英国利物浦大学Andrew I. Cooper报道了太阳能驱动过氧化氢生产所用线性共轭聚合物催化剂稳定性的重要性。相关研究成果于2021年11月10日发表于国际顶尖学术期刊《美国化学会杂志》。

过氧化氢（H₂O₂）是最重要的工业氧化剂之一。原则上，利用阳光从氧气和H₂O光催化合成H₂O₂可以为当前的蒽醌工艺提供一种更清洁的替代路线。近年来，共轭有机材料作为太阳能燃料合成的光催化剂被研究，因为它们在大的化学空间内提供合成可调性。

该文中，研究人员利用高通量实验发现了一种线性共轭聚合物，聚（3-4-乙炔基苯基）乙炔基）吡啶（DE7），其在可见光照明下将H₂O和O₂高效光催化生成H₂O₂，时间长达10小时左右。在420nm处，表观量子产率为8.7%。机理研究表明，H₂O₂是通过光诱导的氧气逐步还原产生的。然而，在较长的光解时间内，该催化剂会分解，表明需要关注有机光催化剂的光稳定性以及初始催化产率。

附：英文原文

Title: Linear Conjugated Polymers for Solar-Driven Hydrogen Peroxide Production: The Importance of Catalyst Stability

Author: Lunjie Liu, Mei-Yan Gao, Haofan Yang, Xiaoyan Wang, Xiaobo Li, Andrew I. Cooper

Issue&Volume: November 10, 2021

Abstract: Hydrogen peroxide (H2O2) is one of the most important industrial oxidants. In principle, photocatalytic H2O2 synthesis from oxygen and H2O using sunlight could provide a cleaner alternative route to the current anthraquinone process. Recently, conjugated organic materials have been studied as photocatalysts for solar fuels synthesis because they offer synthetic tunability over a large chemical space. Here, we used high-throughput experiments to discover a linear conjugated polymer, poly(3-4-ethynylphenyl)ethynyl)pyridine (DE7), which exhibits efficient photocatalytic H2O2 production from H2O and O2 under visible light illumination for periods of up to 10 h or so. The apparent quantum yield was 8.7% at 420 nm. Mechanistic investigations showed that the H2O2 was produced via the photoinduced stepwise reduction of O2. At longer photolysis times, however, this catalyst decomposed, suggesting a need to focus the photostability of organic photocatalysts, as well as the initial catalytic production rates.

DOI: 10.1021/jacs.1c09979

Source: https://pubs.acs.org/doi/10.1021/jacs.1c09979