Zhao Bo, Li Chong, Hu Tuoping, Gao Yanpeng, Fan Liming, Zhang Xiutang
School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, People's Republic of China.
College of Chemical Engineering, Ordos Institute of Technology, Ordos 017000, P. R. China.
Inorg Chem. 2024 Jul 29;63(30):14183-14192. doi: 10.1021/acs.inorgchem.4c02093. Epub 2024 Jul 15.
Developing a highly active catalyst that can efficiently capture and convert carbon dioxide (CO) into high-value-added energy materials remains a severe challenge, which inspires us to explore effective metal-organic frameworks (MOFs) with high chemical stability and high-density active sites. Herein, we report a robust 3D lead(II)-organic framework of {(MeNH)[Pb(PTTPA)(HO)]·2DMF·3HO} () with unreported [Pb(COO)(HO)] clusters (abbreviated as {Pb}) as nodes (HPTTPA = 4,4',4″-(pyridine-2,4,6-triyl)triisophthalic acid). After thermal activation, is functionalized by the multifarious symbiotic acid-base active sites of open Pb sites and uncoordinated pyridine groups on the inner surface of the void volume. Gas adsorption tests confirm that displays a higher separation performance for mixed gases of f CO and CH with the selectivity of CO/CH at 273 K and 101 kPa being 31 (1:99, v/v), 23 (15:85, v/v), and 8 (50:50, v/v), respectively. When the temperature rises to 298 K, the selectivity of CO/CH at 101 kPa is 26 (1:99, v/v), 22 (15:85, v/v), and 11 (50:50, v/v). Moreover, activated exhibited excellent catalytic performance, stability, and recyclability for the cycloaddition of CO with epoxides under mild conditions. Hence, this work provides valuable insight into designing MOFs with multifunctionality for CO capture, separation, and conversion.
开发一种能够有效捕获二氧化碳（CO₂）并将其转化为高附加值能源材料的高活性催化剂仍然是一项严峻挑战，这促使我们探索具有高化学稳定性和高密度活性位点的有效金属有机框架（MOF）。在此，我们报道了一种坚固的三维铅（II）有机框架{（MeNH₃）[Pb（PTTPA）（H₂O）]·2DMF·3H₂O}（ ），其具有未报道的[Pb（COO）（H₂O）]簇（简称为{Pb}）作为节点（HPTTPA = 4,4',4″-（吡啶-2,4,6-三基）三异苯二甲酸）。热活化后， 通过开放的铅位点的多种共生酸碱活性位点以及孔隙内表面上未配位的吡啶基团进行功能化。气体吸附测试证实， 对CO₂和CH₄的混合气体表现出更高的分离性能，在273 K和101 kPa下CO₂/CH₄的选择性分别为31（1:99，v/v）、23（15:85，v/v）和8（50:50，v/v）。当温度升至298 K时，在101 kPa下CO₂/CH₄的选择性为26（1:99，v/v）、22（15:85，v/v）和11（50:50，v/v）。此外，活化后的 在温和条件下对CO₂与环氧化物的环加成反应表现出优异的催化性能、稳定性和可回收性。因此，这项工作为设计具有多功能性的用于CO₂捕获、分离和转化的MOF提供了有价值的见解。
