Unraveling the High Uptake and Selectivity of CO2 in the Zeolitic Imidazolate Frameworks ZIF-68 and ZIF-69
文献类型：期刊论文
| 作者 | Hou, Xin-Juan; Li, Huiquan |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY C
 |
| 出版日期 | 2010-08-19 |
| 卷号 | 114期号:32页码:13501-13508 |
| 关键词 | metal-organic frameworks monte-carlo-simulation dot-o interactions molecular simulation carbon-dioxide embedded oniom hydrogen-bond adsorption separation density |
| ISSN号 | 1932-7447 |
| 其他题名 | J. Phys. Chem. C |
| 中文摘要 | Understanding the CO2 adsorption mechanism of zeolitic imidazole frameworks (ZIFs) is the key to improving the adsorption ability of new metal-organic framework materials for gas capture applications and designing novel frameworks. In this work, the ONIOM2(B3LYP/6-31G**:UFF) method is used to investigate the interactions between CO2 and CO molecules with ZIF-68 and ZIF-69, respectively. Calculation results indicate that a strong Lewis acid-base interaction exists between the gas molecules and nitro groups of 2-nitroimidazole linkers, which thus prevents the entry of gas molecules into the small pores of ZlFs. The simultaneous interaction of both oxygen atoms of CO2 with the H atoms of the benzimidazole (5-chlorobenzimidazole) rings in the large pores results in the high CO2 selectivity observed for both ZIFs. The presence of electron-withdrawing groups in the phenylimidazole linker of ZIP increases the interaction between the oxygen atoms of CO2 and hydrogen atoms of the phenyl rings in its large pores. This work elucidates the adsorption mechanism of CO2 and CO to ZIFs at the molecular level and provides useful information for the design of MOFs in gas purification and separation applications. |
| 英文摘要 | Understanding the CO2 adsorption mechanism of zeolitic imidazole frameworks (ZIFs) is the key to improving the adsorption ability of new metal-organic framework materials for gas capture applications and designing novel frameworks. In this work, the ONIOM2(B3LYP/6-31G**:UFF) method is used to investigate the interactions between CO2 and CO molecules with ZIF-68 and ZIF-69, respectively. Calculation results indicate that a strong Lewis acid-base interaction exists between the gas molecules and nitro groups of 2-nitroimidazole linkers, which thus prevents the entry of gas molecules into the small pores of ZlFs. The simultaneous interaction of both oxygen atoms of CO2 with the H atoms of the benzimidazole (5-chlorobenzimidazole) rings in the large pores results in the high CO2 selectivity observed for both ZIFs. The presence of electron-withdrawing groups in the phenylimidazole linker of ZIP increases the interaction between the oxygen atoms of CO2 and hydrogen atoms of the phenyl rings in its large pores. This work elucidates the adsorption mechanism of CO2 and CO to ZIFs at the molecular level and provides useful information for the design of MOFs in gas purification and separation applications. |
| WOS标题词 | Science & Technology ; Physical Sciences ; Technology |
| 类目[WOS] | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| 研究领域[WOS] | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| 关键词[WOS] | METAL-ORGANIC FRAMEWORKS ; MONTE-CARLO-SIMULATION ; DOT-O INTERACTIONS ; MOLECULAR SIMULATION ; CARBON-DIOXIDE ; EMBEDDED ONIOM ; HYDROGEN-BOND ; ADSORPTION ; SEPARATION ; DENSITY |
| 收录类别 | SCI |
| 原文出处 | |
| 语种 | 英语 |
| WOS记录号 | WOS:000280727500014 |
| 公开日期 | 2013-11-28 |
| 版本 | 出版稿 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/6515]  |
| 专题 | 过程工程研究所_研究所（批量导入） |
| 作者单位 | Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Hou, Xin-Juan,Li, Huiquan. Unraveling the High Uptake and Selectivity of CO2 in the Zeolitic Imidazolate Frameworks ZIF-68 and ZIF-69[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2010,114(32):13501-13508. |
| APA | Hou, Xin-Juan,&Li, Huiquan.(2010).Unraveling the High Uptake and Selectivity of CO2 in the Zeolitic Imidazolate Frameworks ZIF-68 and ZIF-69.JOURNAL OF PHYSICAL CHEMISTRY C,114(32),13501-13508. |
| MLA | Hou, Xin-Juan,et al."Unraveling the High Uptake and Selectivity of CO2 in the Zeolitic Imidazolate Frameworks ZIF-68 and ZIF-69".JOURNAL OF PHYSICAL CHEMISTRY C 114.32(2010):13501-13508. |
入库方式： OAI收割
来源：过程工程研究所
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