Nature Communications ( IF 14.7 ) Pub Date : 2024-03-26 , DOI: 10.1038/s41467-024-47023-y Xiangcheng Zhang 1 , Silian Cheng 1 , Chao Chen 2 , Xue Wen 1 , Jie Miao 1 , Baoxue Zhou 1 , Mingce Long 1 , Lizhi Zhang 1
Hydrogen peroxide photosynthesis suffers from insufficient catalytic activity due to the high energy barrier of hydrogen extraction from H2O. Herein, we report that mechanochemically synthesized keto-form anthraquinone covalent organic framework which is able to directly synthesize H2O2 (4784 μmol h−1 g−1 at λ > 400 nm) from oxygen and alkaline water (pH = 13) in the absence of any sacrificial reagents. The strong alkalinity resulted in the formation of OH-(H2O)n clusters in water, which were adsorbed on keto moieties within the framework and then dissociated into O2 and active hydrogen, because the energy barrier of hydrogen extraction was largely lowered. The produced hydrogen reacted with anthraquinone to generate anthrahydroquinone, which was subsequently oxidized by O2 to produce H2O2. This study ultimately sheds light on the importance of hydrogen extraction from H2O for H2O2 photosynthesis and demonstrates that H2O2 synthesis is achievable under alkaline conditions.
中文翻译:
酮-蒽醌共价有机框架用于 H2O2 与氧气和碱性水的光合作用
由于从H 2 O中提取氢的高能垒,过氧化氢光合作用催化活性不足。在此,我们报道了机械化学合成的酮型蒽醌共价有机骨架,能够直接合成H 2 O 2 (4784 μmol h) −1 g −1 at λ > 400 nm),在没有任何牺牲试剂的情况下,从氧气和碱性水 (pH = 13) 中获得。强碱性导致水中形成OH - (H 2 O) n簇,其被吸附在骨架内的酮部分上,然后解离成O 2和活性氢,因为提氢的能垒大大降低。产生的氢气与蒽醌反应生成蒽氢醌,随后被O 2氧化生成H 2 O 2 。这项研究最终揭示了从H 2 O 中提取氢对于H 2 O 2光合作用的重要性,并证明H 2 O 2合成在碱性条件下是可以实现的。