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非金属掺杂纳米二氧化钛修饰的还原氧化石墨烯的制备:一种高效的可见光驱动光催化剂及微生物细胞杀菌试剂

Fabrication of Reduced Graphene Oxide Decorated with Nonmetal-Doped Nanotitania: An Efficient Visible Light-Driven Photocatalyst and Sterilizing Agent for Microbial Cells.

作者信息

Yoosuf Shanavas, Kuthirummal Narayanan, Tharayil Shalina Begum

机构信息

Postgraduate and Research Department of Chemistry, Farook College (Autonomous), Affiliated to University of Calicut, Kozhikode, Kerala 673632, India.

Department of Physics and Astronomy, College of Charleston, 66 George Street, Charleston, South Carolina 29424, United States.

出版信息

ACS Omega. 2025 Feb 10;10(6):5296-5311. doi: 10.1021/acsomega.4c05015. eCollection 2025 Feb 18.

Abstract

The present study pertains to the fabrication of a visible light-responsive nanocomposite of nitrogen and sulfur-doped TiO anchoring reduced graphene oxide (NSNTG) using a facile microwave method for enhanced photocatalytic activity. Two other nanocomposites, TiO/rGO (NTG) and nitrogen-doped TiO/rGO (NNTG), were also synthesized by using the same method. X-ray diffraction (XRD) and Raman spectroscopy were employed to confirm the presence of the crystalline anatase TiO phase. Elemental composition and formation of a homogeneous dispersion of modified TiO on the GO surface were explored using Field-emission scanning electron microscopy (FESEM) with energy-dispersive X-ray (EDX), and transmission electron microscopy (TEM). X-ray photoelectron spectroscopy (XPS) and photoluminescence (PL) studies revealed surface composition, chemical state, and the presence of oxygen vacancy defects. A lower bandgap energy and stronger absorption in the visible region were confirmed by UV-visible diffuse reflectance spectroscopy (DRS) analysis. Mott-Schottky analysis revealed the flat band potentials and band alignment of NTG, NNTG, and NSNTG, indicating n-type semiconductor behaviors with flat band potential values of -0.50, -0.60, and -0.68 V, respectively, providing insights into their charge transfer processes. The high photocurrent response in NSNTG facilitates efficient charge migration by inhibiting charge recombination, aligning with the results from PL and EIS measurements. In addition, the large surface area (233.0 m/g) and a small pore size distribution (7.8 nm) of NSNTG nanocomposites were confirmed using N adsorption-desorption analysis, supporting enhanced adsorption of organic pollutants. The photocatalytic activity of the synthesized nanocomposites was studied by the degradation of organic dyes under visible light; NSNTG exhibited higher removal rates, 97 and 90% within 35 and 60 min, for methylene blue (MB) and rhodamine B (RhB), respectively. The optimal conditions for degradation were pH 8, dye concentration of 50 mg/L, and photocatalyst dosage of 50 mg. Mineralization rates evaluated from TOC analysis were 85.21 and 82.30% for MB and RhB, respectively. The key reactive species involved in photocatalytic degradation were identified as photogenerated hydroxyl radicals, holes, and superoxide radicals. The synthesized nanocomposites were also tested for their antimicrobial efficacy against Gram-negative and Gram-positive bacteria, by the disc diffusion method, NSNTG exhibited a maximum zone of inhibition against and , comparable to gentamycin. This study outlines the potential of NSNTG as a cost-effective, high-yield, and reusable material for environmental applications.

摘要

本研究涉及采用简便的微波法制备氮和硫共掺杂二氧化钛负载还原氧化石墨烯的可见光响应纳米复合材料(NSNTG),以增强光催化活性。还使用相同方法合成了另外两种纳米复合材料,即TiO/rGO(NTG)和氮掺杂TiO/rGO(NNTG)。采用X射线衍射(XRD)和拉曼光谱来确认结晶锐钛矿TiO相的存在。利用场发射扫描电子显微镜(FESEM)结合能量色散X射线(EDX)以及透射电子显微镜(TEM),探究了改性TiO在氧化石墨烯(GO)表面的元素组成和均匀分散体的形成。X射线光电子能谱(XPS)和光致发光(PL)研究揭示了表面组成、化学状态以及氧空位缺陷的存在。通过紫外可见漫反射光谱(DRS)分析证实了较低的带隙能量和在可见光区域更强的吸收。莫特-肖特基分析揭示了NTG、NNTG和NSNTG的平带电位和能带排列,表明它们具有n型半导体行为,平带电位值分别为-0.50、-0.60和-0.68 V,这为其电荷转移过程提供了见解。NSNTG中的高光电流响应通过抑制电荷复合促进了有效的电荷迁移,这与PL和电化学阻抗谱(EIS)测量结果一致。此外,使用N吸附-脱附分析证实了NSNTG纳米复合材料具有大表面积(233.0 m²/g)和小的孔径分布(7.8 nm),支持了对有机污染物的增强吸附。通过在可见光下降解有机染料研究了合成纳米复合材料的光催化活性;NSNTG对亚甲基蓝(MB)和罗丹明B(RhB)分别在35和60分钟内表现出较高的去除率,分别为97%和90%。降解的最佳条件为pH 8、染料浓度50 mg/L和光催化剂用量50 mg。通过总有机碳(TOC)分析评估的矿化率对于MB和RhB分别为85.21%和82.30%。光催化降解中涉及的关键活性物种被鉴定为光生羟基自由基、空穴和超氧自由基。还通过纸片扩散法测试了合成纳米复合材料对革兰氏阴性和革兰氏阳性细菌的抗菌效果,NSNTG对大肠杆菌和金黄色葡萄球菌表现出最大抑菌圈,与庆大霉素相当。本研究概述了NSNTG作为一种用于环境应用的经济高效、高产且可重复使用材料的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ed1b/11840782/290d36c52cd1/ao4c05015_0016.jpg

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