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Rigidity and Flexibility: Unraveling the Role of Fulvic Acid in Uranyl Sorption on Graphene Oxide Using Molecular Dynamics Simulations
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-07-03 , DOI: 10.1021/acs.est.3c01026
Tu Lan 1 , Peng Wu 1 , Xiaoyu Yin 1 , Yufan Zhao 1 , Jiali Liao 1 , Dongqi Wang 2 , Ning Liu 1
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-07-03 , DOI: 10.1021/acs.est.3c01026
Tu Lan 1 , Peng Wu 1 , Xiaoyu Yin 1 , Yufan Zhao 1 , Jiali Liao 1 , Dongqi Wang 2 , Ning Liu 1
Affiliation
Using molecular dynamics simulations, this work targets a molecular understanding on the rigidity and flexibility of fulvic acid (FA) in uranyl sorption on graphene oxide (GO). The simulations demonstrated that both rigid Wang’s FA (WFA) and flexible Suwannee River FA (SRFA) can provide multiple sites to cooperate with GO for uranyl sorption and act as “bridges” to connect uranyl and GO to form GO–FA–U (type B) ternary surface complexes. The presence of flexible SRFA was more beneficial to uranyl sorption on GO. The interactions of WFA and SRFA with uranyl were primarily driven by electrostatics, and the electrostatic interaction of SRFA–uranyl was significantly stronger owing to the formation of more complexes. The flexible SRFA could markedly enhance the bonding strength of uranyl with GO by folding itself to provide more sites to coordinate with uranyl. The rigid WFAs tended to be adsorbed on the GO surface in parallel due to π–π interactions, whereas the flexible SRFAs took more slant configurations resulting from intermolecular hydrogen bonds. This work provides new insights into the sorption dynamics, structure, and mechanism and addresses the effect of molecular rigidity and flexibility, with great significance for FA-based remediation strategies of uranium-contaminated sites.
中文翻译:
刚性和灵活性:利用分子动力学模拟揭示黄腐酸在氧化石墨烯吸附铀酰中的作用
这项工作利用分子动力学模拟,旨在从分子角度理解黄腐酸 (FA) 在氧化石墨烯 (GO) 上吸附铀酰时的刚性和灵活性。模拟结果表明,刚性Wang's FA(WFA)和柔性Suwannee River FA(SRFA)都可以提供多个位点与GO配合进行铀酰吸附,并充当连接铀酰和GO的“桥梁”,形成GO–FA–U(类型B) 三元表面配合物。柔性SRFA的存在更有利于GO上铀酰的吸附。WFA和SRFA与铀酰的相互作用主要由静电驱动,并且由于形成更多络合物,SRFA-铀酰的静电相互作用明显更强。柔性SRFA可以通过自身折叠提供更多与铀酰配位的位点,从而显着增强铀酰与GO的键合强度。由于π-π相互作用,刚性WFA倾向于平行吸附在GO表面,而柔性SRFA由于分子间氢键而采取更多倾斜构型。这项工作为吸附动力学、结构和机制提供了新的见解,并解决了分子刚性和柔性的影响,对于基于 FA 的铀污染场地修复策略具有重要意义。
更新日期:2023-07-03
中文翻译:
刚性和灵活性:利用分子动力学模拟揭示黄腐酸在氧化石墨烯吸附铀酰中的作用
这项工作利用分子动力学模拟,旨在从分子角度理解黄腐酸 (FA) 在氧化石墨烯 (GO) 上吸附铀酰时的刚性和灵活性。模拟结果表明,刚性Wang's FA(WFA)和柔性Suwannee River FA(SRFA)都可以提供多个位点与GO配合进行铀酰吸附,并充当连接铀酰和GO的“桥梁”,形成GO–FA–U(类型B) 三元表面配合物。柔性SRFA的存在更有利于GO上铀酰的吸附。WFA和SRFA与铀酰的相互作用主要由静电驱动,并且由于形成更多络合物,SRFA-铀酰的静电相互作用明显更强。柔性SRFA可以通过自身折叠提供更多与铀酰配位的位点,从而显着增强铀酰与GO的键合强度。由于π-π相互作用,刚性WFA倾向于平行吸附在GO表面,而柔性SRFA由于分子间氢键而采取更多倾斜构型。这项工作为吸附动力学、结构和机制提供了新的见解,并解决了分子刚性和柔性的影响,对于基于 FA 的铀污染场地修复策略具有重要意义。