【摘要】 二氧化碳（CO₂）捕集是实现双碳目标的关键。本工作提出了一种四乙烯五胺（TEPA）功能化碳纳米纤维（CNFs）复合膜的制备工艺：结合溶液喷射纺丝（Solution blow spinning, SBS）和梯度碳化工艺制备出分级多孔CNFs骨架，并基于浸渍法利用TEPA溶液对CNFs骨架进行表面改性，成功构建了CNFs/TEPA复合膜。通过扫描电子显微镜（SEM）、傅里叶红外光谱仪（FTIR）、比表面积与孔径分析仪（BET）、热重分析仪（TGA）等表征手段探究了复合膜的比表面积、孔径分布以及CO₂吸附性能等关键参数。性能测试表明：CNFs/TEPA复合膜可有效协调TEPA的化学吸附机制与CNFs骨架的物理吸附特性，其吸附量符合“活性位点增益-结构损伤损耗”的竞争模型。当TEPA负载量为10%（质量分数）时，复合膜的吸附活性位点数量与比表面积、孔径达到平衡，在25℃、常压条件下的CO₂吸附容量可达2.41 mmol/g,较CNFs骨架提升了约10倍；此外，复合膜还展现出优异的选择吸附能力与可循环使用性能，分离因子高达30.125,且经15次吸脱附循环后仍能保持91%的初始吸附量，在CO₂捕集领域具有广阔的发展前景。更多还原

【Abstract】 Carbon dioxide（CO₂） capture is pivotal for achieving carbon neutrality goals. This work presents a novel fabrication process for tetraethylenepentamine（TEPA）-functionalized carbon nanofiber（CNFs） composite membranes: hierarchical porous CNFs skeletons were first prepared via solution blow spinning（SBS） combined with gradient carbonization, followed by surface modification using TEPA solution via impregnation to construct CNFs/TEPA composite membranes. Key properties including specific surface area, pore size distribution, and CO₂ adsorption perfor-mance were characterized using scanning electron microscopy（SEM）, Fourier transform infrared spectroscopy（FTIR）, Brunauer-Emmett-Teller（BET） surface area analysis, and thermogravimetric analysis（TGA）. Performance tests revealed that the CNFs/TEPA composite membranes effectively integrate TEPA’s chemical adsorption mechanism with the physical adsorption characteristics of CNFs skeletons, exhibiting an adsorption behavior following a "active site enhancement-structural damage loss" competitive model. At an optimal TEPA loading of 10%, the composite membrane achieved a balance between active site density and preserved pore structure（specific surface area and pore diameter）, demonstrating a CO₂ adsorption capacity of 2.41 mmol/g at 25 ℃ under atmospheric pressure—approximately 10 times higher than the pristine CNFs skeleton. Additionally, the composite membrane showed excellent selective adsorption capability with a separation factor of 30 and maintained 91% of its initial adsorption capacity after 15 adsorption-desorption cycles, highlighting its promising potential for practical CO₂ capture applications.更多还原