Pulsed electrosynthesis of glycolic acid through polyethylene terephthalate upcycling over a mesoporous PdCu catalyst

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Shu Han, Lizhi Sun, Dongping Fan, Ben Liu
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Abstract

Electrocatalytic upcycling of polyethylene terephthalate (PET) plastics offers a promising and sustainable route that not only addresses serious waste pollution but also produces high value-added chemicals. Despite some important achievements, their activity and selectivity have been slower than needed. In this work, pulsed electrocatalysis is employed to engineer chemisorption properties on a lamellar mesoporous PdCu (LM-PdCu) catalyst, which delivers high activity and stability for selective electrosynthesis of high value-added glycolic acid (GA) from PET upcycling under ambient conditions. LM-PdCu is synthesized by in situ nucleation and attachment strategy along assembled lamellar templates, whose stacked morphology and lamellar mesoporous structure kinetically accelerate selective desorption of GA and expose fresh active sites of metal catalysts for continuous electrocatalysis at pulsed mode. This strategy thus delivers GA Faraday efficiency of >92% in wide potential windows, yield rate of reaching 0.475 mmol cm–2 h–1, and cycling stability of exceeding 20 cycles for electrocatalytic PET upcycling. Moreover, pulsed electrocatalysis discloses good electrocatalytic performance for scaled-up GA electrosynthesis from real bottle waste plastics. This work presents a sustainable route for selective electrosynthesis of value-added chemicals through upcycling of various waste feedstocks.

Abstract Image

聚对苯二甲酸乙二醇酯(PET)塑料的电催化升级再循环提供了一条前景广阔的可持续发展途径,不仅能解决严重的废物污染问题,还能生产高附加值的化学品。尽管取得了一些重要成果,但其活性和选择性仍低于需要。在这项研究中,利用脉冲电催化技术在片状介孔钯铜催化剂(LM-PdCu)上设计了化学吸附特性,该催化剂具有高活性和高稳定性,可在环境条件下从 PET 上循环中选择性地电合成高附加值的乙醇酸(GA)。LM-PdCu 是通过原位成核和附着策略沿着组装好的片状模板合成的,其堆叠形态和片状介孔结构可加速 GA 的选择性解吸,并暴露出金属催化剂的新活性位点,从而在脉冲模式下进行连续电催化。因此,在宽电位窗口中,这种策略可使 GA 的法拉第效率达到 92%,产率达到 0.475 mmol cm-2 h-1,循环稳定性超过 20 次,可用于电催化 PET 的上循环。此外,脉冲电催化技术还具有良好的电催化性能,可用于从真正的瓶子废塑料中扩大 GA 的电合成规模。这项工作提出了一条可持续的路线,通过对各种废原料进行升级再循环,选择性地电合成高附加值化学品。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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