Mengli Li, Ruobin Cheng, Zhufeng Lu, Ai-Jun Wang, Wenchao Yang
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引用次数: 0
摘要
在可持续能源的驱动下,将粗乙二醇(EG)电化学氧化为精细化学品,是对报废聚对苯二甲酸乙二醇酯(PET)废料进行再循环利用的一种生态友好型解决方案。本文设计并合成了能够将 EG 混合氧化为甲酸盐(FA)的假 Agx-PtyPdz 核壳电催化剂。该三金属体系由银纳米线和带有孔和凹槽等缺陷的超薄铂钯合金表皮组成。这些缺陷使银核暴露在周围环境中,并在适当的电位(1.2 V vs RHE)下将 Ag0 转化为 Ag2+ 活性物种。因此,在 Agx-PtyPdz 电催化剂上实现了 EG 混合氧化反应,其中 PtPd 表皮由于铂和钯的固有活性,通过传统的法拉第电极过程催化 EG 氧化,而 Ag2+ 作为辅助氧化剂氧化 EG/中间体(非法拉第反应)。这种混合氧化策略加强了 Agx-PtyPdz 电催化剂上吸附剂的清除,并及时刷新了活性位点。最终,该系统实现了超高比活度(24.45 A mg-1PtPd )和长期稳定性(电流密度≥ 400 mA cm-2 时为 3000 h)。Ag2+ 增强醇氧化反应的发现为设计能源和环境应用领域的高性能电催化剂引入了新的范式。
Hybrid Oxidization of Ethylene Glycol on Defective Ag-PtPd Electrocatalyst Beyond 3000 h Stability at an Industrial-Scale Current Density
Electrochemical oxidization of crude ethylene glycol (EG) to fine chemicals driven by sustainable energy is an eco-friendly solution to the upcycling of end-of-life polyethylene terephthalate (PET) wastes. Here, pseudo Agx-PtyPdz core–shell electrocatalyst capable of hybrid oxidation of EG to formate (FA) is designed and synthesized. The trimetallic system consists of Ag nanowire and ultrathin PtPd alloy skin with defects, such as holes and grooves. The defects expose the Ag core to the surroundings and convert Ag0 to Ag2+ active species at appropriate potential (> 1.2 V vs RHE). Thus, hybrid EG oxidization reaction is realized on the Agx-PtyPdz electrocatalyst, where PtPd skin catalyzes EG oxidization through conventional Faradaic electrode process owing to inherent activities of Pt and Pd, while Ag2+ serves as auxiliar oxidant to oxidize EG/intermediates (non-Faradaic reaction). Such a hybrid oxidization strategy reinforces the removal of adsorbates on Agx-PtyPdz electrocatalyst and refresh the active sites timely. Eventually, ultrahigh specific activity (24.45 A mg−1PtPd) and long-term stability (> 3000 h at current density ≥ 400 mA cm−2) are delivered by the system. The finding of Ag2+-enhanced alcohol oxidization reactions introduces a new paradigm for designing high-performance electrocatalysts for energy and environmental applications.
期刊介绍:
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