The synergistic coupling of nonthermal plasma (NTP) with catalysts offers a promising route for converting CO 2 /H 2 O into high-value-added chemicals, but its efficiency is hindered by low-activity catalysts and electron quenching by gaseous H 2 O. Herein, we propose a “surface electron-enriched microenvironment” strategy to construct a UiO-66(SH) 2 catalyst to boost NPT CO 2 conversion. Under dielectric barrier discharge (DBD) plasma conditions, the UiO-66(SH) 2 catalytic system achieves a CO 2 conversion rate of 42.19%, which is 1.88 and 38.87 times higher than that of the unmodified UiO-66 system and plasma-only system, respectively. CO was identified as the dominant carbon-containing product with a selectivity of 82.39%, along with CH 4 and trace C 2 –C 3 hydrocarbons. Theoretical calculations and experimental results confirm that the thiol groups in UiO-66(SH) 2 create an electron-enriched microenvironment, which significantly enhances the adsorption and activation of CO 2 while effectively suppressing the electron quenching effect of gaseous H 2 O on a plasma-induced CO 2 dissociation process. Furthermore, thiol functional groups create an electron-rich microenvironment, effectively reducing the free-energy barrier for the formation of the key intermediate *COOH and thereby accelerating CO 2 conversion kinetics. This research provides a rational strategy for achieving efficient and highly selective plasma catalytic CO 2 conversion through the metal–organic frameworks (MOFs) functionalization.
He et al. (Sun,) studied this question.
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