School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China; Instrumental Analysis Center of Zhejiang Gongshang University, Hangzhou 310018, China.
School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China.
J Hazard Mater. 2023 Jun 5;451:131149. doi: 10.1016/j.jhazmat.2023.131149. Epub 2023 Mar 7.
Selectively regulating active factors in photocatalytic reactions by designing materials is one of the very important factors. Herein, we prepared spindle-like core-shell Ag@NH-MIL-88B composites (Ag@NM-88) by a two-step hydrothermal method. The as-prepared Ag@NM-88 displayed superior photocatalytic activity for Cr(VI) reduction under LED light, compared with the activities of pure NH-MIL-88B (NM-88) and Ag/NM-88 (Ag was deposited on NH-MIL-88B). The core-shell structure Ag@NM-88 was not only beneficial to the absorption of light but also beneficial to the separation of photogenerated e and h. More importantly, it was further confirmed by active radical capture experiments and nitroblue tetrazolium (NBT) conversion experiments that the design of the core-shell structure could effectively prevent photogenerated e from combing with O to form •O, so that photogenerated e directly reduced Cr(VI), thereby improving the reaction rate. In addition, it could still maintain good stability after 5 cycles, indicating that the construction of a core-shell structure is also conducive to improving stability. This work provides a strategy for selectively regulating the active components of photocatalysts, and provides new insights into the relationship between interfacial charge transfer and molecular oxygen activation in photocatalytic reduction Cr(VI) systems.
通过设计材料选择性调节光催化反应中的活性因素是非常重要的因素之一。在此,我们通过两步水热法制备了纺锤状核壳 Ag@NH-MIL-88B 复合材料(Ag@NM-88)。与纯 NH-MIL-88B(NM-88)和 Ag/NM-88(Ag 沉积在 NH-MIL-88B 上)相比,所制备的 Ag@NM-88 在 LED 光下对 Cr(VI)还原具有优异的光催化活性。核壳结构 Ag@NM-88 不仅有利于光的吸收,而且有利于光生电子和空穴的分离。更重要的是,通过活性自由基捕获实验和硝基蓝四唑(NBT)转化实验进一步证实,核壳结构的设计可以有效地防止光生电子与 O 结合形成•O,从而使光生电子直接还原 Cr(VI),从而提高反应速率。此外,它在 5 个循环后仍能保持良好的稳定性,表明构建核壳结构也有利于提高稳定性。这项工作为选择性调节光催化剂的活性成分提供了一种策略,并为光催化还原 Cr(VI)体系中界面电荷转移与分子氧活化之间的关系提供了新的见解。