Integrated electrochemical and chemical system for ampere-level production of terephthalic acid alternatives and hydrogen

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Lin Chen, Chang Yu, Xuedan Song, Junting Dong, Jiawei Mu, Jieshan Qiu
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Abstract

2,5-Furandicarboxylic acid (FDCA), a critical polymer platform molecule that can potentially replace terephthalic acid, coupled hydrogen coproduction holds great prospects via electrolysis. However, the electrosynthesis of FDCA faces challenges in product separation from complex electrolytes and unclear electrochemical and nonelectrochemical reactions during the 5-hydroxymethylfurfural (HMF) oxidation. Herein, an electrochemical/chemical integrated system of alkaline HMF-H2O co-electrolysis is proposed, achieving distillation-free synthesis of high-purity FDCA by acidic separation/purification and hydrogen coproduction. This system achieves ampere-level current densities of 812 and 1290 mA cm−2 at potentials of 1.50 and 1.60 V, with nearly 100% FDCA yield and HMF conversion in only 6 min at 1.50 V. The electrooxidation of HMF involves a coupling of electrochemical and nonelectrochemical reactions, wherein the aldehyde group is dehydrogenated and oxidized, followed by dehydrated and oxidized of the hydroxyl group, ultimately forming FDCA. Concurrently, nonelectrochemical reactions of intermolecular electron transfer occur in HMF and aldehyde group-containing intermediates.

Abstract Image

用于安培级对苯二甲酸替代品和氢气生产的集成电化学和化学系统
2,5-呋喃二甲酸(FDCA)是一种重要的聚合物平台分子,有可能取代对苯二甲酸,通过电解耦合制氢具有广阔的前景。然而,电合成 FDCA 面临着从复杂电解质中分离产物的挑战,以及在 5-hydroxymethylfurfural (HMF) 氧化过程中电化学和非电化学反应不明确的问题。本文提出了一种碱性 HMF-H2O 共电解的电化学/化学集成系统,通过酸性分离/提纯和氢气共生实现了高纯度 FDCA 的免蒸馏合成。该系统在 1.50 和 1.60 V 的电位下可实现 812 和 1290 mA cm-2 的安培级电流密度,在 1.50 V 的电位下仅需 6 分钟即可实现近 100% 的 FDCA 产量和 HMF 转化。HMF 的电氧化涉及电化学反应和非电化学反应的耦合,其中醛基脱氢和氧化,然后羟基脱水和氧化,最终形成 FDCA。同时,在 HMF 和含醛基的中间产物中发生分子间电子转移的非电化学反应。
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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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