Freese Thomas, Meijer Jelmer T, Brands Maria B, Alachouzos Georgios, Stuart Marc C A, Tarozo Rafael, Gerlach Dominic, Smits Joost, Rudolf Petra, Reek Joost N H, Feringa Ben L
Stratingh Institute for Chemistry, University of Groningen Nijenborgh 4 9747 AG Groningen The Netherlands
van't Hoff Institute for Molecular Sciences, University of Amsterdam Science Park 904 1098 XH Amsterdam The Netherlands.
EES Catal. 2023 Nov 24;2(1):262-275. doi: 10.1039/d3ey00256j. eCollection 2024 Jan 11.
Hydrogen peroxide (HO) is a valuable green oxidant with a wide range of applications. Furthermore, it is recognized as a possible future energy carrier achieving safe operation, storage and transportation. The photochemical production of HO serves as a promising alternative to the waste- and energy-intensive anthraquinone process. Following the 12 principles of Green Chemistry, we demonstrate a facile and general approach to sustainable catalyst development utilizing earth-abundant iron and biobased sources only. We developed several iron oxide (FeO) nanoparticles (NPs) for successful photochemical oxygen reduction to HO under visible light illumination (445 nm). Achieving a selectivity for HO of >99%, the catalyst material could be recycled for up to four consecutive rounds. An apparent quantum yield (AQY) of 0.11% was achieved for the photochemical oxygen reduction to HO with visible light (445 nm) at ambient temperatures and pressures (9.4-14.8 mmol g L). Reaching productivities of HO of at least 1.7 ± 0.3 mmol g L h, production of HO was further possible sunlight irradiation and in seawater. Finally, a detailed mechanism has been proposed on the basis of experimental investigation of the catalyst's properties and computational results.
过氧化氢（HO）是一种具有广泛应用价值的绿色氧化剂。此外，它被认为是未来一种有望实现安全运行、储存和运输的能量载体。HO的光化学制备是一种有前景的替代方法，可替代浪费能源且能耗大的蒽醌法。遵循绿色化学的12条原则，我们展示了一种仅利用储量丰富的铁和生物基来源来开发可持续催化剂的简便通用方法。我们开发了几种氧化铁（FeO）纳米颗粒（NPs），用于在可见光照射（445 nm）下成功将光化学氧还原为HO。该催化剂材料对HO的选择性大于99%，可连续循环使用多达四轮。在环境温度和压力下（9.4 - 14.8 mmol g L），用可见光（445 nm）将光化学氧还原为HO的表观量子产率（AQY）达到0.11%。HO的生产率至少达到1.7 ± 0.3 mmol g L h，在阳光照射和海水中进一步实现了HO的生产。最后，在对催化剂性能进行实验研究和计算结果的基础上，提出了详细的机理。
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