Department of Chemistry and Biochemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
International Institute for Carbon-Neutral Energy Research (WPI Academy I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
J Am Chem Soc. 2023 Mar 1;145(8):4384-4388. doi: 10.1021/jacs.2c13149. Epub 2023 Feb 16.
Hydrogen peroxide is an environmentally friendly oxidizing agent but current synthetic methods are wasteful. This is a result of the high flammability of H/O mixtures and/or the requirement for cocatalysts. In this paper, we report the synthesis of HO by means of a homogeneous catalyst, which allows a safe, one-pot synthesis in water, using only H and O. This catalyst is capable of removing electrons from H, storing them for the reduction of O, and then permitting the protonation of the reduced oxygen to HO. The turnover number (TON) is 910 under an H/O (95/5) atmosphere (1.9 MPa) for 12 h at 23 °C, which is the highest of any homogeneous catalyst. Furthermore, we propose a reaction mechanism based on two crystal structures.
过氧化氢是一种环保的氧化剂，但目前的合成方法很浪费。这是由于 H/O 混合物的高可燃性和/或需要共催化剂造成的。在本文中，我们报告了通过均相催化剂合成 HO 的方法，该方法允许在水中进行安全的一锅合成，仅使用 H 和 O。该催化剂能够从 H 中去除电子，将其储存起来用于还原 O，然后允许还原氧质子化为 HO。在 H/O（95/5）气氛（1.9 MPa）下，在 23°C 下反应 12 小时，TON 为 910，这是任何均相催化剂中最高的。此外，我们基于两个晶体结构提出了一种反应机制。
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