Boosting Photocatalytic CO2 Cycloaddition via Dual-Active Site Coordination over Amino-Functionalized UiO-66(Zr)
Yajing Lv, Haohao Yan, Wenhui Ye, Lin Ye, Jinmei Chen, Yutong Lin, Shuying Zhu, Dengrong Sun, Xiyao Liu, Ruowen Liang
TL;DR
A new catalyst boosts CO2 conversion into useful chemicals by using dual active sites in a material called UiO-66(Zr)-NH2.
Contribution
The study introduces dual-active site coordination in amino-functionalized UiO-66(Zr) for efficient CO2 cycloaddition.
Findings
UZN achieves a 99.5% PC yield in CO2-epoxide cycloaddition.
UZN's production rate is 9.97 mmol·g−1·h−1, outperforming UZH.
Dual active sites enhance light harvesting and charge separation.
Abstract
CO2 cycloaddition with epoxides offers a sustainable route for CO2 utilization, yet the simultaneous activation of both substrates remains challenging. Herein, using UiO-66(Zr)-NH2 (denoted as UZN) as a model system, we illustrate that dual-active sites consisting of unsaturated Zr4+ centers and amine groups can efficiently accelerate CO2 fixation with epoxides under visible light. The unique ensemble in UZN optimizes light harvesting, promotes charge carrier separation, and enriches bifunctional active sites for efficient adsorption and activation of epoxides and CO2. Consequently, UZN exhibits significantly improved CO2-epoxide cycloaddition performance compared to UiO-66(Zr)-H (denoted as UZH), achieving a PC yield of 99.5%, with a production rate of 9.97 mmol·g−1·h−1. This work establishes a clear coordination–photocatalytic synergy in MOF-based systems and provides fundamental…
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Taxonomy
TopicsCarbon dioxide utilization in catalysis · Advanced Photocatalysis Techniques · CO2 Reduction Techniques and Catalysts