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水热碳化碳基可见光光催化:改性以增强去除有机污染物和对光催化机制的新见解。

Hydrothermal carbonation carbon-based photocatalysis under visible light: Modification for enhanced removal of organic pollutant and novel insight into the photocatalytic mechanism.

机构信息

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.

出版信息

J Hazard Mater. 2022 Mar 15;426:127821. doi: 10.1016/j.jhazmat.2021.127821. Epub 2021 Nov 17.

Abstract

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.

摘要

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。

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