南开大学罗京山团队报道了利用金属氧化物光电极进行乙二醇氧化耦合制氢的光电化学研究。相关研究成果于2024年10月7日发表于国际一流学术期刊《德国应用化学》。

光电化学（PEC）水分解代表了一种利用太阳能并将其转化为可储存氢气的有前景的方法。然而，水氧化反应复杂的4-电子转移过程对整体效率施加了动力学限制。

该文中，研究人员提出了一种用乙二醇（EG）的氧化代替水氧化的策略，其中乙二醇是聚对苯二甲酸乙二醇酯（PET）塑料废物的水解副产物。为了实现这一目标，研究人员开发并合成了BiVO₄/NiCo-LDH光阳极，该阳极能够在强碱性环境中将EG氧化为甲酸盐，实现超过85%的高法拉第效率（FE）。

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，通过将半透明的Mo:BiVO4/NiCo-LDH光阳极与最先进的Cu₂O光电阴极配对，成功构建了一个用于EG氧化和氢气产生的无辅助PEC装置，其光电流密度约为2.3 mA/cm²。

该研究不仅为将PET塑料转化为有价值的化学品提供了PEC途径，而且能够同时生产氢气。

附：英文原文

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

Author: Fusong Kang, Qingjie Wang, Dongfeng Du, Linxiao Wu, Daniel Wun Fung Cheung, Jingshan Luo

Issue&Volume: 2024-10-07

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.

DOI: 10.1002/anie.202417648

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202417648