文献类型： 外文期刊

作者： Li, Guo-Bi ¹ ; Chen, Jing ¹ ; Song, Bai-Qiao ² ; Zhang, Xin ³ ; Zhang, Zhong ⁴ ; Pan, Rong-Kai ¹ ; Pei, Ling-Min ⁵ ; Liao, Lu-Sheng ⁶ ; Guan, Guo-Wei ³ ; Wang, Jian ⁷ ; Liu, Sheng-Gui ¹ ; Yang, Qing-Yuan ³ ;

作者机构： 1.Lingnan Normal Univ, Sch Chem & Chem Engn, Zhanjiang 524048, Peoples R China

2.Univ Limerick, Bernal Inst, Dept Chem Sci, Limerick, Ireland

3.Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian 710049, Peoples R China

4.Northwest A&F Univ, Coll Sci, Yangling 712100, Shaanxi, Peoples R China

5.Xizang Minzu Univ, Sch Basic Med, Xianyang 712082, Peoples R China

6.Minist Agr & Rural Affairs, Key Lab Trop Crop Prod Proc, Chinese Acad Trop Agr Sci, Agr Prod Proc Res Inst, Zhanjiang 524001, Guangdong, Peoples R China

7.China Tobacco Anhui Ind Co Ltd, Key Lab Combust & Pyrolysis, Hefei 230088, Anhui, Peoples R China

关键词： Naphthalene diimide; Ethanol-trapping adsorbent; Ethanol/water separation; Coordination networks; Metal-organic framework

期刊名称：SEPARATION AND PURIFICATION TECHNOLOGY （ 影响因子：9.136； 五年影响因子：8.258 ）

ISSN： 1383-5866

年卷期： 2022 年 293 卷

页码：

收录情况： SCI

摘要： Bioethanol is an essential energy source and is produced from agricultural feedstocks. However, raw bioethanol contains much water and methanol, and the traditional distillation approach has hardly removed it. Adsorptive separation of ethanol from water and methanol by adsorbents is an energy-efficient and promising method to produce fuel-grade ethanol. In this work, by regulating the pore surface in a new coordination network, [Cd(4-pmntd)(tpa)] (4-pmntd = N,N'-Bis(4-pyridymethy) naphthalene diimide; tpa = terephthalic acid), we target ultrahigh ethanol uptake and efficient ethanol/water separation, surpassing most benchmark materials. Explicitly, the ethanol uptake of Cd(4-pmntd)(tpa) (62.5 wt% at 100 kPa and 298 K) has the second-highest adsorption capacity among all the metal-organic frameworks (MOFs). In addition, Cd(4-pmntd)(tpa) gives ethanol/water selectivity of 32 toward a mixture of ethanol and water. Dynamic breakthrough measurements confirmed the excellent separation of ethanol and water. Under different ethanol/water ratios, Cd(4-pmntd)(tpa) extracts a low ethanol concentration from an ethanol/water mixture and produces ethanol in 99.1% purity in one step. Spectroscopic measurement and grand canonical Monte Carlo (GCMC) simulations provide critical insight into the adsorption/separation mechanism. The framework can form rich intermolecular C-H-guest...pi(host), C-H-guest...O-host and C-H-host...O(guest )interactions with ethanol molecules because of the suitable pore size and pore surface set in Cd(4-pmntd)(tpa). Thus, the adsorption enthalpies for ethanol in Cd(4-pmntd)(tpa) reached 66.16 kJ/mol, but only 29.44 kJ/mol and 49.21 kJ/mol for water and methanol, respectively. Moreover, the porous material exhibits good stability and can be easily combined with chitosan to form filter film, which is vital for potential industrial applications.