Boosted production of formate via paired electro-reforming of poly (ethylene terephthalate) plastic and CO2 reduction

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Jianghui Qiu, Zhixin Jing, Dongping Zhan, Juan Peng
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Abstract

Electrocatalytic upcycling of polyethylene terephthalate (PET)-derived ethylene glycol into high-value formate enables dual environmental and economic benefits. Here, we developed a SnO2/NF electrode that achieved exceptional formate production via PET upcycling, delivering 99.8% Faraday efficiency and a superior production rate of 3.24 mmol cm−2 h−1. Mechanistic studies revealed that the ethylene glycol oxidation reaction on SnO2/NF followed an electrochemical-chemical cascade pathway, NiOOH served as the active site, while SnO2 functioned as an “electron transfer layer” and a catalytic modulator. The oxygen-affinity sites of SnO2 effectively suppressed the competing activity of oxygen evolution reaction and concurrently shifted the d-band center of the active Ni center toward the Fermi level. This electronic structure modulation facilitated the adsorption and conversion of aldehyde intermediates, thereby significantly enhancing the selectivity for formate production. In a paired electrolysis system (POR||CO2RR), the electrode achieved an apparent Faraday efficiency of 182% for formate at a cell voltage of 2.9 V. This study provides novel insights for designing low-cost and high-performance electrocatalysts for the value-added conversion of waste PET plastics.

Abstract Image

通过对聚对苯二甲酸乙酯塑料的电重整和二氧化碳的减少,提高了甲酸酯的产量
电催化升级回收聚对苯二甲酸乙二醇酯(PET)衍生的高价值甲酸乙二醇具有双重环境和经济效益。在这里,我们开发了一种SnO2/NF电极,通过PET升级回收实现了优异的甲酸生产,法拉第效率达到99.8%,产率达到3.24 mmol cm−2 h−1。机理研究表明,SnO2/NF上的乙二醇氧化反应遵循电化学-化学级联反应途径,NiOOH作为活性位点,SnO2作为“电子传递层”和催化调节剂。SnO2的亲氧位点有效地抑制了析氧反应的竞争活性,同时使活性Ni中心的d带中心向费米能级移动。这种电子结构调制促进了醛中间体的吸附和转化,从而显著提高了甲酸酯生产的选择性。在配对电解系统(POR||CO2RR)中,电极在2.9 V的电池电压下获得了182%的显法拉第效率。本研究为设计低成本、高性能的PET废塑料增值转化电催化剂提供了新的思路。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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