Hydrated cation–π interactions of π-electrons with hydrated Li+, Na+, and K+ cations

Mu, Liuhua; Yang, Yizhou; Liu, Jian; Du, Wei; Chen, Jige; Shi, Guosheng; Fang, Haiping

doi:10.1039/d1cp01609a

Cited by 26 publications

(16 citation statements)

References 69 publications

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“…The loci of oxidized groups on GO sheets comes from our previous paper. 37,38 The electron wave functions in the Gaussian function basis were employed. Geometry optimizations for the adsorption structures of each system were at the B3LYP/6-31G(d)/Lan2dz level.…”

Section: Methodsmentioning

confidence: 99%

“…We have also performed DFT calculations for hydration energy of these cations, as the comparison of the feasibility for hydrated ions dehydrating. The loci of oxidized groups on GO sheets comes from our previous paper. , The electron wave functions in the Gaussian function basis were employed. Geometry optimizations for the adsorption structures of each system were at the B3LYP/6-31G(d)/Lan2dz level.…”

Section: Methodsmentioning

confidence: 99%

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Enhanced Separation Performance of Radioactive Cesium and Cobalt in Graphene Oxide Membrane via Cationic Control

Wang

Yang

et al. 2022

Langmuir

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The great applications of nuclear power for the most promising clean energy sources have been challenged by a large amount of radioactive wastewater generated, specifically the Cs + /Co 2+ separation for nuclear waste storage, retreatment or recycling of radioactive wastewater, because of their wide difference in half-life and high heat release. In this work, graphene oxide membranes (GOMs) with interlayer spacing controlled by cations were used to separate mixed Cs + /Co 2+ ions. The separation factors of Cs + /Co 2+ for K + -controlled graphene oxide membranes (K-GOMs) was 2∼3 times higher than that of GOMs without treatment. In addition, the separation factors of Cs + /Co 2+ for K-GOMs can be further enhanced with the increase of membranes thickness and change the initial ratios of the two ions. Typically, the separation factors of K-GOMs with a thickness of ∼300 nm reached up to 73.7 ± 3.9. Moreover, the K-GOM showed outstanding stability of the separation performance under long-term operation within 7 days. First-principles calculation revealed that the enhanced ionic selectivity of controlled GOM is induced by the difference of adsorption energies between the hydrated cations and aromatic rings, resulting in a significant increase in the mobility differences between Cs + and Co 2+ through a fixed narrow interlayer spacing. This study demonstrated excellent separation performances of GO-based membranes based on their size-exclusion effect rather than electrostatic repulsion effect, and we believe this work can enable potential efficient treatment technologies for radioactive wastewater needed urgently.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Enhanced Separation Performance of Radioactive Cesium and Cobalt in Graphene Oxide Membrane via Cationic Control

Wang

Yang

et al. 2022

Langmuir

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“…In solution, the hydration shell of a cation dramatically reduces its cation−π interaction with a carbon-based surface, , especially when the surface matter contains only a single or a few aromatic rings. For example, the cation−π interaction (calculated by the adsorption energy) between a single Na + cation and a benzene molecule decreases from −23.1 kcal/mol in the gas phase to about −6.2 kcal/mol in aqueous solution .…”

Section: Remarkable Statistical Effect Accumulated By Hydrated Cation...mentioning

confidence: 99%

“…The radii of hydrated cations decreased in the order Mg 2+ aq > Ca 2+ aq > Li + aq > Na + aq > K + aq , which, except for Li + , are consistent with experimental observations in literature. 28 This exception can be attribute to the weaker hydrated cation−π interaction of hydrated Li + compared with the other four kinds of hydrated cations, 28,40 which caused the connection to be more frequently interrupted. As a result, the percentage time during which GOMs are connected by Li + is lower than the other four cations.…”

Section: Statistical and Precise Control Of Gom Interlayer Spacing By...mentioning

confidence: 99%

Revisit the Hydrated Cation−π Interaction at the Interface: A New View of Dynamics and Statistics

Yang

Liang

et al. 2022

Langmuir

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Carbon-based matter, such as biomolecules and graphitic structures, often form a liquid–solid/soft matter interface in salt solution and continuously affect the surrounding cations through hydrated cation−π interactions. In this Perspective, we revisit the effect of the hydrated cation−π interactions at the interface using statistical physics, which reveals how hydrated cation−π interactions affect every component dynamically and cause a time-dependent statistical effect at the liquid–solid/soft interface. We also highlight several pieces of experimental evidence from a statistical perspective and discuss the remarkable applications related to environmental protection, industrial manufacturing, and biological sciences.

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“…Ab initio molecular dynamics (AIMD) simulation can describe the interfacial evolution at an electronic level, where the atomic nuclei are propagated by the Newtonian equation of motion based on forces obtained from the ab initio electronic structure theory. Therefore, AIMD has a simulated temperature comparable to the experimental temperature, and it has been used to analyze interface phenomena and clarify the solvation structure and ion diffusivity at various interfaces. − Hence, Na + -ion behaviors inside nanochannels can be well understood using tools like AIMD simulations.…”

Section: Introductionmentioning

confidence: 99%

Electronic-Level Insight into Interfacial Effects and Their Induced Anisotropic Ion Diffusion and Ion Selectivity in Nanochannels

Wang

Zhang

et al. 2022

ACS Appl. Mater. Interfaces

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Osmotic energy conversion features directional ion migration in selective nanochannels, dominated by interfacial effects, temperature, and concentration. Current efforts emphasize membrane modification for superior reliability and durability, whereas the origin and implication of interfacial effects are unclear. This work performs ab initio molecular dynamics simulations for hydrated ion–graphene oxide interfaces by regulating the temperature and concentration. The interfacial effects associated with their induced anisotropic ion diffusion and ion selectivity are revealed. The scientific essence of the interfacial effects is an electron transfer triggered by hydrated ion–functional group interactions. The interfacial effects are clarified to include dynamic solvation structures, interfacial H-bonds, and chemical reactions. Ions possess incomplete hydration shells, and their arrangements vary from ordered to disordered to overlapped. Interfacial H-bonds restrict hydrated ions by constraining water molecules, whereas continuous reactions provide lateral pathways to generate anisotropy. Cation selectivity is further clarified by negative surface charges from hydroxyl deprotonation. Besides, temperature rise induces disordered hydrated ions as well as frequent and violent reactions, enhancing ion diffusion, selectivity, and anisotropy; excessive concentrations produce overlapped hydrated ions, more H-bonds, and inferior reactions, weakening ion diffusion, selectivity, and anisotropy. Finally, the bottom-up concept for osmotic energy conversion is summarized, and elevated temperature combined with low concentration is found to boost ion diffusion and ion selectivity synergistically. This work provides an in-depth understanding of interfacial phenomena and ion behaviors in nanochannels.

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Hydrated cation–π interactions of π-electrons with hydrated Li⁺, Na⁺, and K⁺ cations

Abstract: Cation-π interactions are essential for many chemical, biological, and material processes, and these processes usually involve an aqueous salt solution. However, there is still a lack of a full understanding...

Cited by 26 publications

References 69 publications

Enhanced Separation Performance of Radioactive Cesium and Cobalt in Graphene Oxide Membrane via Cationic Control

Enhanced Separation Performance of Radioactive Cesium and Cobalt in Graphene Oxide Membrane via Cationic Control

Revisit the Hydrated Cation−π Interaction at the Interface: A New View of Dynamics and Statistics

Electronic-Level Insight into Interfacial Effects and Their Induced Anisotropic Ion Diffusion and Ion Selectivity in Nanochannels

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