在“双碳”政策下，高效CO₂捕集剂的开发与设计对于实现碳中和战略目标具有至关重要的意义。矿物资源开发与利用一直是我国经济建设的重点内容，廉价、储量丰富且可塑性高的黏土矿物在CO₂捕集材料的制备中扮演着重要角色。然而目前单一状态CO₂捕集材料（液体吸收材料或者固体吸附材料）难以满足高效低耗捕集CO₂的要求。因此，本文基于阴离子黏土矿物-水滑石（LDH）材料结构的灵活可调性，通过控制LDH的层片厚度、三维结构和生长方式，依据“理论指导-应用探索-结构优化-性能提升-机理阐明”的思路，构筑了利于CO₂传质的LDH基纳米流体，克服了单一状态捕集剂的限制，为新型高效黏土矿物基CO₂捕集剂的开发与设计提供了思路。

通过将有机低聚物接枝到LDH纳米片（LDH-NS）表面制备了LDH-NS基纳米流体（LNS-F）。与传统纳米流体相比，LNS-F在室温且无溶剂条件下表现出宏观流动行为，并且在不同有机溶剂中表现出优异的分散稳定性。通过改变LDH的金属组成、有机低聚物种类和黏土矿物种类，证实了有机低聚物接枝可以作为一种通用方法制备黏土矿物基纳米流体。通过分子动力学与量子化学模拟，查明了LDH与有机低聚物通过脱水缩合发生共价作用而相互结合，为后续LDH基纳米流体的结构优化提供了基础。

对LNS-F作为CO₂捕集材料的性能进行了探索。LNS-F具有较低的黏度（30 °C时粘度为6.60 Pa·s）有利于其在实际应用过程中的输送和CO₂传质。LNS-F-M2070在25 °C下10 bar和30 bar压力时，CO₂捕集量分别为0.48 mmol/g和1.37 mmol/g。由于有机液相对CO₂和N₂的溶解度不同，LNS-F-M2070表现出优异的CO₂/N₂分离选择性。由于纳米颗粒的存在增强了LNS-F捕集CO₂过程中的物理吸附作用，改善了纳米流体的循环再生能力，通过真空脱附循环再生8次后CO₂捕集量保持了最高捕集量的80%。

通过奥斯特瓦尔德反应设计合成了具有丰富暴露-OH的纳米花状LDH（NFL），进而与有机低聚物通过脱水缩合制备了NFL基纳米流体（NFL-F），改善了LNS-F接枝位点不足和捕集性能较差的缺点，探明了接枝密度与纳米流体的黏度及其CO₂捕集性能之间的构效关系。研究表明OS-M2070在NFL表面的高饱和接枝密度增加了纳米颗粒的位阻效应，降低了其黏度（NFL-F3在25 °C时的黏度为3.69 Pa·s），并且提高了NFL-F3的分散稳定性。随着接枝密度的增加，NFL-F3的CO₂捕集性能显著提高（在10 bar和25 °C测试条件下捕集量为1.44 mmol/g），这主要归功于有机低聚物之间的空隙、物理吸附作用以及NFL-F3表面高饱和接枝所带来的良好流动性。此外，NFL-F3具有良好的CO₂/N₂分离选择性和循环稳定性（在循环再生12次后CO₂捕集量保持了最高捕集量的86%）。

（4）为了提高反应效率和增强纳米流体结构中纳米颗粒LDH对CO₂的捕集容量，在NFL表面暴露了大量接枝位点的基础上，利用静电自组装方法在NFL内部构建介孔SiO₂，制备了核壳结构的SiO₂@LDH。利用离子液体代替有机低聚物制备了SiO₂@LDH-离子液体体系的纳米流体（SLDH-2-2h-10%BF₄），其黏度显著降低了（25 °C下黏度为0.12 Pa·s）。LDH表面丰富的-OH和有机液相之间的氢键相互作用增强了二者之间的溶解效应，保持了优异的分散稳定性。LDH-NS在介孔SiO₂表面作为一层“保护壳”，阻碍了离子液体占据介孔SiO₂的孔隙，提升了SLDH-2-2h-10%BF₄的CO₂捕集性能，在10 bar和25 °C条件下CO₂捕集量为1.52 mmol/g；同时提高了LDH基纳米流体捕集CO₂的循环稳定性能，在经过10个周期后，捕集量保持在最高捕集量的97%，为LDH基纳米流体捕集CO₂的工业应用提供了可能。

（5）LDH基纳米流体的结构（包括纳米颗粒和有机液相）对CO₂捕集性能具有重要影响。研究了LDH基纳米流体的结构优化对CO₂捕集行为和捕集性能的影响机制，阐明了纳米流体中纳米颗粒与有机液相对CO₂捕集的协同强化作用，结合分子模拟方法提出了LDH基纳米流体对CO₂的捕集机理。通过等温吸附模型拟合，确定了LDH基纳米流体捕集CO₂是化学作用和物理作用共同影响的，其中物理作用占主导；通过吸附动力学模型拟合证实了CO₂是先溶解在纳米流体的有机液相中，然后与有机液相中的作用位点相互作用，最后扩散到核心LDH结构中；利用分子模拟结果表明了LDH基纳米流体捕集CO₂的作用位点，包括有机液相中长链之间的空隙、有机液相中的作用位点（醚键和胺基）和无机纳米颗粒LDH本身。

基于对LDH基纳米流体的结构优化，实现了其优异的流动性能和分散性能，解决了固体LDH在应用过程中的团聚问题，所开发的LDH基纳米流体对CO₂具有较高的捕集性能、CO₂/N₂选择性能和优异的循环再生能力。LDH基纳米流体在CO₂捕集过程中，避免了传统液体吸收剂在高温脱附过程中对设备的腐蚀和高能量消耗，也解决了传统固体吸附剂吸附容量和分离选择性难以兼顾的问题，为高效低耗的黏土矿物基CO₂捕集材料的开发与设计提供了新的思路。

Under the "carbon peaking and carbon neutrality" policy, the development and design of efficient CO₂ capture agents hold crucial significance for achieving the strategic goal of carbon neutrality. The development and utilization of mineral resources have always been the focal points of China's economic construction, and clay minerals, which are inexpensive, abundant in reserves, and highly plastic, play a significant role in the preparation of CO₂ capture materials. Currently, single-state CO₂ capture materials (liquid absorption materials or solid adsorption materials) are insufficient to meet the requirements for efficient and low-cost CO₂ capture. Consequently, leveraging the flexible adjustability of the anionic clay mineral-layered double hydroxide (LDH) material structure, this study endeavors to construct LDH-based nanofluids that facilitate CO₂ mass transfer by meticulously controlling the layer thickness, three-dimensional structure, and growth mode of LDH. Adhering to the framework of "theoretical guidance, structural optimization, performance enhancement, and mechanism elucidation", this approach overcomes the limitations of single-state adsorbents and offers a insight for the development and design of novel, efficient mineral-based CO₂ capture agents.

LDH-NS-based nanofluids (LNS-F) were prepared by grafting organic oligomers onto the surface of LDH nanosheets (LDH-NS). Compared with traditional nanofluids, LNS-F exhibited macroscopic flow behavior at room temperature without solvents and demonstrated higher dispersion stability in various organic solvents. The grafting of organic oligomers was validated as a versatile method for the preparation of clay mineral-based nanofluids through alterations in the metal composition of LDH, types of organic oligomers, and clay varieties. Molecular dynamics simulations and quantum simulations revealed that LDH and organic oligomers covalently interact through dehydration condensation, providing a foundation for the subsequent structural optimization of LDH-based nanofluids.

The application performance of LNS-F as a CO₂ capture material was explored. LNS-F exhibited a lower viscosity (6.60 Pa·s at 30 °C), favoring its transportation and CO₂ mass transfer during practical applications. At 25 °C, LNS-F-M2070 demonstrated CO₂ capacities of 0.48 mmol/g and 1.37 mmol/g under pressures of 10 bar and 30 bar, respectively. Due to the different solubilities of organic liquids for CO₂ and N₂, LNS-F-M2070 exhibited an excellent CO₂/N₂ selectivity. The presence of nanoparticles enhanced physical interactions, favoring the cyclic stability of the nanofluid. After eight cycles of regeneration through vacuum desorption, the CO₂ capacity retained 80% of the maximum capacity.

Through the Ostwald ripening reaction, nanoflower-like LDH (NFL) with abundant exposed -OH groups were designed and synthesized. Subsequently, NFL-based nanofluids (NFL-F) were prepared by dehydration condensation with organic oligomers, addressing the limitations of insufficient grafting sites and poor CO₂ capacity in LNS-F. The study elucidated the structure-activity relationship between the grafting density, viscosity, and CO₂ capacity of the nanofluids. It was found that the high saturation grafting density on the surface of NFL increased the steric hindrance effect of the nanoparticles, resulting in reduced viscosity (3.69 Pa·s at 25 °C) and improved dispersion stability of NFL-F3. Notably, as the grafting density increased, the CO₂ capacity of NFL-F3 significantly improved (2.27 mmol/g at 15 bar and 25 °C), primarily attributed to the gaps between organic oligomers, physical adsorption, and the excellent fluidity conferred by the high saturation grafting of organic oligomers. Additionally, NFL-F3 exhibited an excellent CO₂/N₂ separation performance and cyclic stability, maintaining 86% of its maximum CO₂ capacity after 12 cycles of regeneration.

To enhance the reaction efficiency and boost the CO₂ capacity of the core LDH within the nanofluid, a mesoporous SiO₂ was constructed at the center of the nanoflower-like LDH using the electrostatic self-assembly method, resulting in a core-shell SiO₂@LDH while maintaining the exposure of numerous grafting sites. Furthermore, a nanofluid based on the SiO₂@LDH-ionic liquid system (SLDH-2-2h-10%BF₄) was prepared by replacing organic oligomers with ionic liquids, significantly reducing its viscosity (0.12 Pa·s at 25 °C). The strong hydrogen bonding interaction between the abundant -OH groups on the LDH surface and the sterically hindered solvent enhanced the dissolution effect, maintaining excellent dispersion stability. The LDH-NS served as a protective shell on the surface of the mesoporous SiO₂, preventing the ionic liquid from occupying the pores of the SiO₂ and enhancing the CO₂ capacity of SLDH-2-2h-10%BF₄. Under conditions of 15 bar and 25 °C, the CO₂ capacity reached 1.51 mmol/g. Additionally, the cyclic stability of the LDH-based nanofluids was improved, maintaining 97% of its maximum capacity after 10 cycles, providing a promising avenue for the industrial application of LDH-based nanofluids in CO₂ capture.

The structure of LDH-based nanofluids, encompassing both nanoparticles and organic liquid phases, holds significant implications for their CO₂ capacity. This study investigated the impact of structural optimization in LDH-based nanofluids on the mechanisms underlying CO₂ capture behavior and performance. The synergistic enhancement effects of nanoparticles and organic liquids on CO₂ capture within the nanofluid were elucidated. Furthermore, a capture mechanism for CO₂ in LDH-based nanofluids was proposed, incorporating molecular simulation methods. By fitting the isothermal adsorption model, it was determined that the adsorption of CO₂ by LDH-based nanofluids was influenced by both chemical and physical interactions, with physical interactions playing a dominant role. The adsorption kinetics model fitting confirmed that CO₂ first dissolves in the organic liquid phase of the nanofluids, interacts with the functional sites within the organic liquid phase, and then diffuses into the core LDH structure. Molecular simulation results revealed the interaction sites between the LDH-based nanofluids and CO₂ molecules, including the gaps between long chains in the organic liquid phase, functional sites in the organic liquid phase (ether bonds and amine groups), and the inorganic solid phase of LDH itself.

Through structural optimization of LDH-based nanofluids, this study achieved excellent flow and dispersion properties, addressing the aggregation issues encountered during the application of solid LDH. The developed LDH-based nanofluids adsorption material exhibits high CO₂ capture performance, superior CO₂/N₂ selectivity, and excellent regeneration capability. As a CO₂ capture material, LDH-based nanofluids eliminate the issues of equipment corrosion and high energy consumption associated with traditional liquid materials during desorption at high temperatures. Simultaneously, they overcome the problems of wear and mechanical fatigue encountered with traditional solid adsorbents during application. The LDH-based nanofluids designed and synthesized in this study provides a promising avenue for the development of efficient and low-consumption CO₂ capture materials.

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