1,3,5-苯三羧酸构建的锌(II)配位聚合物和活性炭衍生纳米复合材料的实验和密度泛函理论研究,ACS Omega

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1,3,5-苯三羧酸构建的锌(II)配位聚合物和活性炭衍生纳米复合材料的实验和密度泛函理论研究
ACS Omega ( IF 3.7 ) Pub Date : 2021-10-21 , DOI: 10.1021/acsomega.1c04037
Chinyere A Anyama ₁ , Benedict I Ita ₂ , Ayi A Ayi ₁ , Hitler Louis ₃ , Emmanuel E D Okon ₁ , Joseph O Ogar _{1,

4} , Charles O Oseghale ₅

Affiliation

一种配位聚合物，其组成为 C ₁₂ H ₂₀ O ₁₆ Zn ₂(ZnBTC) (BTC = 苯-1,3,5-三羧酸盐) 在 120 °C 的水热条件下合成，并使用单晶 X 射线晶体学确定其晶体结构。使用密度泛函理论计算方法进行化合物的第一性原理电子结构研究。使用隐式溶剂化模型在气相和溶剂相中研究了 ZnBTC 的最高占据分子轨道、最低未占据分子轨道、能隙和全局反应性描述符，同时使用自然溶剂化模型研究了供体 - 受体相互作用键轨道分析。结果表明，ZnBTC 在溶剂介质中更稳定但反应性较低。较大的稳定能E ⁽²⁾表明 ZnBTC 在溶剂中的相互作用比在气相中更大。用ZnCl ₂和/或KOH化学处理的橙皮活性炭和香蕉皮活性炭对ZnBTC的合成进行改性以获得纳米复合材料。ZnBTC 和纳米复合材料通过粉末 X 射线衍射 (PXRD)、热重分析和傅里叶变换红外光谱进行表征。比表面积（S _BET) 和材料的平均孔径通过使用布鲁瑙尔-埃米特-泰勒 (BET) 方法的氮吸附测量确定，而扫描电子显微镜和透射电子显微镜分别用于观察它们的形态和粒径。所有活性炭材料的 PXRD 在 12.7 和 13.9° 的 2θ 值处显示出峰值，分别对应于6.94 和 6.32的d间距。材料的 N ₂吸附-解吸等温线属于 II 型，纳米复合材料显示出增强的S _BET与原始的 ZnBTC 相比。结果还表明，来自香蕉皮和衍生纳米复合材料的活性炭比从橙皮中获得的活性炭表现出更好的多孔结构参数。发现使用 ZnBTC 作为光催化剂的水溶液中甲基橙的降解效率为 52%，而纳米复合材料的降解效率提高了 79%。

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Experimental and Density Functional Theory Studies on a Zinc(II) Coordination Polymer Constructed with 1,3,5-Benzenetricarboxylic Acid and the Derived Nanocomposites from Activated Carbon

A coordination polymer with the composition C₁₂H₂₀O₁₆Zn₂ (ZnBTC) (BTC = benzene-1,3,5-tricarboxylate) was synthesized under hydrothermal conditions at 120 °C, and its crystal structure was determined using single-crystal X-ray crystallography. First-principles electronic structure investigation of the compound was carried out using the density functional theory computational approach. The highest occupied molecular orbital, the lowest unoccupied molecular orbital, the energy gap, and the global reactivity descriptors of ZnBTC were investigated in both the gas phase and the solvent phase using the implicit solvation model, while the donor–acceptor interactions were studied using natural bond orbital analyses. The results revealed that ZnBTC is more stable but less reactive in solvent medium. The larger stabilization energy E⁽²⁾ indicates a greater interaction of ZnBTC in the solvent than in the gas phase. Orange peel activated carbon and banana peel activated carbon chemically treated with ZnCl₂ and/or KOH were used to modify the synthesis of ZnBTC to obtain nanocomposites. ZnBTC and the nanocomposites were characterized by powder X-ray diffraction (PXRD), thermogravimetric analysis, and Fourier transform infrared. The specific surface area (S_BET) and the average pore diameter of the materials were determined by nitrogen sorption measurements using the Brunauer–Emmett–Teller (BET) method, while scanning electron microscopy and transmission electron microscopy were used to observe their morphology and particle size, respectively. The PXRD of all the activated carbon materials exhibited peaks at 2θ values of 12.7 and 13.9° corresponding to a d-spacing of 6.94 and 6.32 Å, respectively. The N₂ adsorption–desorption isotherm of the materials are of type II with nanocomposites showing enhanced S_BET compared to the pristine ZnBTC. The results also revealed that activated carbons from the banana peel and the derived nanocomposites exhibited better porous structure parameters than those obtained from orange peel. The degradation efficiency of methyl orange in aqueous solutions using ZnBTC as a photocatalyst was found to be 52 %, while that of the nanocomposites were enhanced up to 79 %.

更新日期：2021-11-02

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