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Eco-friendly porous composite of octaphenyl polyhedral oligomeric silsesquioxane and HKUST-1 with hydrophobic–oleophilic properties towards sorption of oils and organic solvents
Dalton Transactions ( IF 3.5 ) Pub Date : 2024-07-23 , DOI: 10.1039/d4dt01397b Kanakarasu Dharmaraj 1 , Mohandas Sanjay Kumar 2 , Nallasamy Palanisami 3 , Muthuramalingam Prakash 2 , Pushparaj Loganathan 1 , Swaminathan Shanmugan 1
Dalton Transactions ( IF 3.5 ) Pub Date : 2024-07-23 , DOI: 10.1039/d4dt01397b Kanakarasu Dharmaraj 1 , Mohandas Sanjay Kumar 2 , Nallasamy Palanisami 3 , Muthuramalingam Prakash 2 , Pushparaj Loganathan 1 , Swaminathan Shanmugan 1
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The degradation of water bodies caused by organic pollutants from industrial wastewater discharge has made it necessary to develop new functional materials like hydrophobic–oleophilic materials that can efficiently remediate water. It is factual that many of the synthetic methods for creating hydrophobic–oleophilic materials involve the use of toxic or harmful reactants, such as fluorine or sulfur compounds. However, these methods often have significant drawbacks, including being hazardous to the environment, expensive, and complex to utilize. Therefore, there is an urgent need to develop a hydrophobic/oleophilic material that is non-toxic and eco-friendly in order to overcome the existing drawbacks. In this regard, we have proposed a modest and eco-friendly approach for constructing a hydrophobic–oleophilic Ph-POSS@HKUST-1 composite material by solution-assisted self-assembly for the conversion of hydrophilic HKUST-1 into hydrophobic HKUST-1 for separation applications. The incorporation of fluorine-free, low surface energy and hydrophobic POSS into HKUST-1 increased the hydrophobicity and oleophilicity of the system. The synthesized Ph-POSS@HKUST-1 composite material has been thoroughly characterized through FT-IR, PXRD, HR-SEM, BET, and thermogravimetric analysis. It has been observed that the material exhibits a contact angle of 137 ± 4° and shows high selectivity and absorption capacity towards organic solvents and oils from water mixtures. Concurrently, the Ph-POSS@HKUST-1@PDA@sponge has been effectively utilized for the separation of solvents and oils and it has shown more than 95% separation efficiency for up to 15 cycles. It is interesting to note that Ph-POSS@HKUST-1 and the Ph-POSS@HKUST-1@PDA@sponge have outstanding stability in abrasive chemical environments which is due to the presence of a mechanically and chemically stable inorganic–organic hybrid POSS nanocage. In addition, ab initio and DFT calculations elicit that the Ph-POSS@HKUST-1 composite is stabilized through π⋯π stacking instead of the C–H⋯π mode of interaction at the HKUST-1⋯Ph-POSS interface. Further electron density features confirm the interfacial interaction at the interface. Our latest research has led us to propose an eco-friendly and non-toxic hybrid composite material for efficiently tackling the issue of organic solvent and oil pollution in water mixtures.
中文翻译：
八苯基多面体低聚倍半硅氧烷和 HKUST-1 的环保多孔复合材料，具有疏水亲油特性，可吸附油和有机溶剂
工业废水排放中的有机污染物导致水体退化，因此有必要开发新型功能材料，例如能够有效修复水体的疏水亲油材料。事实上，许多制造疏水亲油材料的合成方法都涉及使用有毒或有害的反应物，例如氟或硫化合物。然而，这些方法通常具有显着的缺点，包括对环境有害、昂贵且使用复杂。因此，迫切需要开发一种无毒且环保的疏水/亲油材料以克服现有的缺陷。在这方面，我们提出了一种温和且环保的方法，通过溶液辅助自组装构建疏水亲油Ph-POSS@HKUST-1复合材料，将亲水性HKUST-1转化为疏水性HKUST-1分离应用。 HKUST-1中加入无氟、低表面能、疏水性的POSS，增加了体系的疏水性和亲油性。通过 FT-IR、PXRD、HR-SEM、BET 和热重分析对合成的 Ph-POSS@HKUST-1 复合材料进行了全面表征。据观察，该材料表现出 137 ± 4° 的接触角，并对水混合物中的有机溶剂和油表现出高选择性和吸收能力。同时，Ph-POSS@HKUST-1@PDA@sponge 已被有效地用于溶剂和油的分离，并且在长达 15 个循环中显示出超过 95% 的分离效率。 有趣的是，Ph-POSS@HKUST-1 和 Ph-POSS@HKUST-1@PDA@sponge 在磨料化学环境中具有出色的稳定性，这是由于机械和化学稳定的无机-有机杂化 POSS 的存在纳米笼。此外，从头计算和 DFT 计算表明，Ph-POSS@HKUST-1 复合材料是通过 π⋯π 堆积而不是 HKUST-1⋯Ph-POSS 界面处的 C-H⋯π 相互作用模式稳定的。进一步的电子密度特征证实了界面处的界面相互作用。我们的最新研究使我们提出了一种环保无毒的杂化复合材料，可有效解决水混合物中的有机溶剂和油污染问题。
更新日期：2024-07-23
中文翻译：
八苯基多面体低聚倍半硅氧烷和 HKUST-1 的环保多孔复合材料，具有疏水亲油特性，可吸附油和有机溶剂
工业废水排放中的有机污染物导致水体退化，因此有必要开发新型功能材料，例如能够有效修复水体的疏水亲油材料。事实上，许多制造疏水亲油材料的合成方法都涉及使用有毒或有害的反应物，例如氟或硫化合物。然而，这些方法通常具有显着的缺点，包括对环境有害、昂贵且使用复杂。因此，迫切需要开发一种无毒且环保的疏水/亲油材料以克服现有的缺陷。在这方面，我们提出了一种温和且环保的方法，通过溶液辅助自组装构建疏水亲油Ph-POSS@HKUST-1复合材料，将亲水性HKUST-1转化为疏水性HKUST-1分离应用。 HKUST-1中加入无氟、低表面能、疏水性的POSS，增加了体系的疏水性和亲油性。通过 FT-IR、PXRD、HR-SEM、BET 和热重分析对合成的 Ph-POSS@HKUST-1 复合材料进行了全面表征。据观察，该材料表现出 137 ± 4° 的接触角，并对水混合物中的有机溶剂和油表现出高选择性和吸收能力。同时，Ph-POSS@HKUST-1@PDA@sponge 已被有效地用于溶剂和油的分离，并且在长达 15 个循环中显示出超过 95% 的分离效率。 有趣的是，Ph-POSS@HKUST-1 和 Ph-POSS@HKUST-1@PDA@sponge 在磨料化学环境中具有出色的稳定性，这是由于机械和化学稳定的无机-有机杂化 POSS 的存在纳米笼。此外，从头计算和 DFT 计算表明，Ph-POSS@HKUST-1 复合材料是通过 π⋯π 堆积而不是 HKUST-1⋯Ph-POSS 界面处的 C-H⋯π 相互作用模式稳定的。进一步的电子密度特征证实了界面处的界面相互作用。我们的最新研究使我们提出了一种环保无毒的杂化复合材料，可有效解决水混合物中的有机溶剂和油污染问题。
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