Cu Evolution over Bimetallic Cu‐Y/Beta Zeolite Under H <sub>2</sub> and Ethanol Atmospheres: Unveiling the Role of Diatomic Metal–Metal Interactions

Understanding the dynamic evolution of Cu species under varying environmental conditions is critical for addressing challenges related to the activity and the stability of copper-based catalysts in thermo-, photo-, and electrocatalysis. However, metal-metal interactions between dual single atoms and their effects on Cu evolution after exposure to different environmental molecules remain underexplored. Herein, we synthesized bimetallic Cu-Y/Beta catalysts with dual single-atom Cu and Y sites and monometallic Cu-Beta catalysts with isolated Cu sites in dealuminated Beta zeolites. By varying Cu and Y compositions, diatomic interactions were studied under H<sub>2</sub> and ethanol atmospheres. With 6 wt% Y loading, approximately 0.4 wt% of Cu species in Cu-Y/Beta remained partially oxidized as Cu(I) after reduction in pure H<sub>2</sub> at 350 °C, in contrast to the full transition to metallic Cu observed in Cu-Beta. Combining X-ray absorption spectroscopy with kinetic studies revealed that metallic Cu became the predominant species after reduction with H<sub>2</sub> as Cu loading increased from 0.4 to 1.7 wt%, quadrupling the initial ethanol dehydrogenation rate and demonstrating the dominant role of Cu(0) sites. Scanning transmission electron microscopy and density functional theory simulations indicated spatial proximity between dual single-atom Cu and Y sites and elucidated Cu speciation controlled by diatomic interactions.

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Journal
Angewandte Chemie International Edition
Published
2025-09-29
DOI
https://doi.org/10.1002/anie.202514920
Primary Topic
Catalytic Processes in Materials Science
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article
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article

Cu Evolution over Bimetallic Cu‐Y/Beta Zeolite Under H 2 and Ethanol Atmospheres: Unveiling the Role of Diatomic Metal–Metal Interactions

Felipe Polo‐Garzon, Kinga A. Unocic, Jeffrey T. Miller, James W. Harris et al.
Angewandte Chemie International Edition
Catalytic Processes in Materials Science
article

Cu Evolution over Bimetallic Cu‐Y/Beta Zeolite Under H 2 and Ethanol Atmospheres: Unveiling the Role of Diatomic Metal–Metal Interactions

Felipe Polo‐Garzon, Kinga A. Unocic, Jeffrey T. Miller, James W. Harris, Stephen C. Purdy, Shan Jiang, Brandon C. Bukowski, Pengfei Xie, Evan C. Wegener, Zili Wu, Mingze Zheng, Nohor “River” Samad, Sheng Dai, Dongxia Liu, Wenbo Li, Junyan Zhang, Zhenglong Li, Meijun Li, Andrew D. Sutton, Theodore R. Krause, Yanran Cui
article en

Abstract

Understanding the dynamic evolution of Cu species under varying environmental conditions is critical for addressing challenges related to the activity and the stability of copper-based catalysts in thermo-, photo-, and electrocatalysis. However, metal-metal interactions between dual single atoms and their effects on Cu evolution after exposure to different environmental molecules remain underexplored. Herein, we synthesized bimetallic Cu-Y/Beta catalysts with dual single-atom Cu and Y sites and monometallic Cu-Beta catalysts with isolated Cu sites in dealuminated Beta zeolites. By varying Cu and Y compositions, diatomic interactions were studied under H<sub>2</sub> and ethanol atmospheres. With 6 wt% Y loading, approximately 0.4 wt% of Cu species in Cu-Y/Beta remained partially oxidized as Cu(I) after reduction in pure H<sub>2</sub> at 350 °C, in contrast to the full transition to metallic Cu observed in Cu-Beta. Combining X-ray absorption spectroscopy with kinetic studies revealed that metallic Cu became the predominant species after reduction with H<sub>2</sub> as Cu loading increased from 0.4 to 1.7 wt%, quadrupling the initial ethanol dehydrogenation rate and demonstrating the dominant role of Cu(0) sites. Scanning transmission electron microscopy and density functional theory simulations indicated spatial proximity between dual single-atom Cu and Y sites and elucidated Cu speciation controlled by diatomic interactions.

Angewandte Chemie International EditionVol. 64(47)
Argonne National Laboratory (US), Oak Ridge National Laboratory (US), North Carolina State University (US), East China University of Science and Technology (CN), Johns Hopkins University (US), University of Alabama (US), Purdue University West Lafayette (US), North Central State College (US), Quzhou University (CN), University of Maryland, College Park (US), Zhejiang University (CN)
Openalex Percentile: Top 79%
Catalytic Processes in Materials Science
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