铜基和锡基中熵合金氧化物制氢与废聚对苯二甲酸乙二醇酯（PET）升级回收的比较

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science Pub Date : 2025-05-28 DOI:10.1016/j.jcis.2025.138018

Xinjie Xie , Shilong Zhou , Chunyong Zhang , Shuang Dong , Zhou Yang

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引用次数: 0

摘要

电催化水裂解制氢是解决全球能源危机的一种很有前途的方法。废弃PET（聚对苯二甲酸乙二醇酯）的高价值回收利用为解决塑料造成的“白色污染”提供了一种环保的解决方案。如何把这两个反应联系起来？值得注意的是，在PET水解液中，析氢反应（HER）发生在阴极，乙二醇氧化反应（EGOR）发生在阳极，分别产生氢和甲酸（FA）。电催化剂的设计是关键。在此，我们合成并评价了三种铜（Cu）和锡（Sn）基中熵合金氧化物（MEAOs）： Cu0.5Co0.5SnO3.17, Cu0.5Ga0.5SnO3.25和Cu0.5Ni0.5SnO3。Cu0.5Co0.5SnO3.17的电化学性能最好，在10 mA cm−2下的HER过电位为181 mV，电池电压低至1.26 V。其电化学性能优于商用RuO2 + Pt/C体系。此外，Cu0.5Co0.5SnO3.17有效地将EG转化为FA，在1.6 V下达到97.7%的法拉第效率（FE），略高于Cu0.5Ni0.5SnO3和Cu0.5Ga0.5SnO3.25 MEAOs的性能。密度泛函理论（DFT）表明，Cu0.5Co0.5SnO3.17具有一个更接近费米能级的d波段中心，而Co 3d轨道对态密度（DOS）的贡献最大，在Cu0.5Co0.5SnO3.17中反映出更强的协同效应。

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Comparing copper and tin-based medium-entropy alloy oxide for producing hydrogen linking to waste polyethylene terephthalate (PET) upcycling

Electrocatalytic water splitting for hydrogen production presents a promising solution to the global energy crisis. The high-value recycling and utilization of waste polyethylene terephthalate (PET) presents an environmental-friendly solution to address the “white pollution” caused by plastics. How to link the two reactions? Significantly, in a PET hydrolysate solution, the hydrogen evolution reaction (HER) occurs at the cathode, while the ethylene glycol oxidative reaction (EGOR) occurs at the anode, producing hydrogen and formic acid (FA), respectively. The design of electrocatalyst is the key point. Herein, we synthesised and evaluated three copper (Cu) and tin (Sn)-based medium-entropy alloy oxides (MEAOs): Cu_0.5Co_0.5SnO_3.17, Cu_0.5Ga_0.5SnO_3.25 and Cu_0.5Ni_0.5SnO₃. Cu_0.5Co_0.5SnO_3.17 showed the most favourable electrochemical performance, with an HER overpotential of 181 mV at 10 mA cm⁻² and a low cell voltage of 1.26 V. Its electrochemical performance was better than that of the commercial RuO₂ + Pt/C system. Besides, Cu_0.5Co_0.5SnO_3.17 efficiently converts EG to FA, achieving a Faradaic efficiency (FE) of 97.7 % at 1.6 V, slightly surpassing the performances of Cu_0.5Ni_0.5SnO₃ and Cu_0.5Ga_0.5SnO_3.25 MEAOs. Density functional theory (DFT) reveals that the Cu_0.5Co_0.5SnO_3.17 possesses a d-band center that is closer to the Fermi level, and the Co 3d orbit has the most contribution to the density of state (DOS), reflecting more synergetic effect in the Cu_0.5Co_0.5SnO_3.17.

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来源期刊

Journal of Colloid and Interface Science 化学-物理化学

CiteScore

16.10

自引率

7.10%

发文量

2568

审稿时长

2 months

期刊介绍： The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies