School of Environment and Energy, South China University of Technology, Guangzhou 510006, PR China.
School of Environment and Energy, South China University of Technology, Guangzhou 510006, PR China; Guangdong Provincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency Disposal, Guangzhou 510006, PR China; The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006, PR China.
Sci Total Environ. 2022 Oct 10;842:156836. doi: 10.1016/j.scitotenv.2022.156836. Epub 2022 Jun 21.
The development of efficacious photocatalysts for removal of heavy metal and dyes coexisting pollutants simultaneously remains a challenge. Herein, we designed a three-layered Pd@MIL-101/P25 composite photocatalyst, which had the characteristics of directional photogenerated carrier separation. Pd nanoparticles were encapsulated in the MIL-101 to enrich the e, while P25 was loaded on the outer surface of MIL-101 as the valence band of the heterojunction with MIL-101 to enrich the h. The photocatalytic kinetic constants (K) of Pd@MIL-101/P25 for the removal of Cr (VI) and RhB were 3.4 and 4.2 times greater than that of MIL-101, respectively. The photocatalytic efficiency of the catalyst in the mixed pollutants of Cr(VI) and RhB was much higher than that when Cr(VI) and RhB were present separately. Due to the 1.2 and 1.6 nm windows of MIL-101, two target pollutants can be directionally separated. Cr (VI) was reduced by e on the inner surface, and RhB was blocked on the outer surface and oxidized by h. These results suggested that the directional spatially separation of target pollutants are able to separate the reaction sites of oxidation and reduction, improving the utilization efficiency of photogenerated carriers. This work not only provided a new strategy for the design and construction of photocatalytic materials, but also provided a new idea for the treatment of mixed pollutants.
开发同时去除重金属和染料共存污染物的有效光催化剂仍然是一个挑战。在此,我们设计了一种具有定向光生载流子分离特性的三层 Pd@MIL-101/P25 复合光催化剂。钯纳米颗粒被包裹在 MIL-101 中以富集 e,而 P25 则负载在 MIL-101 的外表面上,作为与 MIL-101 的价带异质结的 h 进行富集。Pd@MIL-101/P25 对 Cr(VI)和 RhB 的去除的光催化动力学常数(K)分别比 MIL-101 高 3.4 倍和 4.2 倍。催化剂在 Cr(VI)和 RhB 混合污染物中的光催化效率远高于 Cr(VI)和 RhB 单独存在时的效率。由于 MIL-101 的 1.2 和 1.6nm 窗口,两种目标污染物可以定向分离。Cr(VI)在内表面被 e 还原,而 RhB 在外表面被阻挡并被 h 氧化。这些结果表明,目标污染物的定向空间分离能够分离氧化和还原的反应位点,提高光生载流子的利用效率。这项工作不仅为光催化材料的设计和构建提供了新策略,也为混合污染物的处理提供了新的思路。