Selective hydrogenation via precise hydrogen bond interactions on catalytic scaffolds.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 36702821.
- Also identified by DOI 10.1038/s41467-023-36015-z and PMC identifier 9879947.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
The active site environment in enzymes has been known to affect catalyst performance through weak interactions with a substrate, but precise synthetic control of enzyme inspired heterogeneous catalysts remains challenging. Here, we synthesize hyper-crosslinked porous polymer (HCPs) with solely -OH or -CH<sub>3</sub> groups on the polymer scaffold to tune the environment of active sites. Reaction rate measurements, spectroscopic techniques, along with DFT calculations show that HCP-OH catalysts enhance the hydrogenation rate of H-acceptor substrates containing carbonyl groups whereas hydrophobic HCP- CH<sub>3</sub> ones promote non-H bond substrate activation. The functional groups go beyond enhancing substrate adsorption to partially activate the C = O bond and tune the catalytic sites. They also expose selectivity control in the hydrogenation of multifunctional substrates through preferential substrate functional group adsorption. The proposed synthetic strategy opens a new class of porous polymers for selective catalysis.