Photoelectrochemical Ethylene Glycol Oxidization Coupled with Hydrogen Generation Using Metal Oxide Photoelectrodes

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Fusong Kang, Qingjie Wang, Dongfeng Du, Linxiao Wu, Daniel Wun Fung Cheung, Jingshan Luo
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Abstract

Photoelectrochemical (PEC) water splitting represents a promising approach for harnessing solar energy and transforming it into storable hydrogen. However, the complicated 4-electron transfer process of water oxidation reaction imposes kinetic limitations on the overall efficiency. Herein, we proposed a strategy by substituting water oxidation with the oxidation of ethylene glycol (EG), which is a hydrolysis byproduct of polyethylene terephthalate (PET) plastic waste. To achieve this, we developed and synthesized BiVO4/NiCo-LDH photoanodes capable of achieving a high Faradaic efficiency (FE) exceeding 85 % for the oxidation of EG to formate in a strongly alkaline environment. The reaction mechanism was further elucidated using in situ FTIR spectroscopy. Additionally, we successfully constructed an unassisted PEC device for EG oxidation and hydrogen generation by pairing the translucent Mo : BiVO4/NiCo-LDH photoanode with a state-of-the-art Cu2O photocathode, resulting in an approximate photocurrent density of 2.3 mA/cm2. Our research not only offers a PEC pathway for converting PET plastics into valuable chemicals but also enables simultaneous hydrogen production.

Abstract Image

利用金属氧化物光电电极进行乙二醇氧化与氢气生成的光电化学反应
光电化学(PEC)水分裂是利用太阳能并将其转化为可储存氢气的一种前景广阔的方法。然而,水氧化反应中复杂的 4 电子转移过程对整体效率造成了动力学限制。在此,我们提出了一种用乙二醇(EG)氧化代替水氧化的策略,乙二醇是聚对苯二甲酸乙二醇酯(PET)塑料废弃物的水解副产品。为此,我们开发并合成了 BiVO4/NiCo-LDH 光阳极,在强碱性环境中将 EG 氧化为甲酸酯时,其法拉第效率(FE)可超过 85%。我们还利用原位傅立叶变换红外光谱进一步阐明了反应机理。此外,通过将半透明的 Mo:BiVO4/NiCoLDH 光阳极与最先进的 Cu2O 阴极配对,我们成功地构建了一个用于 EG 氧化和制氢的无辅助 PEC 器件,其光电流密度约为 2.3 mA/cm2。我们的研究不仅为将 PET 塑料转化为有价值的化学品提供了一种 PEC 途径,而且还能同时制氢。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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