为了应对二氧化碳排放引起的全球变暖、海平面上升等严重气候问题，二氧化碳的转化、捕获和分离受到广泛关注。CO₂的微孔填充机理，需要多孔材料具有较高的微孔比表面积或孔尺寸接近吸附质分子的动力学直径使其具有分子筛效应从而提高二氧化碳吸附量和选择性。此外，各种杂原子，例如氮，氧，硫，磷和硼等引入碳骨架中提升材料的四极矩和极性也可以增强CO₂的吸附和选择性。然而，直接改变多孔材料的结构、将不同杂原子掺杂进去是非常具有挑战的任务。因此，我们通过选取富含大量官能团的氧化石墨烯（GO）为操作平台，对GO进行功能化或非功能化改性从而达到引进其他杂原子或者改善多孔材料结构的目的。   

首先，采用管式炉化学活化法，以半焦（SC）为碳前驱体，以不同质量比的石墨粉为原料，制备了碘吸附值为1223.99 mg·g^-1和比表面积为1072.08 m²·g^-1的石墨烯基多孔碳材料。通过傅里叶红外光谱对其结构的官能团变化进行了分析，拉曼光谱分析揭示了石墨碳和无定形碳之间的变化情况，X射线衍射分析得出石墨烯基多孔碳的低角度散射增加表明孔结构的变化，静态吸附测试得出二氧化碳吸附量为5.39 mmol·g^-1（298 K, 30 bar），通过IAST模型预测了烟气成分（CO₂/N₂=15/85 vol%）下半焦石墨烯比为300:1的石墨烯基半焦多孔碳在1 bar和298 K下的CO₂/N₂选择性为28.64。

为了更进一步的提高二氧化碳的吸附量和选择性，我们提出了一种新的策略来设计和生产石墨烯基半焦多孔碳，这种多孔碳材料是富氮的层状三明治结构。共价功能化是通过SC和GO与乙二胺（EDA）的缩合和亲核取代实现的。采用合适的吸附等温线模型对CO₂的平衡吸附量进行了测定和分析。通过改变GO与SC的质量比，研究了GO含量对CO₂吸收的影响。富氮层状三明治结构的石墨烯基半焦多孔碳具有高比表面积（701.53 m²·g^-1）和大量以0.8~2.0 nm为中心的微孔结构，新合成的多孔碳材料不仅在吸附容量（7.11 mmol∙g^-1，298 K）上有所提高，而且在选择性（34.25）方面具有优异的性能。

最后，通过4,4′-氧代二苯二甲酸酐（ODPA）、2,4,6-三甲基-1,3-苯二胺（DAM）、UiO-66-NH₂和GO的化学原位编织，制备了新型多孔超交联聚酰亚胺-UiO-石墨烯复合吸附剂。在UiO-66-NH₂/GO中加入了一种富含氮和氧的聚酰亚胺（PIs）聚合物，其末端带有-NH₂基团，并且其含有的超微孔可以提供CO₂亲和力。PI-UiO/GOs具有优异的耐酸碱性能、适宜的吸附热和优异的循环稳定性，说明该复合多孔材料具有优异的循环利用能力，为吸附剂在复杂工业环境中的应用提供了多种可能性。在298 K和1 bar下，PI-UiO/GO-1在烟气中的CO₂穿透时间达到369 s，所得材料（PI-UiO/GO-1）的CO₂容量约为原始UiO-66-NH₂的3倍（298 K和30 bar时为8.24 vs 2.8 mmol·g^-1），CO₂/N₂选择性高出4.2倍（64.71 vs 15.43）。突破时间和吸附容量的提高证明了该策略的适用性。这一合成方法对设计新型的二氧化碳捕集和烟气分离材料有一定的指导意义。

To deal with the global warming, sea level rise and other serious climate problems caused by CO₂ emissions, the conversion, capture and separation of CO₂ have been widely concerned. On the one hand, the micropore filling mechanism of CO₂ requires that porous materials with high micropore specific surface area or close to the size of adsorbate molecules will have molecular sieve effect, so as to improve the adsorption capacity and selectivity of CO₂. In addition, various heteroatoms (such as nitrogen, oxygen, sulfur, phosphorus and boron) are introduced into the carbon skeleton to enhance the quadrupole moment and polarity of the materials, which can also enhance the CO₂ adsorption and selectivity. However, it is a challenging task to directly change the structure of porous materials and dope different heteroatoms. Therefore, we select graphene oxide (GO) rich in a large number of functional groups as the operating platform to carry out functional or non functional modification of GO, so as to introduce other heteroatoms or improve the structure of porous materials.

Firstly, the porous carbon materials with iodine adsorption value of 1223.99 mg·g^-1 and specific surface area of 1072.08 m²·g^-1 were prepared by tubular furnace chemical activation method using semi-coke (SC) as carbon precursor and GO with different mass ratios as raw materials. Fourier transform infrared spectroscopy (FTIR) was used to analyze the change of functional groups in the structure. Raman spectroscopy revealed the change between graphite carbon and amorphous carbon. X-ray diffraction analysis showed that the increase of low angle scattering of graphene based porous carbon indicated the change of pore structure. Static adsorption test showed that the adsorption capacity of CO₂ was 5.39 mmol·g^-1 (298 K, 30 bar). The IAST model predicts that the CO₂/N₂ selectivity of graphene-based porous carbon with 300:1 SC to GO ratio at 1 bar and 298 K is 28.64 at the flue gas composition (CO₂/N₂=15/85 vol%).

To further improve the adsorption capacity and selectivity of CO₂, we proposed a new strategy to design and produce graphene-based semi-coke porous carbons with N-rich layered sandwich structure. Covalent functionalization is achieved by condensation and nucleophilic substitution of SC and GO with ethylenediamine (EDA). An appropriate adsorption isotherm model was used to measure and analyze the equilibrium adsorption capacity of CO₂. The effect of GO content on CO₂ absorption was studied by changing the mass ratio of GO to SC. Graphene-based semi-coke porous carbon with N-rich layered sandwich structure has high specific surface area (701.53 m²·g^-1) and a large number of micropores centered at 0.8-2.0 nm. The most obvious is that the synthesized porous carbon materials not only improve the adsorption capacity (7.11 mmol·g^-1, 298 K), but also have excellent selectivity (34.25).

Finally, a novel porous hyper-cross-linked polyimide-UiO-graphene composite adsorbent was prepared by chemical in-situ braiding of 4,4′-oxodiphthalic anhydride (ODPA), 2,4,6-trimethyl-1,3-phenylenediamine (DAM), UiO-66-NH₂ and GO. A polyimide (PIs) rich in nitrogen and oxides was added to UiO-66-NH₂/GO with -NH₂ group at the end, and the supermicropores could provide enhanced CO₂ affinity. PI-UiO/GO has excellent acid-base resistance, suitable adsorption heat and excellent cycling stability, which indicates that the composite porous material has excellent recycling ability, which provides a variety of possibilities for the application of adsorbent in complex industrial environment. Under 298 K and 1 bar, the breakthrough time of PI-UiO/GO-1 in flue gas reaches 369 s. As expected, the resulting composite (PI-UiO/GO-1) exhibited a three-fold CO₂ capacity (8.24 vs 2.8 mmol·g^-1 at 298 K and 30 bar), 4.2 times higher CO₂/N₂ selectivity (64.71 vs 15.43), and significantly improved acid-base resistance stability compared with those values of pristine UiO-66-NH_2. The improvement of breakthrough time and adsorption capacity proved the applicability of the strategy. This synthesis method has a certain guiding significance for the design of new CO₂ capture and flue gas separation materials.

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