利用太陽能將空氣中的二氧化碳(CO2)光催化還原成有價值的化合物或能源，能達成能源永續應用並降低大氣中二氧化碳濃度解決全球暖化的問題。本研究設計了一種光催化複合薄膜，在模擬太陽光的光源下，同時將空氣中的CO2提濃並光催化還原成甲烷(CH4)。光催化複合薄膜為氣體選擇層和光催化反應層所組成，氣體選擇層為無缺陷的聚醯亞胺(Polyimide)緻密薄膜，其具有優秀的氣體選擇性，有效地從空氣中將CO2提濃；光催化反應層為含有光觸媒二氧化鈦(TiO2)的Polyimide多孔混合基質薄膜，反應層能將滲透的CO2光催化還原成CH4。
改善薄膜的光催化效率，除了可改良光觸媒的催化活性和提升氣體選擇層的CO2選擇性之外，亦可延長CO2於光催化反應層的滯留時間，增加CO2和TiO2的反應機會，提升CH4產率。本研究根據成膜機制的理論，利用霧點、黏度、光穿透及染色實驗，探討添加疏水性的界面活性劑和改變非溶劑對薄膜孔洞結構之影響。透過SEM、EDS、孔隙度、機械性質和氣體通量等實驗，鑑定不同薄膜之結構。GPA被用於分析光催化複合薄膜之CO2分離性能。選用封閉孔洞結構之多孔薄膜做為光催化反應層(20 wt% TiO2)，可以有效地延長CO2在反應層內的滯留時間，提升CH4產率至0.70 μmol gcat-1 h-1。最佳添加量的TiO2 (30 wt%)能在反應層中均勻分散且增加反應位點，得到1.17 μmol gcat-1 h-1的最佳CH4產率。複合薄膜經過連續七日的光催化反應後，CH4產率損失了82 %。
本研究成功結合成膜機制、氣體分離和光催化還原的技術，製備出一種能同時能將CO2提濃並還原成CH4的光催化複合薄膜，對於解決CO2排放的危機提供一個相當有潛力的方法。

The use of solar energy to photocatalyze the carbon dioxide in the air into valuable compounds or energy can achieve sustainable energy applications and solve the problem of global warming. In this work, a photocatalytic composite membrane was designed to simultaneously enrich and photocatalytically reduce CO2 in the air to CH4 under the simulating sunlight. The photocatalytic composite membrane is composed of a gas selective layer and a photocatalytic reactive layer. The gas selective layer is a defect-free polyimide dense membrane, which has excellent gas selectivity and can enrich CO2 from the air. The photocatalytic reactive layer is a polyimide porous mix-matrix membrane containing photocatalyst TiO2, which can photocatalytically reduce the permeated CO2 to CH4.
Improving the catalytic activity of the photocatalyst and increasing the CO2 flux and selectivity of the gas selective layer can improve the CO2 photocatalytic efficiency of the composite membrane. In addition, extending the residence time of CO2 in the photocatalytic reaction layer can increase the reaction opportunity of CO2 and TiO2 and then increase the yield of CH4. Based on the theory of membrane formation mechanism, the effects of adding hydrophobic surfactants and changing non-solvents on the pore structure of the membranes were investigated by cloud point, viscosity, light transmittance and optical observation experiments. Through SEM, EDS, porosity, mechanical properties and gas permeance, the structure of different membranes was identified. GPA was used to analyze the CO2 separation performance of the photocatalytic composite membranes. Selecting the porous membrane with closed pore structure as the photocatalytic reactive layer (20 wt% TiO2) can effectively prolong the residence time of CO2 in the reactive layer and get the CH4 yield of 0.70 μmol gcat-1 h-1. The optimal amount of TiO2 (30 wt%) can make the catalyst evenly dispersed in the reaction layer and increase the reaction sites, which obtains the best CH4 yield for 1.17 μmol gcat-1 h-1. After seven consecutive days of photocatalytic reaction, the CH4 yield decreased by 82 % of the photocatalytic composite membrane.
This work successfully combines the membrane formation mechanism, gas separation and photocatalytic reduction technology to prepare a photocatalytic composite membrane. The composite membrane can simultaneously enrich and photocatalytically reduce CO2 to CH4. This work provides a promising method for solving the CO2 emission problem.

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