聚合物半导体光催化合成过氧化氢:光氧化还原中心的空间分离和协同利用
Semiconducting Polymers for Photosynthesis of H2O2:Spatial Separation and Synergistic Utilization of Photoredox Centers
摘要
Abstract
The photocatalytic synthesis of hydrogen peroxide using earth-abundant water and/or O2 as raw materials and solar energy as the sole energy input is an attractive route to achieving a carbon-neutral future.In particular,semiconducting polymer photocatalysts have piqued the interest of researchers working on the photocatalytic synthesis of H2O2 because their bandgap structures,reactivation sites,and components are easily tunable at the molecular level.However,there are two major challenges:1)the photoredox centers are difficult to separate and recombine easily,resulting in low reactivity in the photocatalytic production of H2O2,and 2)the low utilization rate of the redox centers.In several cases,only one side of the redox center is used for the photocatalytic synthesis of H2O2,while the other side typically reacts with a sacrificial agent.In this review,we provide a timely survey of recent advances in the spatial separation and synergistic utilization of photoredox centers for photocatalytic H2O2 production.The key aspect for achieving spatial separation of the redox centers is to engineer electron donor-acceptor(D-A)units on a single photocatalyst,such as by incorporating atomically dispersed metals into the polymer frameworks to build metal-organic D-A units or constructing all-organic D-A units.Depending on the photocatalytic behavior of the redox centers,the synergistic utilization of photoredox centers can be classified into three major reaction models:1)the oxygen reduction reaction(ORR)combined with the oxidative production of chemicals;2)the water oxidation reaction(WOR)combined with the reductive production of chemicals;and 3)the ORR combined with the WOR.Based on this,the regulation modes,characteristics,catalytic mechanisms,and reaction pathways to overcome the two challenges of efficient H2O2 production are summarized and discussed.Finally,we demonstrate efficient photocatalytic H2O2 production and provide prospects and challenges for the photocatalytic production of H2O2 using photoredox centers.关键词
过氧化氢合成/氧化还原中心/空间分离/协同利用/聚合物光催化剂Key words
H2O2 synthesis/Photo-redox center/Spatial separation/Synergistic utilization/Polymer photocatalyst分类
化学引用本文复制引用
谢垚,张启涛,孙宏丽,滕镇远,苏陈良..聚合物半导体光催化合成过氧化氢:光氧化还原中心的空间分离和协同利用[J].物理化学学报,2023,39(11):59-80,22.基金项目
国家自然科学基金(21972094,21805191,22102102),国家重点研发计划(2021YFA1600800),广东省教育厅基金(839-0000013131),广东基础和应用基础研究基金(2020A1515010982),深圳科技计划(JCYJ2019080808142001745,RCJC2020200714114434086),深圳稳定支持项目(20200812160737002,20200812122947002),深圳孔雀计划(20180921273B,202108022524B,20210308299C)资助 The project was supported by the National Natural Science Foundation of China(21972094,21805191,22102102),National Key Research and Development Program of China(2021YFA1600800),Educational Commission of Guangdong Province,China(839-0000013131),Guangdong Basic and Applied Basic Research Foundation,China(2020A1515010982),Shenzhen Science and Technology Program,China(JCYJ20190808142001745,RCJC20200714114434086),Shenzhen Stable Support Project,China(20200812160737002,20200812122947002),Shenzhen Peacock Plan,China(20180921273B,202108022524B,20210308299C). （21972094,21805191,22102102）
