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Ligand-Engineered CuO/Cu2O Heterointerfaces on Metal-Organic Framework-Derived Carbon-Zeolite Hybrids for Enhanced Oxygen Activation in Low-Temperature Toluene Oxidation.

Created on 12 Sep 2026

Authors

Jie Liu, Wenju Jiang, Jianbei Zhang, Yang Xiao, Runqing Wang, Zhongde Dai, Junfeng Zheng, Lu Yao, Lin Yang

Published in

ACS applied materials & interfaces. Sep 11, 2026. Epub Sep 11, 2026.

Abstract

Developing highly efficient catalysts for the low-temperature oxidation of volatile organic compounds (VOCs) remains a significant challenge, particularly in regulating the electronic structure of transition metal sites. In this study, we demonstrate that the topological design of Cu-MOF precursors is associated with distinct interfacial electronic reconstruction of derived carbon-zeolite hybrid catalysts (Cu/C-Y). By systematically comparing four ligands-specific precursors (H3BTC, H2BDC, H2IPA, and H2DHTP), we tailored the local microenvironments and electronic configurations of the resulting Cu species. Specifically, the symmetric planar H2BDC-derived precursor system favors the formation of a representative electron-deficient CuO/Cu2O heterointerface during pyrolysis. Density functional theory (DFT) calculations reveal that this ligand-engineered architecture induces substantial interfacial charge redistribution, upshifting the Cu d-band center and reducing the oxygen vacancy formation energy from +1.88 eV to -2.11 eV. These are consistent with enhanced oxygen activation required for the possible contributions from L-H-like and MvK-like pathways. Consequently, the optimal Cubdc/C-Y catalyst exhibits superior catalytic activity for toluene oxidation (T90 = 254 °C) and an exceptionally low apparent activation energy (41.9 kJ mol-1), while maintaining good long-term stability and largely reversible water tolerance. These results provide a fundamental strategy for leveraging ligand-directed electronic programming to design advanced environmental catalysts.

PMID:
42726938
Bibliographic data and abstract were imported from PubMed on 12 Sep 2026.

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