Journal
CHEM
Volume 5, Issue 3, Pages 693-705Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2018.12.014
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Funding
- National Key R&D Program of China [2016YFB0600902]
- Chinese Academy of Sciences [XDB17000000]
- National Natural Science Foundation of China [21476226, 21776269, 21503125]
- Dalian Science Foundation for Distinguished Young Scholars [2016RJ04]
- Youth Innovation Promotion Association CAS
- Natural Science Basic Research Plan in Shaanxi Province of China [2018JM2048]
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Heterogeneous single-atom catalysts (SACs) with atomically dispersed active metal centers represent an intermediary between heterogeneous and homogeneous catalysis. In this work, a porous organic polymer with aminopyridine functionalities was designed to fabricate a stable, atomically dispersed Ir catalyst. This Ir-based SAC exhibits excellent catalytic activity during the liquid-phase hydrogenation of CO2 to formate. The associated turnover number is as high as 25,135, representing the best performance yet for a heterogeneous conversion of CO2 to formate. Spectral characterization and density functional theory modeling demonstrate that the chemical structure of the Ir single-atom active site is analogous to that of a homogeneous mononuclear Ir pincer complex catalyst. As a result, a catalytic mechanism similar to that over a homogeneous Ir catalyst occurs during CO2 hydrogenation with this quasi-homogeneous Ir-based SAC. This work suggests a promising basis for the design of efficient SACs for the once-dominant homogeneous catalytic processes.
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