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镍/钛层状双氢氧化物:合成、表征及其作为光催化剂用于可见光降解水溶液中亚甲基蓝的应用。

Ni/Ti layered double hydroxide: synthesis, characterization and application as a photocatalyst for visible light degradation of aqueous methylene blue.

作者信息

Roy Chowdhury Priyadarshi, Bhattacharyya Krishna G

机构信息

Department of Chemistry, Gauhati University, Guwahati 781014, Assam, India.

出版信息

Dalton Trans. 2015 Apr 21;44(15):6809-24. doi: 10.1039/c5dt00257e.

Abstract

Visible light responsive 2 : 1 Ni/Ti layered double hydroxide (LDH) was synthesized by a single step hydrothermal route using commercially available Ni(NO3)2·6H2O, TiCl4 and urea. The material exhibited significant absorption in the visible range with a very narrow band gap (2.68 eV). This could be attributed to structural defects as confirmed by diffuse reflectance spectroscopy (DRS), photoluminescence (PL), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) measurements. FT-IR, TGA, DTA, DSC, HR-TEM and SEM-EDX measurements yielded information about structural aspects, thermal stability and surface morphology. Surface and pore characteristics of the material were obtained from the BET isotherm for N2 adsorption at 77 K. Zeta potential measurements were used to characterize the electrical properties of the surface while XPS revealed changes in surface states and oxygen deficiencies. The material was found to be an excellent photocatalyst for the degradation of aqueous methylene blue in visible light. The photocatalytic properties of the material were explained on the basis of the narrow band gap, the high surface area and the presence of surface defects. The photocatalytic activity improved in alkaline media [pH 11.0, catalyst load 15 mg in 200 ml dye solution, dye concentration 1 × 10(-6) M (= 0.3198 mg L(-1))] due to the electrostatic attractions between the dye cations and the negative charges on the Ni/Ti LDH surface. The catalytic activity was found to be higher than the common commercial catalysts like ZnO, ZnS, NiO, TiO2 and Degussa P25. The catalytic activity was retained even after five methylene blue degradation cycles, demonstrating that the LDH could be an important addition to the field of wastewater treatment.

摘要

采用市售的硝酸镍六水合物、四氯化钛和尿素,通过一步水热法合成了可见光响应型2:1镍/钛层状双氢氧化物(LDH)。该材料在可见光范围内表现出显著吸收,带隙非常窄(2.68电子伏特)。这可归因于结构缺陷,漫反射光谱(DRS)、光致发光(PL)、X射线衍射(XRD)和X射线光电子能谱(XPS)测量证实了这一点。傅里叶变换红外光谱(FT-IR)、热重分析(TGA)、差热分析(DTA)、差示扫描量热法(DSC)、高分辨透射电子显微镜(HR-TEM)和扫描电子显微镜-能谱分析(SEM-EDX)测量得出了有关结构方面、热稳定性和表面形态的信息。通过77K下氮气吸附的BET等温线获得了该材料的表面和孔隙特征。zeta电位测量用于表征表面的电学性质,而XPS揭示了表面态和氧缺陷的变化。发现该材料是可见光下降解水溶液中亚甲基蓝的优异光催化剂。基于窄带隙、高比表面积和表面缺陷的存在解释了该材料的光催化性能。在碱性介质中[pH 11.0,200毫升染料溶液中催化剂负载量15毫克,染料浓度1×10⁻⁶M(=0.3198毫克/升)],由于染料阳离子与镍/钛LDH表面负电荷之间的静电吸引,光催化活性提高。发现该催化活性高于常见的商业催化剂,如氧化锌、硫化锌、氧化镍、二氧化钛和德固赛P25。即使经过五个亚甲基蓝降解循环,催化活性仍得以保留,表明LDH可能是废水处理领域的一项重要补充。

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