Efficient and selective H_(2)O_(2)production through uranyl-assisted photocatalytic oxygen reduction reaction process in a uranium-organic framework  

作　　者：Jianxin Song Chao Liang Baoyu Li Xuemin Wang Min Lei Lisha Jiang Zhenyu Li Yugang Zhang Jian Xie Zuju Ma Xing Dai Yanlong Wang Shuao Wang Wei Liu 

机构地区：[1]School of Environmental and Materials Engineering,Yantai University,Yantai 264005,China [2]State Key Laboratory of Radiation Medicine and Protection,School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions,Soochow University,Suzhou 215123,China [3]School of Life and Environmental Sciences,Shaoxing University,Shaoxing 312000,China [4]School of Nuclear Science and Technology,Xi’an Jiaotong University,Xi’an 710049,China

出　　处：《Science China Chemistry》2024年第7期2274-2281,共8页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(22176163,22106117,52200204);the Natural Science Foundation of Shandong Province(ZR2020QB147,ZR2022QE032);the Young Taishan Scholars Program(tsqn201909082);the Interdisciplinary Basic Frontier Innovation Program of Suzhou Medical College of Soochow University(YXY2304031)。

摘　　要：Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy issues.It is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing H_(2)O_(2)production.Herein,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)production.The material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge carriers.Benefiting from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for H_(2)O_(2)production with yield efficiency of 221μmol h^(-1)g^(-1).Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)measurement.DFTcalculations were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)production.This research introduces an innovative approach to photo-driven H_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.

关 键 词：URANYL metal-organic frameworks oxygen reduction reaction photocatalytic H_(2)O_(2)synthesis 

分 类 号：TQ123.6[化学工程—无机化工] O643.36[理学—物理化学] O644.1[理学—化学]