吸附去除金刚石绿G的三金属CuCrFe-BTC MOF的快速合成及表征:动力学、等温线和热力学研究

IF 3.7 2区 化学 Q2 CHEMISTRY, APPLIED
Ali Umar, Sultan Alam, Hira Zaman, Muhammad Zahoor, Riaz Ullah, Essam A. Ali, Muhammad Naveed Umar
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引用次数: 0

摘要

本研究采用溶剂热法合成了三金属有机骨架(CuCrFe-BTC MOF),并将其应用于对金刚石绿G染料的吸附去除。采用SEM、FTIR、XRD、TGA、Zeta电位分析仪和比表面积分析仪对合成的CuCrFe-BTC MOF进行了表征。结果表明,合成的MOF在纳米(80 nm)范围内具有球形颗粒,FTIR分析证实了必要的官能团的存在,XRD分析表明结晶度高,峰明显,TGA分析表明热稳定性高达500℃。zeta电位分析预测的中等负电荷值(- 14.7 mV)表明其适合阳离子污染物的修复。BET分析显示,该材料的表面积高达767 m2/g,具有微孔结构。然后将合成的MOF用于间歇吸附法去除水中的金刚石绿G染料。考察了接触时间、吸附剂用量、pH、初始染料浓度和温度对吸附的影响,优化了吸附工艺。最佳吸附时间为60 min,吸附剂用量为0.01 g, pH为8,初始染料浓度为100 ppm,温度为298 K。采用不同的等温线和动力学模型对吸附实验数据进行了分析。动力学数据分析表明,数据与拟二阶模型拟合最佳,证实了吸附过程的化学吸附性质。等温线研究数据符合Langmuir等温线模型,表明单层吸附的最大吸附量Qm为434 mg.g−1。热力学研究表明,吸附过程为吸热过程,焓变∆H°为14.74 jmol−1,熵变∆S°为53.44 jmol−1 K−1。吉布斯自由能∆G°在所有实验温度下均为负。Gibbs自由能随温度的升高而增大(在293、313和333 K时分别为- 0.921、- 1.989和- 3.058),表明该工艺在高温下是可行的。整个吸附过程可能涉及几种潜在的机制,包括涉及π-π键的化学吸附、孔填充、静电相互作用和氢键。用氢氧化钠和乙醇对吸附剂进行多次循环再生,直到第7次循环,吸附剂的吸附容量几乎没有变化。该研究验证了CuCrFe-BTC MOF的结构稳定性和性能,并显示了其在工业应用中的再生潜力,因此可以被认为是商业活性炭的最佳替代品。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Facile Synthesis and Characterization of Trimetallic CuCrFe-BTC MOF for the Adsorptive Removal of Diamond Green G: Kinetic, Isotherm, and Thermodynamic Study

Facile Synthesis and Characterization of Trimetallic CuCrFe-BTC MOF for the Adsorptive Removal of Diamond Green G: Kinetic, Isotherm, and Thermodynamic Study

In this study, trimetallic organic frameworks (CuCrFe-BTC MOF) was synthesized via the solvothermal method and applied for the adsorptive removal of diamond green G dye from aqueous medium. The synthesized CuCrFe-BTC MOF was characterized by SEM, FTIR, XRD, TGA, Zeta potential analyzer, and surface area analyzer. The results revealed that the synthesized MOF has spherical particles in the nanoscale range (80 nm), FTIR analysis confirmed the presence of necessary functional groups, XRD indicated high crystallinity with distinct peaks and TGA analysis demonstrated the thermal stability up to 500°C. The moderate negative charge value (−14.7 mV) as predicted by zeta potential analysis suggests its suitability for remediation of cationic pollutants. BET analysis revealed a high surface area of 767 m2/g, with a microporous structure. The synthesized MOF were then employed for the removal of diamond green G dye from water using batch adsorption approach. The effect of contact time, adsorbent dosage, pH, initial dye concentration, and temperature on adsorption was also evaluated to optimize the adsorption process. The maximum adsorption was achieved at optimum contact time of 60 min, adsorbent dosage of 0.01 g, pH 8, initial dye concentration of 100 ppm, and temperature 298 K. Different isotherm and kinetic models were applied to the adsorption experimental data. Kinetic data analysis revealed the best fit of the data with pseudo-second-order model confirming the chemisorption nature of the adsorption process. The isotherm studies data fitted well into Langmuir isotherm model, indicating monolayer adsorption with a maximum adsorption capacity Qm of 434 mg.g−1. Thermodynamic studies revealed that the adsorption process was endothermic with an enthalpy change ∆H° of 14.74 kjmol−1 and an entropy change ∆S° of 53.44 jmol−1 K−1. Gibbs free energy ∆G° was negative at all tested experimental temperatures. The Gibbs free energy value increased with increase in temperature (−0.921, −1.989, and −3.058 at 293, 313, and 333 K respectively) indicated the feasibility of the process at high temperature. The overall adsorption process might involve several potential mechanisms including chemisorption involving π-π bonding, pore-filling, electrostatic interactions, and hydrogen bonding. The adsorbent was regenerated with sodium hydroxide and ethanol for many cycles and very little differences in adsorption capacity were recorded till 7th cycle. The study verified the structural stability and performance of CuCrFe-BTC MOF and showed its regeneration potential in industrial applications and could therefore, be considered as best alternative of commercial activated carbon.

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来源期刊
Applied Organometallic Chemistry
Applied Organometallic Chemistry 化学-无机化学与核化学
CiteScore
7.80
自引率
10.30%
发文量
408
审稿时长
2.2 months
期刊介绍: All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.
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