Kang Fusong, Wang Qingjie, Du Dongfeng, Wu Linxiao, Cheung Daniel Wun Fung, Luo Jingshan
Institute of Photoelectronic Thin Film Devices and Technology, State Key Laboratory of Photovoltaic Materials and Cells, Key Laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin, Ministry of Education Engineering Research Center of Thin Film Photoelectronic Technology, Nankai University, Tianjin, 300350, China.
Frontiers Science Center for New Organic Matter, Nankai University, Tianjin, 300071, China.
Angew Chem Int Ed Engl. 2025 Jan 27;64(5):e202417648. doi: 10.1002/anie.202417648. Epub 2024 Nov 13.
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 BiVO/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 : BiVO/NiCo-LDH photoanode with a state-of-the-art CuO photocathode, resulting in an approximate photocurrent density of 2.3 mA/cm. Our research not only offers a PEC pathway for converting PET plastics into valuable chemicals but also enables simultaneous hydrogen production.
光电化学（PEC）水分解是一种利用太阳能并将其转化为可储存氢气的很有前景的方法。然而，水氧化反应复杂的4电子转移过程对整体效率造成了动力学限制。在此，我们提出了一种策略，用乙二醇（EG）氧化替代水氧化，EG是聚对苯二甲酸乙二酯（PET）塑料废料的水解副产物。为实现这一目标，我们开发并合成了BiVO/NiCo-LDH光阳极，在强碱性环境中，该光阳极对EG氧化生成甲酸盐的法拉第效率（FE）能超过85%。利用原位傅里叶变换红外光谱进一步阐明了反应机理。此外，我们通过将半透明的Mo : BiVO/NiCo-LDH光阳极与先进的CuO光阴极配对，成功构建了用于EG氧化和制氢的无辅助PEC装置，产生了约2.3 mA/cm的光电流密度。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条PEC途径，还能同时制氢。
