{"title":"具有低极性孔隙环境的四核簇基 MOF 可实现 C2H6/C2H4 的高效分离","authors":"Meng Feng, Jiantang Li, Xirong Wang, Jingyu Wang, Dongmei Wang, Banglin Chen","doi":"10.1039/d4qi01685h","DOIUrl":null,"url":null,"abstract":"Removing trace ethane (C<small><sub>2</sub></small>H<small><sub>6</sub></small>) from ethylene (C<small><sub>2</sub></small>H<small><sub>4</sub></small>) to obtain high-purity C<small><sub>2</sub></small>H<small><sub>4</sub></small> is of great industrial significance. However, the construction of C<small><sub>2</sub></small>H<small><sub>6</sub></small>-selective metal-organic frameworks (MOFs) remains challenging, mainly because C<small><sub>2</sub></small>H<small><sub>4</sub></small> has a small dynamic diameter and a large quadrupole moment. It has been reported that ultramicroporous MOFs with tailored pore sizes and weakly polar pore environment can effectively purify C<small><sub>2</sub></small>H<small><sub>4</sub></small> from C<small><sub>2</sub></small>H<small><sub>6</sub></small>-C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixtures. For this purpose, we successfully designed and synthesized one novel MOF material ZJNU-400 with non-polar pore environment. The channel size of ZJNU-400 is equivalent to the size of the C<small><sub>2</sub></small>H<small><sub>6</sub></small> molecule, which can provide a more accessible channel surface for C<small><sub>2</sub></small>H<small><sub>6</sub></small>. The pore environment of ZJNU-400 is rich in low-polarity aromatic groups, and uncoordinated N and O atoms can interact strongly with C<small><sub>2</sub></small>H<small><sub>6</sub></small> molecules. Therefore, ZJNU-400 exhibits significant C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> (50/50) selectivity (2.82) and C<small><sub>2</sub></small>H<small><sub>6</sub></small> uptake (64.3 cm<small><sup>3</sup></small> g<small><sup>-1</sup></small>) at 298 K and 1 bar, which is superior to many C<small><sub>2</sub></small>H<small><sub>6</sub></small>-selective adsorbents. Breakthrough experiment shows that ZJNU-400 can purify C<small><sub>2</sub></small>H<small><sub>4</sub></small> from C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixture in one step. GCMC and DFT calculations further revealed that the multiple synergistic interactions between the MOF and C<small><sub>2</sub></small>H<small><sub>6</sub></small> enable efficient separation of the C<small><sub>2</sub></small>H<small><sub>6</sub></small>-C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixture. These results indicate that ZJNU-400 is a promising adsorbent for C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> separation.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":6.1000,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tetranuclear-cluster-based MOF with low-polar pore environment for efficient C2H6/C2H4 separation\",\"authors\":\"Meng Feng, Jiantang Li, Xirong Wang, Jingyu Wang, Dongmei Wang, Banglin Chen\",\"doi\":\"10.1039/d4qi01685h\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Removing trace ethane (C<small><sub>2</sub></small>H<small><sub>6</sub></small>) from ethylene (C<small><sub>2</sub></small>H<small><sub>4</sub></small>) to obtain high-purity C<small><sub>2</sub></small>H<small><sub>4</sub></small> is of great industrial significance. However, the construction of C<small><sub>2</sub></small>H<small><sub>6</sub></small>-selective metal-organic frameworks (MOFs) remains challenging, mainly because C<small><sub>2</sub></small>H<small><sub>4</sub></small> has a small dynamic diameter and a large quadrupole moment. It has been reported that ultramicroporous MOFs with tailored pore sizes and weakly polar pore environment can effectively purify C<small><sub>2</sub></small>H<small><sub>4</sub></small> from C<small><sub>2</sub></small>H<small><sub>6</sub></small>-C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixtures. For this purpose, we successfully designed and synthesized one novel MOF material ZJNU-400 with non-polar pore environment. The channel size of ZJNU-400 is equivalent to the size of the C<small><sub>2</sub></small>H<small><sub>6</sub></small> molecule, which can provide a more accessible channel surface for C<small><sub>2</sub></small>H<small><sub>6</sub></small>. The pore environment of ZJNU-400 is rich in low-polarity aromatic groups, and uncoordinated N and O atoms can interact strongly with C<small><sub>2</sub></small>H<small><sub>6</sub></small> molecules. Therefore, ZJNU-400 exhibits significant C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> (50/50) selectivity (2.82) and C<small><sub>2</sub></small>H<small><sub>6</sub></small> uptake (64.3 cm<small><sup>3</sup></small> g<small><sup>-1</sup></small>) at 298 K and 1 bar, which is superior to many C<small><sub>2</sub></small>H<small><sub>6</sub></small>-selective adsorbents. Breakthrough experiment shows that ZJNU-400 can purify C<small><sub>2</sub></small>H<small><sub>4</sub></small> from C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixture in one step. GCMC and DFT calculations further revealed that the multiple synergistic interactions between the MOF and C<small><sub>2</sub></small>H<small><sub>6</sub></small> enable efficient separation of the C<small><sub>2</sub></small>H<small><sub>6</sub></small>-C<small><sub>2</sub></small>H<small><sub>4</sub></small> mixture. These results indicate that ZJNU-400 is a promising adsorbent for C<small><sub>2</sub></small>H<small><sub>6</sub></small>/C<small><sub>2</sub></small>H<small><sub>4</sub></small> separation.\",\"PeriodicalId\":79,\"journal\":{\"name\":\"Inorganic Chemistry Frontiers\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.1000,\"publicationDate\":\"2024-09-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganic Chemistry Frontiers\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d4qi01685h\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry Frontiers","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d4qi01685h","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
Tetranuclear-cluster-based MOF with low-polar pore environment for efficient C2H6/C2H4 separation
Removing trace ethane (C2H6) from ethylene (C2H4) to obtain high-purity C2H4 is of great industrial significance. However, the construction of C2H6-selective metal-organic frameworks (MOFs) remains challenging, mainly because C2H4 has a small dynamic diameter and a large quadrupole moment. It has been reported that ultramicroporous MOFs with tailored pore sizes and weakly polar pore environment can effectively purify C2H4 from C2H6-C2H4 mixtures. For this purpose, we successfully designed and synthesized one novel MOF material ZJNU-400 with non-polar pore environment. The channel size of ZJNU-400 is equivalent to the size of the C2H6 molecule, which can provide a more accessible channel surface for C2H6. The pore environment of ZJNU-400 is rich in low-polarity aromatic groups, and uncoordinated N and O atoms can interact strongly with C2H6 molecules. Therefore, ZJNU-400 exhibits significant C2H6/C2H4 (50/50) selectivity (2.82) and C2H6 uptake (64.3 cm3 g-1) at 298 K and 1 bar, which is superior to many C2H6-selective adsorbents. Breakthrough experiment shows that ZJNU-400 can purify C2H4 from C2H6/C2H4 mixture in one step. GCMC and DFT calculations further revealed that the multiple synergistic interactions between the MOF and C2H6 enable efficient separation of the C2H6-C2H4 mixture. These results indicate that ZJNU-400 is a promising adsorbent for C2H6/C2H4 separation.