Journal
SCIENCE ADVANCES
Volume 6, Issue 17, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.aaz4824
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Funding
- National Key Basic Research Program of China [2014CB931801, 2016YFA0200700]
- National Natural Science Foundation of China [21890381, 21721002, 21475029, 21722102, 51672053, 21303029]
- Beijing Natural Science Foundation [2182087]
- Frontier Science Key Project of Chinese Academy of Sciences [QYZDJ-SSW-SLH038]
- CAS-CSIRO Cooperative Research Program [GJHZ1503]
- project of K. C. Wong Education Foundation
- Youth Innovation Promotion Association CAS [2016036]
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CO2 cycloaddition with epoxides at low temperature and pressure has been broadly recognized as an ambitious but challenging goal, which requires the catalysts to have precisely controlled Lewis acid sites. Here, we demonstrate that both stereochemical environment and oxidation state of single cobalt active sites in cobalt tetraaminophthalocyanine [CoPc(NH2)(4)] are finely tuned via molecular engineering with 2,5-di-tert-butyl-1,4-benzoquinone (DTBBQ). Notably, DTBBQ incorporation not only enables formation of 5-nm-thick conjugated microporous polymer (CMP) nanosheets due to the steric hindrance effect of tert-butyl groups but also makes isolated cobalt sites with high oxidation state due to the presence of delocalized electron-withdrawing effect of alkene groups in DTBBQ via conjugated skeleton. Notably, when used as heterogeneous catalysts for CO2 cycloaddition with different epoxides, single cobalt active sites on the ultrathin CMP nanosheets exhibit unprecedentedly high activity and excellent stability under mild reaction conditions.
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