甲烷可提供的能量大約是煤的兩倍，且於燃燒反應不會逸散劇毒的汞蒸氣與產生富含鈾和釷的灰燼。然而，甲烷如同二氧化碳作為溫室氣體的主要成分，為導致全球暖化之主因。甲烷與二氧化碳的吸附研究，對於捕獲和儲存這兩種分子至關重要。開發具捕獲和儲存應用價值的吸附劑，將得以充分利用清潔能源並防止污染與暖化的持續。

金屬有機框架(MOF)作為近年最流行的吸附劑選擇，提供極高的表面積、孔體積和與可調的多功能結構，其優異特性使其成為最具吸引力的儲氣應用材料之一。活性炭(AC)由不同的前體生產並基於低成本優勢，提供了大範圍的孔結構和表面化學，幾十年來亦廣泛應用於吸附劑領域。
由於填充床吸附系統具有壓降缺陷，粉末形式的MOF和AC於利用率較低。塊材吸附劑在壓降和傳質動力學方面優於傳統顆粒吸附劑。相較於傳統的密實化成型工藝，3D列印開拓新穎的製備方法，快速成型、低成本效益與高活性的優勢，使該技術更適合製備具有可調結構的塊材吸附劑。

本研究中嘗試了兩種塊材吸附劑的製備方法，即(1)全集成式 與 (2)吸附劑塗佈式 3D列印塊材吸附劑，並採用經優化設計的毫米級晶格作為3D列印架構。
對於氣體儲存應用，研究了甲烷與二氧化碳在具備不同MOF(或AC)附載量之塊材吸附劑的吸附/解吸與利用率。塊材吸附劑皆採用商用MOF和AC粉末進行製備，並對其物理和結構性能進行了特徵，包括氮氣等溫線、吸附參數、吸附容量和吸附動力學。亦研究了孔結構、溫度、壓力與單體比例對吸附和活化條件的影響。 成功開發的塊材吸附劑保留最高73 %的利用率、優異的氣體儲存容量與更快的吸附速率，達到ASTM 3B的吸附劑塗層附著力，且抗壓強度達到12 MPa。該研究結果將有助於設計有效的氣體儲存系統。

關鍵字：金屬有機框架材料(MOF); 活性碳; DLP 3D列印; 甲烷; 二氧化碳

Methane provides about twice as much energy as coal, which does not dissipate mercury or produce ashes rich in uranium and thorium. However, methane is one major component of greenhouse gases causing global warming. The adsorption of carbon dioxide and methane is important for trapping and storage of both molecules and therefore, the development of workable adsorbents is a key issue for the storage and sequestration of these gases in order to utilize clean energy and prevent continuation of air pollution.

Metal-organic frameworks (MOFs) are among the most popular selections for adsorbents, which can provide a very high surface area, high pore volume and tunable versatile structures. The superior characteristics of MOFs make them one of the most attractive materials for gas storage applications. Activated carbon (AC) is conventionally used as adsorbents due to its low-cost advantage, which can be produced from different precursors providing a large spectrum of pore structures and surface chemistry for wide application in adsorption for decades.

Both MOFs and AC in powder form may not be engineeringly suitable for adsorption application owing to the possibly large pressure drop in packed bed adsorption system. Monolithic adsorbents are superior to conventional pellet, both fabricated from powders, in terms of pressure drop and mass transfer kinetics. Comparing to traditional "shaping" processes, utilizing 3D printing technology may provide an alternative cost-effective and simple method to fabricate the monolithic adsorbent with tunable structural morphology.

In this study, we tried two preparation methods of monolithic adsorbents, namely (1) the all integrated adsorbent-based 3D printed structure, and (2) the adsorbent-coated 3D printed structure, for optimal design of millimeter-scale adsorbent “shape”. For gas storage application, we investigated the sorption properties of carbon dioxide and methane on various types of 3D-printed structures with different MOF (or AC) content, in short as 3D-printed MOF/AC. The 3D-printed MOF/AC is prepared from commercially available MOF/AC powders and their physical and structural properties were characterized. Carbon dioxide and methane adsorption/desorption on 3D-printed MOF/AC are examined, including isotherms, adsorption parameters, adsorption capacities, adsorption kinetics. The effects of pore structure, temperature, pressure on adsorption and activation conditions were also investigated.

The fabricated 3D-printed MOF/AC can have a utilization up to 73%, with an adsorbent-coated adhesion of at least ASTM 3B level and a compressive mechanical strength of 12 MPa. The results show that 3D-printed MOF/AC is stable, have an acceptable gas storage capacity and faster adsorption rate in high-pressure gas adsorption applications. The findings of the study would be useful in the design of effective gases storage systems

Keywords: Metal-organic frameworks (MOFs); Activated carbon; Carbon dioxide; Methane; 3D-printed MOFs

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