Solvent Effect on Supramolecular Self-Assembly of Chlorophylls a on Chemically Reduced Graphene Oxide.
Solvent Effect on Supramolecular Self-Assembly of Chlorophylls a on Chemically Reduced Graphene Oxide.
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DOI：
10.1021/acs.langmuir.0c02370
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发表时间：
2020-10
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影响因子：
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通讯作者：
T. R. B. Ramakrishna;M. Mathesh;Zhen Liu;Chunmei Zhang;A. Du;Jingquan Liu;C. Barrow;Min Chen;M. Biggs;Wenrong Yang
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文献类型：
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作者：
T. R. B. Ramakrishna;M. Mathesh;Zhen Liu;Chunmei Zhang;A. Du;Jingquan Liu;C. Barrow;Min Chen;M. Biggs;Wenrong Yang
溶剂在分子的表面相互作用中起着重要的作用。在这项研究中，我们使用“叶绿素a”，一个典型的分子，研究其超分子自组装与化学还原氧化石墨烯在三种不同类型的溶剂：极性质子，极性非质子，和非极性。据观察，只有能够提供质子的极性质子溶剂才能促进混合系统中叶绿素a和化学还原的氧化石墨烯纳米片之间的氢键合。氢键的形成进一步引发了其他非共价相互作用，如π-π堆积和疏水相互作用，这共同发挥了化学还原氧化石墨烯上叶绿素超分子自组装的关键驱动力。实验结果得到了密度泛函理论计算的有力支持，表明叶绿素和化学还原的氧化石墨烯之间存在强有力的电子耦合。
Solvent plays an important role in the surface interaction of molecules. In this study, we use "chlorophyll a", an archetypical molecule, to investigate its supramolecular self-assembly with chemically reduced graphene oxide in three different types of solvents: polar protic, polar aprotic, and non-polar. It was observed that only a polar protic solvent that can donate protons facilitates the hydrogen bonding between chlorophyll a and chemically reduced graphene oxide nanosheets in a hybrid system. The formation of hydrogen bonds further initiates the other non-covalent interactions such as π-π stacking and hydrophobic interaction, which altogether play a key driving force for supramolecular self-assembly of chlorophylls on chemically reduced graphene oxides. The experimental results are strongly supported by density functional theory calculations, which show robust electron coupling between chlorophylls and chemically reduced graphene oxide.