Ke Tao, Shen Shuyi, Rajavel Krishnamoorthy, Yang Kun, Lin Daohui
Department of Environmental Science, Zhejiang University, Hangzhou 310058, China.
Department of Environmental Science, Zhejiang University, Hangzhou 310058, China; Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, Zhejiang University, Hangzhou 310058, China.
J Hazard Mater. 2021 Jan 15;402:124066. doi: 10.1016/j.jhazmat.2020.124066. Epub 2020 Sep 22.
Construction of heterojunction and nitrogen doping is an effective approach for synthesizing photocatalysts with high quantum yield and efficient electron-hole separation. 2D MXene TiC has been considered a good carbonaceous nanomaterial for designing heterojunction, while the original surface groups and stacked structure limit the electron-hole separation. Herein, a hybrid of nitrogen-doped TiC nanosheets and TiO nanoparticles (NPs) composed of TiO NPs in situ growing on isopropyl amine (iPA) modified TiC (iN-TiC) was developed for the first time. The novel iN-TiC/TiO hybrid exhibited an excellent ultraviolet-light photodegradation of methylene blue (MB), with a degradation rate (0.02642 min) significantly higher than that of pure TiO NPs, bulk-TiC/TiO, dimethyl sulfoxide modified TiC/TiO hybrid, and hydrazine monohydrate modified TiC/TiO hybrid. The formation of heterojunction between iN-TiC and TiO and its role in the photocatalysis were systematically analyzed using various characterization techniques and density functional theory calculation. The iPA modification exfoliated TiC and doped N on TiC nanosheets; the in situ grown TiO NPs formed efficient heterojunctions with the nanosheets; the N-doping facilitated electron migration in TiC and inhibited the recombination of photogenerated electron-hole pairs; •OH dominated the photodegradation of MB. This work provides a new approach of constructing efficient photocatalysts for the treatment of organics-polluted water.
构建异质结和氮掺杂是合成具有高量子产率和高效电子 - 空穴分离的光催化剂的有效方法。二维MXene TiC被认为是一种用于设计异质结的良好碳质纳米材料,但其原始表面基团和堆叠结构限制了电子 - 空穴分离。在此,首次开发了一种由异丙胺(iPA)修饰的TiC(iN - TiC)上原位生长的TiO纳米颗粒(NPs)组成的氮掺杂TiC纳米片与TiO纳米颗粒(NPs)的杂化物。新型iN - TiC/TiO杂化物对亚甲基蓝(MB)表现出优异的紫外光光降解性能,降解速率(0.02642 min⁻¹)显著高于纯TiO NPs、块状TiC/TiO、二甲基亚砜修饰的TiC/TiO杂化物和水合肼修饰的TiC/TiO杂化物。利用各种表征技术和密度泛函理论计算系统地分析了iN - TiC与TiO之间异质结的形成及其在光催化中的作用。iPA修饰使TiC剥离并在TiC纳米片上掺杂N;原位生长的TiO NPs与纳米片形成了有效的异质结;N掺杂促进了TiC中的电子迁移并抑制了光生电子 - 空穴对的复合;•OH主导了MB的光降解。这项工作为构建用于处理有机污染水的高效光催化剂提供了一种新方法。