School of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China.
School of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China.
J Hazard Mater. 2022 Mar 15;426:127821. doi: 10.1016/j.jhazmat.2021.127821. Epub 2021 Nov 17.
Hydrothermal carbonation carbon (HTCC) is emerging as a promising alternative for photocatalytic removal of contaminants from water. However, the catalytic activity of HTCC is limited by its poor charge transfer ability, and its photocatalytic mechanism remains unclear. Herein, a unique photosensitization-like mechanism was firstly found on Fe modified HTCC (Fe-HTCC) derived from glucose for effective removal of organic pollutants. Under visible light illumination, the organic pollutant coordinated with Fe-HTCC enabled electrons transfer from its highest occupied molecular orbital (HOMO) to conduction band (CB) of Fe-HTCC, which not only oxidized pollutant itself, but also generated oxygen-centered radical for reducing O into O towards pollutant removal. The degradation kinetic constant of sulfamethoxazole (SMX) over Fe-HTCC was about 1024.4 and 20.5 times higher than that of HTCC and g-CN, respectively. The enhanced performance of Fe-HTCC was originated from dual role of Fe modification: one is to boost the electron-deficient C sites which prefer to coordinate with amino or hydroxyl of pollutants; the other is to enhance the linkage of discrete polyfuran chains in Fe-HTCC for effective electron transfer from pollutant to Fe-HTCC. This work provides new insight into the synthesis and mechanism of HTCC-based high-efficiency photocatalyst for water decontamination.
水热碳化碳(HTCC)作为一种很有前途的替代技术,正在被用于从水中光催化去除污染物。然而,HTCC 的催化活性受到其电荷转移能力差的限制,其光催化机制仍不清楚。本文首次在来源于葡萄糖的 Fe 改性 HTCC(Fe-HTCC)上发现了一种独特的类光敏化机制,用于有效去除有机污染物。在可见光照射下,与 Fe-HTCC 配位的有机污染物使电子从其最高占据分子轨道(HOMO)转移到 Fe-HTCC 的导带(CB),这不仅可以氧化污染物本身,还可以生成氧中心自由基,将 O 还原为 O,从而去除污染物。Fe-HTCC 对磺胺甲恶唑(SMX)的降解动力学常数约为 HTCC 和 g-CN 的 1024.4 和 20.5 倍。Fe-HTCC 性能的增强源于 Fe 改性的双重作用:一方面是增强电子缺 C 位,这些 C 位更容易与污染物的氨基或羟基配位;另一方面是增强离散多呋喃链在 Fe-HTCC 中的连接,以有效地将电子从污染物转移到 Fe-HTCC。这项工作为基于 HTCC 的高效光催化剂用于水净化的合成和机制提供了新的见解。