Biswal Lijarani, Mishra Bhagyashree Priyadarshini, Das Sarmistha, Acharya Lopamudra, Nayak Susanginee, Parida Kulamani
Centre for Nano Science and Nano Technology, Institute of Technical Education and Research, Siksha 'O' Anusandhan University, Bhubaneswar 751030, India.
Inorg Chem. 2023 May 15;62(19):7584-7597. doi: 10.1021/acs.inorgchem.3c01138. Epub 2023 May 1.
Designing of a visible-light-driven semiconductor-based heterojunction with suitable band alignment and well-defined interfacial contact is considered to be an effective strategy for the transformation of solar-to-chemical energy and environmental remediation. In this context, MXenes have received tremendous attention in the research community due to their merits of abundant derivatives, elemental composition, excellent metallic conductivity, and surface termination groups. Meanwhile, a facile synthetic strategy for MXene-derived TiO nanocomposites with stable framework and higher photocatalytic activity under visible-light irradiation still remains a challenge for researchers. Herein, we report a novel synthetic strategy of preparing a two-dimensional TiC@TiO nanohybrid by a facile reflux method under acidic conditions. In this oxidation reaction, protonation of the hydroxyl terminal group of MXene creates Ti more electrophilic and susceptible to an oxidative nucleophilic addition reaction with the presence of both water and oxygen. The physicochemical properties of the nanohybrid TiC@TiO were verified by varieties of characterization techniques. High-resolution transmission electron microscopy and X-ray photoelectron spectroscopy analysis specifically elucidated the intimate interfacial interaction between TiC and TiO. The optimized TiC@TiO-48 h photocatalyst exhibited the highest tetracycline hydrochloride (TCH, 90% in 90 min) degradation efficiency in comparison to pristine TiO with a rate constant () of 0.02463 min. The major contribution of O and OH radicals throughout photocatalytic TCH degradation was confirmed by the trapping experiment. Moreover, the photocatalyst showed the highest hydrogen generation rate of 140.8 μmol h along with an apparent conversion efficiency of 2.2%. The excellent photocatalytic activity of TiC@TiO originated from the superior electrical conductivity of cocatalyst TiC, which facilitated spatial photogenerated e/h separation and transfer at the TiC MXene@TiO interface. Overall, this research work will describe a promising protocol of designing MXene-derived photocatalysts toward efficient environmental remediation and wastewater treatment applications.
设计具有合适能带排列和明确界面接触的可见光驱动半导体基异质结被认为是实现太阳能到化学能转化和环境修复的有效策略。在此背景下,MXenes因其丰富的衍生物、元素组成、优异的金属导电性和表面端基等优点而在研究界受到广泛关注。同时,对于研究人员来说,开发一种简便的合成策略来制备具有稳定框架且在可见光照射下具有更高光催化活性的MXene衍生TiO纳米复合材料仍然是一个挑战。在此,我们报道了一种在酸性条件下通过简便回流法制备二维TiC@TiO纳米杂化物的新型合成策略。在该氧化反应中,MXene羟基端基的质子化使Ti更具亲电性,在水和氧气存在的情况下易发生氧化亲核加成反应。通过各种表征技术验证了纳米杂化物TiC@TiO的物理化学性质。高分辨率透射电子显微镜和X射线光电子能谱分析具体阐明了TiC和TiO之间紧密的界面相互作用。与原始TiO相比,优化后的TiC@TiO-48 h光催化剂表现出最高的盐酸四环素(TCH,90分钟内降解90%)降解效率,速率常数()为0.02463 min。捕获实验证实了O和OH自由基在光催化TCH降解过程中的主要贡献。此外,该光催化剂显示出最高的产氢速率为140.8 μmol h,表观转化效率为2.2%。TiC@TiO优异的光催化活性源于助催化剂TiC的优异导电性,这促进了空间光生电子/空穴在TiC MXene@TiO界面的分离和转移。总体而言,这项研究工作将描述一种有前景的设计MXene衍生光催化剂用于高效环境修复和废水处理应用的方案。