Numerous hyper-cross-linked polymers (HCPs) have been developed as CO adsorbents and photocatalysts. Yet, little is known of the CO and HO adsorption mechanisms on amorphous porous polymers. Gaining a better understanding of these mechanisms and determining the adsorption sites are key to the rational design of improved adsorbents and photocatalysts. Herein, we present a unique approach that combines density functional theory (DFT), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and multivariate spectral analysis to investigate CO and HO adsorption sites on a triazine-biphenyl HCP. We found that CO and HO adsorb on the same HCP sites albeit with different adsorption strengths. The primary amines of the triazines were identified as favoring strong CO binding interactions. Given the potential use of HCPs for CO photoreduction, we also investigated CO and HO adsorption under transient light irradiation. Under irradiation, we observed partial CO and HO desorption and a redistribution of interactions between the HO and CO molecules that remain adsorbed at HCP adsorption sites.
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| http://dx.doi.org/10.1021/acs.jpcb.2c03912 | DOI Listing |
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