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砷和氟的吸附:单一及竞争吸附系统的建模

Adsorption of arsenic and fluoride: Modeling of single and competitive adsorption systems.

作者信息

Acharya Amrutha, Jeppu Gautham, Girish Chikmagalur Raju, Prabhu Balakrishna, Murty Vytla Ramachandra, Martis Alita Stephy, Ramesh Shrividya

机构信息

Department of Chemical Engineering, Manipal Institute of Technology, Manipal Academy of Higher Education, Manipal, 576104, Karnataka, India.

Department of Biotechnology, Manipal Institute of Technology, Manipal Academy of Higher Education, Manipal, 576104, Karnataka, India.

出版信息

Heliyon. 2024 May 25;10(11):e31967. doi: 10.1016/j.heliyon.2024.e31967. eCollection 2024 Jun 15.

Abstract

The elevated co-occurrence of arsenic and fluoride in surface and groundwater poses risks to human health in many parts of the world. Using single and competitive batch equilibrium adsorption studies, this research focuses on As(V) and F adsorption by activated carbon and its modeling. BET, XRD, FESEM, EDS, and FTIR analysis were used to discern the structural characteristics of activated carbon. The influence of dosage, pH, and contact time were also investigated in single and simultaneous adsorption systems. The maximum adsorption capacity of activated carbon for arsenic and fluoride were found to be 3.58 mg/g and 2.32 mg/g, respectively. Kinetics studies indicated that pseudo-second-order kinetic model fit better than pseudo-first-order, Elovich, and intraparticle diffusion kinetic models. The non-linear regression analysis of Langmuir, Freundlich, Toth, Redlich Petersons, and Modified Langmuir Freundlich models was used to determine single-component asorption model parameters. Additionally, the simultaneous adsorption was rigorously modeled and compared using the Extended Langmuir (EL), Extended Langmuir Freundlich (ELF), Modified Competitive Langmuir (MCL), and Jeppu Amrutha Manipal Multicomponent (JAMM) isotherm models, and competitive mechanisms were interpreted for the simultaneous adsorption system. Further, the model performances were evaluated by statistical error analysis using the normalized average percentage error (NAPE), root mean square errors (RMSE), and the correlation coefficient (R). According to the modeling results, single equilibrium data fitted better with the Modified Langmuir Freundlich isotherm model, with a higher R of 0.99 and lower NAPE values of 3.8 % and 1.28 % for As(V) and F, than other models. For the binary adsorption, the Extended Langmuir Freundlich isotherm model demonstrated excellent fit with lowest errors. All the competitive isotherm models fit the As(V) and F simultaneous sorption systems reasonably well. Furthermore, the research unveiled a nuanced hierarchy of isotherm fitting, with ELF > EL > MCL > JAMM in varying arsenic at a constant fluoride concentration, and ELF > JAMM > EL > MCL in varying fluoride at a constant arsenic concentrations. In addition, competitive studies divulged crucial insights into selective adsorption, as As(V) exhibits a pronounced adsorption selectivity over F on activated carbon. In essence, As(V) showed a more pronounced antagonistic behavior over F, whereas F exhibited a much lesser competitive behavior in the adsorption of arsenic.

摘要

地表和地下水中砷与氟的同时超标在世界许多地区对人类健康构成风险。本研究通过单批次和竞争批次平衡吸附研究,聚焦于活性炭对五价砷(As(V))和氟的吸附及其建模。采用比表面积分析仪(BET)、X射线衍射仪(XRD)、场发射扫描电子显微镜(FESEM)、能谱仪(EDS)和傅里叶变换红外光谱仪(FTIR)分析来识别活性炭的结构特征。还在单吸附和同时吸附系统中研究了投加量、pH值和接触时间的影响。发现活性炭对砷和氟的最大吸附容量分别为3.58毫克/克和2.32毫克/克。动力学研究表明,准二级动力学模型比准一级、埃洛维奇(Elovich)和颗粒内扩散动力学模型拟合效果更好。利用朗缪尔(Langmuir)、弗伦德里希(Freundlich)、托特(Toth)、雷德利希 - 彼得森(Redlich Petersons)和修正朗缪尔 - 弗伦德里希(Modified Langmuir Freundlich)模型的非线性回归分析来确定单组分吸附模型参数。此外,使用扩展朗缪尔(EL)、扩展朗缪尔 - 弗伦德里希(ELF)、修正竞争朗缪尔(MCL)和杰普·阿姆鲁塔·马尼帕尔多组分(JAMM)等温线模型对同时吸附进行了严格建模和比较,并解释了同时吸附系统的竞争机制。进一步地,通过使用归一化平均百分比误差(NAPE)、均方根误差(RMSE)和相关系数(R)的统计误差分析来评估模型性能。根据建模结果,单平衡数据与修正朗缪尔 - 弗伦德里希等温线模型拟合更好,对于As(V)和F,其相关系数R更高,分别为0.99,NAPE值更低,As(V)为3.8%,F为1.28%,优于其他模型。对于二元吸附,扩展朗缪尔 - 弗伦德里希等温线模型拟合效果极佳,误差最低。所有竞争等温线模型对As(V)和F的同时吸附系统拟合都相当不错。此外,研究揭示了等温线拟合的细微层次结构,在氟浓度恒定、砷浓度变化时,拟合顺序为ELF > EL > MCL > JAMM;在砷浓度恒定、氟浓度变化时,拟合顺序为ELF > JAMM > EL > MCL。此外,竞争研究揭示了关于选择性吸附的关键见解,因为在活性炭上As(V)对F表现出明显的吸附选择性。本质上,As(V)对F表现出更明显的拮抗行为,而F在砷的吸附中表现出的竞争行为要小得多。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e5ab/11167366/592bb953ec86/ga1.jpg

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