Hefei National Laboratory for Physical Science at the Microscale, iChEM, Synergetic Innovation Center of Quantum Information and Quantum Physics , University of Science and Technology of China , Hefei , Anhui 230026 , P. R. China.
J Am Chem Soc. 2018 Mar 7;140(9):3474-3480. doi: 10.1021/jacs.8b00719. Epub 2018 Feb 21.
Recently low-dimensional materials hold great potential in the field of photocatalysis, whereas the concomitantly promoted many-body effects have long been ignored. Such Coulomb interaction-mediated effects would lead to some intriguing, nontrivial band structures, thus promising versatile photocatalytic performances and optimized strategies. Here, we demonstrate that ultrathin black phosphorus (BP) nanosheets exhibit an exotic, excitation-energy-dependent, optical switching effect in photocatalytic reactive oxygen species (ROS) generation. It is, for the first time, observed that singlet oxygen (O) and hydroxyl radical (•OH) are the dominant ROS products under visible- and ultraviolet-light excitations, respectively. Such an effect can be understood as a result of subband structure, where energy-transfer and charge-transfer processes are feasible under excitations in the first and second subband systems, respectively. This work not only establishes an in-depth understanding on the influence of many-body effects on photocatalysis but also paves the way for optimizing catalytic performances via controllable photoexcitation.
最近,低维材料在光催化领域具有很大的潜力,而同时促进的多体效应长期以来一直被忽视。这种库仑相互作用介导的效应会导致一些有趣的、非平凡的能带结构,从而有望实现多功能的光催化性能和优化的策略。在这里,我们证明了超薄黑磷(BP)纳米片在光催化活性氧(ROS)生成中表现出一种奇特的、与激发能有关的光开关效应。这是首次观察到在可见光和紫外光激发下,单线态氧(O)和羟基自由基(•OH)分别是主要的 ROS 产物。这种效应可以理解为子带结构的结果,其中在第一和第二子带系统的激发下,能量转移和电荷转移过程是可行的。这项工作不仅深入了解了多体效应对光催化的影响,也为通过可控光激发优化催化性能铺平了道路。