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碳点修饰的硫化镉异质结纳米球用于增强可见光驱动的光催化染料降解和制氢。

Carbon dots decorated cadmium sulphide heterojunction-nanospheres for the enhanced visible light driven photocatalytic dye degradation and hydrogen generation.

机构信息

Department of Chemistry, M S Ramaiah Institute of Technology (An Autonomous Institute Affiliated to Visvesvaraya Technological University, Belgaum), Bengaluru 560054, India; Department of Chemistry/Biochemistry, M S Ramaiah College of Arts, Science and Commerce (Affiliated to Bangalore Central University), Bangalore 560054, India.

Department of Chemistry, M S Ramaiah Institute of Technology (An Autonomous Institute Affiliated to Visvesvaraya Technological University, Belgaum), Bengaluru 560054, India.

出版信息

J Colloid Interface Sci. 2022 Dec;627:956-968. doi: 10.1016/j.jcis.2022.07.100. Epub 2022 Jul 19.

DOI:10.1016/j.jcis.2022.07.100
PMID:35901574
Abstract

Carbon dots (C-dots) developed from beetroot is used for the rational design of cadmium sulphide based heterojunction photocatalysts (C-dots@CdS) using hydrothermal technique. The crystal structure, phase, morphology and optical characteristics of the synthesised materials are determined using X-ray diffraction (XRD), High resolution transmission electron microscopy (HR-TEM), Field emission scanning electron microscopy (FESEM), Energy dispersive X-ray analysis (EDAX), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, UV-Visible diffuse reflectance spectroscopy (UV-DRS), photoluminescence spectroscopy (PL spectroscopy), BET adsorption, X-ray photoelectron spectroscopy (XPS) and electrochemical studies. Using C-dots@CdS catalytic system, a superior photocatalytic activity relative to the undecorated CdS is observed. Among the C-dots@CdS samples, the CdS loaded with 6 wt% of C-dots exhibited enhanced hydrogen evolution rate compared with other samples considered for the study. CdS nanospheres modified with C-dots (6 wt%) resulted in the photocatalytic hydrogen evolution rate of 1582 µmolg against 849 µmolg evolution rate obtained for CdS nanospheres within 3 h. In spite of being 0D/0D type nano-heteroarchitecture, C-dots@CdS system obtained an apparent quantum yield of 6.37 % for the catalytic dosage of 20 mg under the irradiation of visible light. CdS in the C-dots@CdS system serves as the light harvester while C-dots with discernible edges can maintain the continuous supply of photo-excited charge carriers and hence can reduce the charge-carrier recombination. Further, the photodegradation of crystal violet dye using the optimised dosage of C-dots@CdS-6 exhibited an efficiency of 97.3 % in 120 min of visible light irradiation under neutral conditions. The detailed kinetic study reveals that the mechanism of photodegradation of crystal violet dye using C-dots@CdS system can be described using pseudo-second-order kinetics. The presence of oxygen rich hydrophilic surface functionalities of C-dots, the formation of near-surface heterojunction and the suitable band structure of C-dots@CdS system leading to the optimum charge carrier separation kinetics can be attributed to the enhanced photocatalytic performance. This work offers a promising strategy to develop bio-derived C-dots based heterojunction photocatalyst to address the burgeoning energy and environmental demands.

摘要

采用水热技术,从甜菜根中开发的碳点(C-dots)用于合理设计硫化镉基异质结光催化剂(C-dots@CdS)。使用 X 射线衍射(XRD)、高分辨率透射电子显微镜(HR-TEM)、场发射扫描电子显微镜(FESEM)、能谱(EDAX)、傅里叶变换红外光谱(FTIR)、拉曼光谱、紫外-可见漫反射光谱(UV-DRS)、光致发光光谱(PL 光谱)、BET 吸附、X 射线光电子能谱(XPS)和电化学研究来确定合成材料的晶体结构、相、形态和光学特性。在 C-dots@CdS 催化体系中,观察到相对于未修饰的 CdS 的优异光催化活性。在所研究的样品中,负载 6wt%的 C-dots 的 CdS 表现出比其他样品更高的析氢速率。CdS 纳米球修饰的 C-dots(6wt%)在 3h 内产生 1582 µmolg 的光催化析氢速率,而 CdS 纳米球的析氢速率为 849 µmolg。尽管 C-dots@CdS 体系为 0D/0D 型纳米异质结构,但在可见光照射下,在 20mg 的催化剂量下,其表观量子产率为 6.37%。C-dots@CdS 体系中的 CdS 作为光收集器,而具有明显边缘的 C-dots 可以保持光生载流子的连续供应,从而减少载流子复合。此外,在中性条件下,优化剂量的 C-dots@CdS-6 对结晶紫染料的光降解效率在 120min 的可见光照射下达到 97.3%。详细的动力学研究表明,使用 C-dots@CdS 体系光降解结晶紫染料的机制可以用拟二级动力学来描述。C-dots 富氧亲水性表面官能团的存在、近表面异质结的形成以及 C-dots@CdS 体系适宜的能带结构导致最佳载流子分离动力学,可以归因于增强的光催化性能。这项工作提供了一种有前途的策略,用于开发基于生物衍生的 C-dots 的异质结光催化剂,以满足新兴的能源和环境需求。

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