CAJ | 학술논문

众所周知,天然气作为一种利用效率高的清洁能源,其需求量正与日俱增。但天然气中包含的H2S等有害气体会危害人类健康、腐蚀设备、污染生态环境等。为解决这一问题,寻找良好的H2S吸附剂,本文采用巨正则系综蒙特卡罗(GCMC)模拟方法,针对天然气中H2S/CH4混合气分离,对33种具有代表性的稳定金属-有机骨架(MOF)材料进行 H2S 选择性和工作容量(变压吸附(PSA)及真空变压吸附(VSA)过程)的筛选。结果表明, ZIF-80, Zn2-bpydtc, CAU-1-(OH)2, CH3O-MOFa 最适用于本体系 VSA 过程的气体分离；而后两者最适用于PSA过程的气体分离。通过分析高选择性和高工作容量材料的结构特征,发现改性官能基团以及小孔作用的出现是影响选择性的关键因素,其中―Cl、―OH、―OCH3基团对H2S气体的吸附作用力最强。具有高的工作容量材料的特点是选择性高,对气体吸附作用力大,吸附位置多。基于筛选出的高选择性、高工作容量的稳定MOF材料总结出的强化H2S选择性及工作容量的一般性规律,为MOF材料应用于天然气脱硫提供了理论基础。
음소주지,천연기작위일충이용효솔고적청길능원,기수구량정여일구증。단천연기중포함적H2S등유해기체회위해인류건강、부식설비、오염생태배경등。위해결저일문제,심조량호적H2S흡부제,본문채용거정칙계종몽특잡라(GCMC)모의방법,침대천연기중H2S/CH4혼합기분리,대33충구유대표성적은정금속-유궤골가(MOF)재료진행 H2S 선택성화공작용량(변압흡부(PSA)급진공변압흡부(VSA)과정)적사선。결과표명, ZIF-80, Zn2-bpydtc, CAU-1-(OH)2, CH3O-MOFa 최괄용우본체계 VSA 과정적기체분리；이후량자최괄용우PSA과정적기체분리。통과분석고선택성화고공작용량재료적결구특정,발현개성관능기단이급소공작용적출현시영향선택성적관건인소,기중―Cl、―OH、―OCH3기단대H2S기체적흡부작용력최강。구유고적공작용량재료적특점시선택성고,대기체흡부작용력대,흡부위치다。기우사선출적고선택성、고공작용량적은정MOF재료총결출적강화H2S선택성급공작용량적일반성규률,위MOF재료응용우천연기탈류제공료이론기출。
Natural gas is a highly efficient energy source subject to growing demand. Natural gas contains H2S, which can harm human health and cause equipment corrosion and environmental pol ution. Effective H2S adsorbents are necessary to overcome these problems. Grand canonical Monte Carlo (GCMS) simulations were performed to study the selectivity and working capacity (pressure swing adsorption (PSA) and vacuum pressure swing adsorption (VSA) processes) of H2S in 33 kinds of stable metal-organic frameworks (MOFs), with the aim of separating H2S from H2S/CH4 gas mixture. ZIF-80, Zn2-bpydtc, CAU-1-(OH)2, and CH3O-MOFa were suitable materials for the VSA process. CAU-1-(OH)2 and CH3O-MOFa were suitable for the PSA process. The structures of materials exhibiting high selectivity and working capacity suggested that appropriate functionality and smal pore sizes were important for high selectivity. MOFs with ―Cl, ―OH, and ―OCH3 functionality exhibited the strongest adsorption. Materials exhibiting high selectivity, strong interaction with H2S, and large numbers of adsorption sites may have high working capacities. High selectivity and high working capacity stable MOFs were screened and analyzed, to enhance the selectivity and working capacity toward H2S. This provides a theoretical basis for separating H2S from natural gas using MOFs.