{"title":"增强离子染料去除的还原性氧化石墨烯的绿色制备","authors":"Ruichao Zhao , Chaoke Bulin , Ting Guo","doi":"10.1016/j.matchemphys.2025.130850","DOIUrl":null,"url":null,"abstract":"<div><div>Reduced graphene oxide was facilely fabricated with a green route based on graphene oxide (GO) reduction by ascorbic acid for adsorptive removal of methyl blue (MLB). Adsorption mechanism was unveiled via combining batch adsorption, adsorption fitting, spectroscopic analysis and the hard-soft acid-base (HSAB) principle. Result shows, reduction ameliorates adsorption efficiency, which can be elucidated from two aspects. From thermodynamic aspect, conjugated structure of GO is restored by reduction, leading to intensified π-π interaction between adsorbent and MLB. From kinetic aspect, enlarged pores generated by reduction facilitates MLB diffusion towards adsorption sites to form stable adsorption configuration. Particularly, reduced graphene oxide reaches adsorption quantity 59.76 mg g<sup>−1</sup> for MLB in 8 min. Adsorption isotherm and kinetic fittings propose favorable chemical adsorption with heterogeneous affinity induced by electrostatic interaction. Ionization state of the functional groups on graphene surface, FTIR and UV–Vis characterizations, HSAB principle calculation further deciphers the adsorption mechanism in three points. (1) Heterogeneous affinity originates from polar and non polar interactions. (2) The polar interaction is hydrogen bond between –OH (or –COOH) and N atom, as well as covalent bond between –OH and S atom. (3) The non polar interaction is π-π interaction. This work enlightens the construction of graphene based adsorbent via green route for dye removal.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"340 ","pages":"Article 130850"},"PeriodicalIF":4.3000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Green fabrication of reduced graphene oxide for enhanced removal of ionic dye\",\"authors\":\"Ruichao Zhao , Chaoke Bulin , Ting Guo\",\"doi\":\"10.1016/j.matchemphys.2025.130850\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Reduced graphene oxide was facilely fabricated with a green route based on graphene oxide (GO) reduction by ascorbic acid for adsorptive removal of methyl blue (MLB). Adsorption mechanism was unveiled via combining batch adsorption, adsorption fitting, spectroscopic analysis and the hard-soft acid-base (HSAB) principle. Result shows, reduction ameliorates adsorption efficiency, which can be elucidated from two aspects. From thermodynamic aspect, conjugated structure of GO is restored by reduction, leading to intensified π-π interaction between adsorbent and MLB. From kinetic aspect, enlarged pores generated by reduction facilitates MLB diffusion towards adsorption sites to form stable adsorption configuration. Particularly, reduced graphene oxide reaches adsorption quantity 59.76 mg g<sup>−1</sup> for MLB in 8 min. Adsorption isotherm and kinetic fittings propose favorable chemical adsorption with heterogeneous affinity induced by electrostatic interaction. Ionization state of the functional groups on graphene surface, FTIR and UV–Vis characterizations, HSAB principle calculation further deciphers the adsorption mechanism in three points. (1) Heterogeneous affinity originates from polar and non polar interactions. (2) The polar interaction is hydrogen bond between –OH (or –COOH) and N atom, as well as covalent bond between –OH and S atom. (3) The non polar interaction is π-π interaction. This work enlightens the construction of graphene based adsorbent via green route for dye removal.</div></div>\",\"PeriodicalId\":18227,\"journal\":{\"name\":\"Materials Chemistry and Physics\",\"volume\":\"340 \",\"pages\":\"Article 130850\"},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2025-04-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Chemistry and Physics\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0254058425004961\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Chemistry and Physics","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0254058425004961","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
基于抗坏血酸还原氧化石墨烯(GO)的绿色工艺路线,轻松制备了还原氧化石墨烯,用于吸附去除甲基蓝(MLB)。通过结合批量吸附、吸附拟合、光谱分析和软硬酸碱(HSAB)原理,揭示了吸附机理。结果表明,还原作用会提高吸附效率,这可以从两个方面来解释。从热力学方面来看,还原作用恢复了 GO 的共轭结构,从而加强了吸附剂与 MLB 之间的 π-π 相互作用。从动力学方面来看,还原产生的孔隙增大,有利于 MLB 向吸附位点扩散,形成稳定的吸附构型。特别是,还原氧化石墨烯在 8 分钟内对 MLB 的吸附量达到 59.76 mg g-1。吸附等温线和动力学测试表明,在静电作用的诱导下,化学吸附具有良好的异质亲和性。石墨烯表面官能团的电离状态、傅立叶变换红外光谱和紫外可见光谱表征、HSAB 原理计算从三个方面进一步揭示了吸附机理。(1)异质亲和力源于极性和非极性相互作用。(2)极性相互作用是 -OH(或 -COOH)与 N 原子间的氢键,以及 -OH 与 S 原子间的共价键。(3) 非极性相互作用是 π-π 作用。这项工作为通过绿色途径构建石墨烯基吸附剂去除染料提供了启示。
Green fabrication of reduced graphene oxide for enhanced removal of ionic dye
Reduced graphene oxide was facilely fabricated with a green route based on graphene oxide (GO) reduction by ascorbic acid for adsorptive removal of methyl blue (MLB). Adsorption mechanism was unveiled via combining batch adsorption, adsorption fitting, spectroscopic analysis and the hard-soft acid-base (HSAB) principle. Result shows, reduction ameliorates adsorption efficiency, which can be elucidated from two aspects. From thermodynamic aspect, conjugated structure of GO is restored by reduction, leading to intensified π-π interaction between adsorbent and MLB. From kinetic aspect, enlarged pores generated by reduction facilitates MLB diffusion towards adsorption sites to form stable adsorption configuration. Particularly, reduced graphene oxide reaches adsorption quantity 59.76 mg g−1 for MLB in 8 min. Adsorption isotherm and kinetic fittings propose favorable chemical adsorption with heterogeneous affinity induced by electrostatic interaction. Ionization state of the functional groups on graphene surface, FTIR and UV–Vis characterizations, HSAB principle calculation further deciphers the adsorption mechanism in three points. (1) Heterogeneous affinity originates from polar and non polar interactions. (2) The polar interaction is hydrogen bond between –OH (or –COOH) and N atom, as well as covalent bond between –OH and S atom. (3) The non polar interaction is π-π interaction. This work enlightens the construction of graphene based adsorbent via green route for dye removal.
期刊介绍:
Materials Chemistry and Physics is devoted to short communications, full-length research papers and feature articles on interrelationships among structure, properties, processing and performance of materials. The Editors welcome manuscripts on thin films, surface and interface science, materials degradation and reliability, metallurgy, semiconductors and optoelectronic materials, fine ceramics, magnetics, superconductors, specialty polymers, nano-materials and composite materials.