Citation: Lele Feng, Xueying Bai, Jifeng Pang, Hongchen Cao, Xiaoyan Liu, Wenhao Luo, Xiaofeng Yang, Pengfei Wu, Mingyuan Zheng. Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation[J]. Acta Physico-Chimica Sinica, ;2025, 41(9): 100100. doi: 10.1016/j.actphy.2025.100100 shu

Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation

Lele Feng ^{1, 2} ,
Xueying Bai ^{1, 3} ,
Jifeng Pang ^1,, ,
Hongchen Cao ^{1, 2} ,
Xiaoyan Liu ¹ ,
Wenhao Luo ⁴ ,
Xiaofeng Yang ^1,, ,
Pengfei Wu ¹ ,
Mingyuan Zheng ^1,,

1.
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
School of Materials Science and Engineering, Dalian Jiaotong University, Dalian 116028, Liaoning Province, China
4.
College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, Inner Mongolia Autonomous Region, China

Corresponding author: Jifeng Pang, jfpang@dicp.ac.cn Xiaofeng Yang, yangxf2003@dicp.ac.cn Mingyuan Zheng, myzheng@dicp.ac.cn
Received Date: 11 March 2025
Revised Date: 29 April 2025
Accepted Date: 30 April 2025

Fund Project: the National Science Foundation of China 22378383the National Science Foundation of China 22279115the NSFC Center for Single-Atom Catalysis 22388102

Ethanol dehydrogenation is a vital elementary step in ethanol upgrading, for which Cu-based alloy catalysts are the most promising candidates. Nevertheless, elucidating the underlying reasons for the synergistic effect between alloying components and host metals remains challenging due to the intrinsic structural complexity and dynamic evolution of alloy catalysts under operational conditions. Herein, single-atom Pd modified Cu-MFI catalysts with well-defined structures were designed for ethanol dehydrogenation to acetaldehyde and hydrogen. Comprehensive characterizations using aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that Pd atoms are isolated by surrounding Cu atoms with a coordination number of 9–10, forming −0.36e charged single-atom sites and being uniformly dispersed on the surface of Cu catalysts. The newly generated Pd^δ− and Cu^δ+ sites synergistically reduced the activation energy barrier for C—H bond cleavage in ethanol. These sites simultaneously enhanced hydrogen adsorption and H—H bond coupling, leading to improved ethanol conversion and acetaldehyde productivity over Pd/Cu-MFI catalysts.
- Ethanol,
- Dehydrogenation,
- Pd-Cu single-atom catalyst,
- Electron transfer,
- Hydrogen
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沈阳化工大学材料科学与工程学院沈阳 110142