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Tailoring the Electron-Enriched Microenvironment of UiO-66 via Thiol Functionalization to Boost Non-Thermal Plasma CO2 Conversion.

Created on 05 Jul 2026

Authors

Junhui He, Mingming Zhang, Xiaochu Zheng, Jianfeng Li, Linjuan Yang, Cong Luo, Xudong Cui, Zhuoyu Ji, Daopeng Sheng, Xiaofang Feng, Tao Chen, Wenkun Zhu

Published in

Inorganic chemistry. Jul 05, 2026. Epub Jul 05, 2026.

Abstract

The synergistic coupling of nonthermal plasma (NTP) with catalysts offers a promising route for converting CO2/H2O into high-value-added chemicals, but its efficiency is hindered by low-activity catalysts and electron quenching by gaseous H2O. Herein, we propose a "surface electron-enriched microenvironment" strategy to construct a UiO-66(SH)2 catalyst to boost NPT CO2 conversion. Under dielectric barrier discharge (DBD) plasma conditions, the UiO-66(SH)2 catalytic system achieves a CO2 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 CH4 and trace C2-C3 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 CO2 while effectively suppressing the electron quenching effect of gaseous H2O on a plasma-induced CO2 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 CO2 conversion kinetics. This research provides a rational strategy for achieving efficient and highly selective plasma catalytic CO2 conversion through the metal-organic frameworks (MOFs) functionalization.

PMID:
42402077
Bibliographic data and abstract were imported from PubMed on 05 Jul 2026.

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