Differentiated adsorption of intermediates on high-entropy intermetallic metallene promotes selective electrocatalytic upgrading of PET plastics to glycolic acid

IF 7.7 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Science China Materials Pub Date : 2026-07-24 DOI:10.1007/s40843-026-4159-y

Jiabing Geng (, ), Jiabao Yu (, ), Ruidong Yang (, ), Hongjie Yu (, ), You Xu (, ), Shibin Yin (, ), Kai Deng (, ), Ziqiang Wang (, ), Liang Wang (, )

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Abstract

The electrocatalytic oxidation of ethylene glycol (EG) derived from polyethylene terephthalate (PET) waste to valuable glycolic acid (GA) represents an attractive route for waste resource upcycling. However, achieving high selectivity remains challenging due to the difficulty in steering the complex reaction pathway. In this study, PdPtCuInBi high-entropy intermetallic metallene (HEI-PdPtCuInBiene) is reported to precisely control EG oxidation reaction (EGOR) pathway for GA production by constructing multiple active sites at the atomic scale. In PET hydrolysate, it achieves a Faradaic efficiency of 99.87% and a production rate of 1.47 mmol h⁻¹ cm⁻², along with excellent stability. Mechanistic studies reveal that the high-entropy structure induces strong p-d orbital hybridization, which optimizes the electronic structure of active sites, thus weakening the adsorption of key carbonyl intermediates and suppressing C–C bond cleavage. The synergistic electronic effect among Pd, Pt, and Cu further enables differential adsorption of distinct intermediates on diverse active sites, enhancing the selective formation of GA. Techno-economic analysis exhibits high profitability (∼$784.9 t⁻¹ PET) of this route, demonstrating the great potential of high-entropy intermetallic metallene in regulating electrocatalytic upcycling of PET waste and beyond.

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中间体在高熵金属间烯上的差异吸附促进了PET塑料选择性电催化升级为乙醇酸

从聚对苯二甲酸乙二醇酯（PET）废料中提取的乙二醇（EG）电催化氧化制有价值的乙醇酸（GA）是一条有吸引力的废物资源化升级途径。然而，由于难以控制复杂的反应途径，实现高选择性仍然具有挑战性。在本研究中，报道了PdPtCuInBi高熵金属间金属烯（HEI-PdPtCuInBiene）通过在原子尺度上构建多个活性位点来精确控制EG氧化反应（EGOR）生成GA的途径。在PET水解产物中，其法拉第效率为99.87%，产率为1.47 mmol h−1 cm−2，具有良好的稳定性。机理研究表明，高熵结构诱导了强p-d轨道杂化，优化了活性位点的电子结构，从而减弱了关键羰基中间体的吸附，抑制了C-C键的裂解。Pd， Pt和Cu之间的协同电子效应进一步使得不同中间体在不同活性位点上的差异吸附，增强了GA的选择性形成。技术经济分析显示，该路线的高盈利能力（约784.9 t - 1 PET），表明高熵金属间金属烯在调节PET废物的电催化升级回收等方面具有巨大潜力。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.