Atomic Cu–O–Zr Sites for Highly Selective Production of p-xylene from Tandem Upcycling of PET and CO2
Qizhuang Zou
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorTairen Long
State Key Laboratory of Physical Chemistry of Solid Surfaces, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 360015 China
Search for more papers by this authorCorresponding Author
Ruiqi Fang
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorXin Zhao
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorFengliang Wang
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorCorresponding Author
Yingwei Li
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorQizhuang Zou
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorTairen Long
State Key Laboratory of Physical Chemistry of Solid Surfaces, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 360015 China
Search for more papers by this authorCorresponding Author
Ruiqi Fang
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorXin Zhao
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorFengliang Wang
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
Search for more papers by this authorCorresponding Author
Yingwei Li
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorGraphical Abstract
A heterogeneous catalyst Cu/UiO-66-NH2-A with atomic Cu–O–Zr sites was successfully developed at ambient temperature and pressure, which not only exhibits efficient activation of C═O and H─H bonds but also possesses a fast hydrogen spillover effect. These properties endow this catalyst with superior catalytic activity for the upcycling of waste PET and CO2 into p-xylene (PX) and ethylene glycol (EG).
Abstract
Exploring an efficient catalytic system for tandem upcycling of CO2 and polyethylene terephthalate (PET) is highly desirable for achieving efficient resource utilization of wastes. However, the high activation energy for C═O bonds (in both PET and CO2) and the difficulty in regulating the reaction pathways restricted PET recovery efficiency. Here, we demonstrated the rational design of a single-atom Cu catalyst for precisely catalyzing the hydrogenation of CO2 to methanol and tandem PET upcycling to ethylene glycol (EG) and p-xylene (PX). In the Cu/UiO-66-NH2-A catalyst, Cu atoms are selectively anchored to the Zr-oxo nodes of UiO-66-NH2 to form Cu–O–Zr sites. The Cu–O–Zr sites can effectively activate both CO2 and H2 by reducing the activation energy and accelerate the transformation of PET to dimethyl terephthalate (DMT), which is further hydro-deoxygenated to yield PX. As a result, 20.4% CO2 conversion was obtained within 36 h, with 89.5% and 92.1% yields of PX and EG, respectively. Rapid and precise hydrogen spillover from Cu atoms to adsorbed reactants/intermediates at the Cu–O–Zr sites also drives the reaction process.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
Supporting Information
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Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
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