Sulfur-doped bimetallic phosphides with regulated intermediate adsorption for efficient polyethylene terephthalate upgrading

IF 9.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2025-08-29 DOI:10.1039/D5GC03484A

Xiaofen Huang, Zhiyong Ye, Kaige Yu, Xingchen Zhou, Xianglong Hu, Yixuan Jin, Xueliang Jiang and Huan Yang

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Abstract

Upgrading ethylene glycol (EG) derived from polyethylene terephthalate (PET) waste into valuable formic acid (FA) and H₂ offers a promising solution for plastic pollution. However, high-selectivity oxidation of EG to form FA is limited by the cleavage of the C–C bond with high bond energy during the ethylene glycol oxidation reaction (EGOR) process. To address this challenge, sulfur-doped bimetallic phosphide (NiFeP/FeSP) was designed using a microbial corrosion–phosphidation strategy. The constructed bifunctional NiFeP/FeSP electrocatalyst presents advanced EGOR coupled with hydrogen evolution reaction (HER) performance. The NiFeP/FeSP electrode can enable high-selectivity oxidation of EG to form FA, and requires only 1.38 V @10 mA cm⁻². Experimental and theoretical calculation results reveal that microbial-induced sulfur atom doping regulates the coordination environment of Ni, which can enhance the generation of Ni–O bonds and optimize the adsorption of H* intermediates, lowering the reaction energy barrier. Consequently, NiFeP/FeSP as a bifunctional electrode requires 1.52 V at 10 mA cm⁻² in the HER//EGOR system, which is 110 mV lower than that of the HER//oxygen evolution reaction system. These results suggest that the NiFeP/FeSP catalyst can efficiently convert PET hydrolysis products into high-value chemicals and hydrogen, which is of great significance for the development of sustainable environmental and clean energy technologies.

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调节中间吸附的硫掺杂双金属磷化物用于高效聚对苯二甲酸酯升级

将从聚对苯二甲酸乙二醇酯（PET）废料中提取的乙二醇（EG）转化为有价值的甲酸（FA）和氢气是解决塑料污染的一种有前途的解决方案。然而，乙二醇氧化反应（EGOR）过程中高键能的C-C键断裂限制了EG的高选择性氧化生成FA。为了解决这一挑战，采用微生物腐蚀-磷化策略设计了硫掺杂双金属磷化物（NiFeP/FeSP）。所构建的双功能NiFeP/FeSP电催化剂具有先进的EGOR和析氢反应（HER）性能。NiFeP/FeSP电极可以实现EG的高选择性氧化生成FA，仅需1.38 V @10 mA cm−2。实验和理论计算结果表明，微生物诱导的硫原子掺杂调节了Ni的配位环境，增强了Ni - o键的生成，优化了H*中间体的吸附，降低了反应能垒。因此，NiFeP/FeSP作为双功能电极，在HER//EGOR体系中需要1.52 V，电压为10 mA cm−2，比HER//析氧反应体系低110 mV。这些结果表明，NiFeP/FeSP催化剂可以有效地将PET水解产物转化为高价值化学品和氢气，这对可持续环境和清洁能源技术的发展具有重要意义。

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.