Carbon quantum dots (CQDs)-supported CeO2/Al2O3 with tunable band gap for the efficient degradation of plastic waste into porous carbon materials under mild conditions: experiment and DFT

IF 2.1 4区 材料科学 Q3 CHEMISTRY, MULTIDISCIPLINARY
Jessica Jhovana Villalba Arredondo, Cristian Brayan Palacios Cabrera, Carlos Alberto Huerta Aguilar, Jayanthi Narayanan, María del Carmen Durán Domínguez de Bazúa, Pandiyan Thangarasu, Eduardo Daniel Tecuapa Flores, Alan Javier Santiago Cuevas
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引用次数: 0

Abstract

A novel photocatalyst based on carbon quantum dots (CQDs)-functionalized CeO2/Al2O3 nanoparticles (NPs) was generated and applied for the oxidative degradation of polyethylene terephthalate (PET) and low-density polyethylene (LDPE). The chemical structure and morphology of Al2O3/CeO2@CQDs from the FTIR, XRD, and SEM analysis showed that the incorporation of CQDs increased the band gap value from 4.2 to 2.4 eV due to the quantum confinement effect with CQDs. The degradation of PET and LDPE was monitored through FTIR spectroscopy by registering changes in absorption bands, and the degraded products were analyzed through different analytical techniques. SEM–EDS, XRD, HPLC, and MS spectra revealed effective conversion of PET and LDPE to highly porous carbon materials with weight losses of 98% and 91%, respectively. From the analysis of the degradation products, a suitable degradation mechanism was proposed for both plastics, which was subsequently verified with DFT molecular energy calculations.

Graphical Abstract

具有可调带隙的碳量子点(CQDs)负载CeO2/Al2O3在温和条件下高效降解塑料废物为多孔碳材料:实验和DFT
制备了一种基于碳量子点(CQDs)功能化CeO2/Al2O3纳米颗粒(NPs)的新型光催化剂,并将其应用于聚对苯二甲酸乙二醇酯(PET)和低密度聚乙烯(LDPE)的氧化降解。FTIR、XRD和SEM对Al2O3/CeO2@CQDs的化学结构和形貌分析表明,由于CQDs的量子约束效应,Al2O3/CeO2@CQDs的带隙值从4.2 eV增加到2.4 eV。通过FTIR光谱记录吸收带的变化来监测PET和LDPE的降解,并通过不同的分析技术对降解产物进行分析。SEM-EDS、XRD、HPLC和MS谱显示PET和LDPE有效转化为高孔碳材料,重量损失分别为98%和91%。通过对降解产物的分析,提出了两种塑料的合适降解机理,并用DFT分子能计算对其进行了验证。图形抽象
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来源期刊
Journal of Nanoparticle Research
Journal of Nanoparticle Research 工程技术-材料科学:综合
CiteScore
4.40
自引率
4.00%
发文量
198
审稿时长
3.9 months
期刊介绍: The objective of the Journal of Nanoparticle Research is to disseminate knowledge of the physical, chemical and biological phenomena and processes in structures that have at least one lengthscale ranging from molecular to approximately 100 nm (or submicron in some situations), and exhibit improved and novel properties that are a direct result of their small size. Nanoparticle research is a key component of nanoscience, nanoengineering and nanotechnology. The focus of the Journal is on the specific concepts, properties, phenomena, and processes related to particles, tubes, layers, macromolecules, clusters and other finite structures of the nanoscale size range. Synthesis, assembly, transport, reactivity, and stability of such structures are considered. Development of in-situ and ex-situ instrumentation for characterization of nanoparticles and their interfaces should be based on new principles for probing properties and phenomena not well understood at the nanometer scale. Modeling and simulation may include atom-based quantum mechanics; molecular dynamics; single-particle, multi-body and continuum based models; fractals; other methods suitable for modeling particle synthesis, assembling and interaction processes. Realization and application of systems, structures and devices with novel functions obtained via precursor nanoparticles is emphasized. Approaches may include gas-, liquid-, solid-, and vacuum-based processes, size reduction, chemical- and bio-self assembly. Contributions include utilization of nanoparticle systems for enhancing a phenomenon or process and particle assembling into hierarchical structures, as well as formulation and the administration of drugs. Synergistic approaches originating from different disciplines and technologies, and interaction between the research providers and users in this field, are encouraged.
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