隨著全球氣候變遷與碳排放問題日益嚴重，開發永續且節能的碳捕捉技術非常重要。 薄膜的氣體分離技術，特別是混合基質薄膜，已被視為一種極具潛力的方法。然而，填 料與聚合物基質之間不良的介面相容性，以及高添加量下填料容易發生的嚴重團聚現象， 往往限制了 MMMs 克服傳統滲透率與選擇率權衡的潛力 。 為了解決這些限制，本研究提出了一種 2D/3D 混合填料策略，將 3D 的 UiO-66 NH2 奈米顆粒與 2D 的 MXene 奈米片結合至 PEBAX-2533 基質中，應用於 CO2/N2 分離。透過 XRD、FTIR 與 SEM 等材料特性分析，證實了各別填料的成功合成，以及 其後在聚合物基質中的均勻分散。此外，這些分析結果也驗證了 MOF 上的胺基與 MXene 表面的極性官能基能產生協同作用，改善介面相容性並共同提升對 CO2 的親和 力。3D 的 UiO-66-NH2 提供了互連的奈米通道以提升氣體滲透率，而 2D 的 MXene 奈米片則作為選擇性屏障，形成曲折的擴散路徑。 經由氣體分離實驗證實，製備的 MMMs 能在不同的填料比例中，有效平衡滲透率 與選擇率之間的權衡。具體來說， 10 wt% UiO-66-NH2/MXene 混合填料的 MMM 展現 了最優異的整體分離效率，達到了 393.18 Barrer 的 CO2 滲透率以及 32.18 的最佳 CO2/N2 選擇率。雖然單一填料或不同添加比例的薄膜可能達到更高的滲透率或選擇效 果，但往往會面臨嚴重的選擇率流失或填料團聚問題。10 wt% 的 2D/3D 混合系統成功 緩解了這些問題，超越了純 PEBAX 薄膜與其他測試比例的表現。在本研究中，二維 MXene 奈米片與三維 UiO-66-NH2 奈米顆粒的結合發揮了顯著的協同效應，進一步提 升了 MMMs 的 CO2 分離效率。最後，本研究為製備用於CO2 捕捉與純化的高效能混 合基質薄膜提供了一條新穎的途徑。;As global climate change and carbon emissions intensify， developing sustainable and energy-efficient carbon capture technologies is critical. Membrane-based gas separation， particularly mixed matrix membranes (MMMs)， has emerged as a promising approach. However， inadequate interfacial compatibility between the additives and the polymer matrix， along with the severe agglomeration of fillers at higher loadings， often restrict the potential of MMMs to overcome the traditional permeability-selectivity trade-off. To address these limitations， this study proposes a 2D/3D hybrid filler strategy by integrating 3D metal-organic frameworks (MOFs) nanoparticles and 2D MXene (Ti3C2Tx) nanosheets into a PEBAX-2533 matrix for CO2/N2 separation. Material characterization techniques， including XRD， FTIR， and SEM， confirmed the successful synthesis of the individual nanofillers and their subsequent uniform dispersion within the polymer matrix. Additionally， these analytical results verified that the presence of amino groups on the MOF and polar surface functional groups on MXene synergistically improved interfacial compatibility and enhanced CO2 affinity. The 3D UiO-66-NH2 provides interconnected nanochannels that boost gas permeability， while the 2D MXene nanosheets act as selective barriers to form a tortuous diffusion path. Gas separation experiments demonstrated that the as-prepared MMMs effectively balance the permeability-selectivity trade-off across various filler loadings. Specifically， the MMM incorporating an optimal 10 wt% of the UiO-66-NH2/MXene hybrid filler exhibited the most outstanding overall separation efficiency， achieving a CO2 permeability of 393.18 Barrer and an optimal CO2/N2 selectivity of 32.18. While single-filler membranes or those with different loading percentages could achieve high permeability or basic gas separation， they often suffered from significant selectivity loss or filler agglomeration. The 10 wt% 2D/3D hybrid system successfully mitigated these issues， surpassing the separation performance of the pure PEBAX membrane and other tested ratios. In this study， the combination of 2D MXene nanosheets and 3D UiO-66-NH2 nanoparticles exerted a remarkable synergistic effect in further improving the CO2 separation efficiency of the MMMs. Ultimately， this research provides a novel route for fabricating high-performance mixed matrix membranes for advanced CO2 capture and purification.
