Yeast Inherited Phosphide/Bio-Carbon for Controllable Polyethylene Terephthalate Upcycling

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Tian Xia, Zhengjie Chen, Chungli Dong, Xianglong Hu, Sihan Zhang, Chengchieh Yang, Jinhao Hu, Yuhong Zhang, Xueliang Jiang, Huan Yang, Bao Yu Xia
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Abstract

Electrochemical reforming of polyethylene terephthalate (PET) coupled with hydrogen production is of great significance to realize the sustainable development of clean energy technologies. Nevertheless, precisely controlling the reaction pathways and selectively converting key intermediates during glycol oxidation reaction (EGOR) pose considerable challenges. Herein, theoretical calculations and experiments reveal that the key intermediate (*CHO-CHO) and the role of P in promoting the reconstruction of transition metal phosphides surface during the EGOR process. Consequently, the bio-template strategy is introduced to design bimetal phosphide@bio-carbon pre-catalyst toward efficient EGOR and hydrogen evolution reaction (HER). This design enables controlled *CHO-CHO intermediate formation and transformation through the enhanced adsorption of OH* and *CHO-CHO, leading to a highly selective EGOR. The C1 product of formic acid exhibits superior Faradaic efficiency (99.1%) at 1.35 V. In addition, this constructed catalyst only requires 1.76 V@500 mA cm−2 and can stably perform for more than 240 h at 500 mA cm−2 toward EGOR coupled with HER in the PET hydrolysate. This work proposes a novel strategy to construct superior catalyst for efficient PET upcycling coupled with HER, which is crucial to the sustainable development of multidisciplinary integration with biology and clean energy conversion technologies.

Abstract Image

酵母遗传磷化物/生物炭用于聚对苯二甲酸乙二醇酯的可控升级回收
聚对苯二甲酸乙二醇酯(PET)的电化学重整与制氢耦合对实现清洁能源技术的可持续发展具有重要意义。然而,在乙二醇氧化反应(EGOR)过程中,精确控制反应途径和选择性转化关键中间体是相当大的挑战。本文通过理论计算和实验揭示了关键中间体(*CHO-CHO)和P对EGOR过程中过渡金属磷化物表面重构的促进作用。因此,引入生物模板策略来设计高效EGOR和析氢反应(HER)的双金属phosphide@bio-carbon预催化剂。该设计通过增强OH*和*CHO-CHO的吸附,实现了控制*CHO-CHO中间产物的形成和转化,从而实现了高选择性EGOR。甲酸的C1产物在1.35 V时表现出优异的法拉第效率(99.1%)。此外,该构建的催化剂只需要1.76 V@500 mA cm - 2,并且可以在500 mA cm - 2下稳定地对PET水解产物中的EGOR偶联HER进行240小时以上的反应。本研究提出了构建高效PET升级回收催化剂的新策略,这对生物和清洁能源转化技术的多学科整合的可持续发展至关重要。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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