单原子Pd促进的Cu催化剂用于乙醇脱氢

doi:10.1016/j.actphy.2025.100100

物理化学学报 >> 2025, Vol. 41 >> Issue (9): 100100.doi: 10.1016/j.actphy.2025.100100

单原子Pd促进的Cu催化剂用于乙醇脱氢

冯乐乐¹^,², 白雪莹¹^,³, 庞纪峰¹^,*(), 曹宏晨¹^,², 刘晓艳¹, 罗文豪⁴, 杨小峰¹^,*(), 吴鹏飞¹, 郑明远¹^,*()

¹ 中国科学院大连化学物理研究所, 中国科学院应用催化科学与技术重点实验室, 辽宁大连 116023
² 中国科学院大学, 北京 100049
³ 大连交通大学材料科学与工程学院, 辽宁大连 116028
⁴ 内蒙古大学化学化工学院, 内蒙古自治区呼和浩特 010021

收稿日期:2025-03-11 修回日期:2025-04-29 录用日期:2025-04-30 发布日期:2025-07-04
通讯作者: Email: jfpang@dicp.ac.cn (庞纪峰)yangxf2003@dicp.ac.cn (杨小峰)myzheng@dicp.ac.cn (郑明远)
基金资助:
国家自然科学基金(22378383); 国家自然科学基金(22279115); “单原子催化”基础科学中心(22388102)

Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation

Lele Feng¹^,², Xueying Bai¹^,³, Jifeng Pang¹^,*(), Hongchen Cao¹^,², Xiaoyan Liu¹, Wenhao Luo⁴, Xiaofeng Yang¹^,*(), Pengfei Wu¹, Mingyuan Zheng¹^,*()

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

Received:2025-03-11 Revised:2025-04-29 Accepted:2025-04-30 Published:2025-07-04
Contact: Email: jfpang@dicp.ac.cn (Jifeng Pang)yangxf2003@dicp.ac.cn (Xiaofeng Yang)myzheng@dicp.ac.cn (Mingyuan Zheng)
Supported by:
the National Science Foundation of China(22378383); the National Science Foundation of China(22279115); the NSFC Center for Single-Atom Catalysis(22388102)

摘要/Abstract

摘要：

乙醇脱氢是乙醇催化转化过程中的关键基元步骤，铜(Cu)基合金催化剂是该反应最具前景的候选材料。然而，由于合金催化剂在反应条件下固有的结构复杂性和动态演变特性，阐明合金组分与主体金属间协同效应的内在机制仍具挑战性。本研究设计了结构明确的单原子钯(Pd)修饰Cu-MFI催化剂用于乙醇脱氢制乙醛和氢气。通过球差校正高角环形暗场扫描透射电子显微镜(AC-HAADF-STEM)、X射线吸收光谱(XAS)、X射线光电子能谱(XPS)等系统表征结合密度泛函理论(DFT)计算表明，Pd原子被均匀分散在Cu催化剂表面并被Cu原子隔离，该单原子位点配位数为9–10、带−0.36e电荷。在乙醇脱氢反应中，新生成的Pd^δ−和Cu^δ+位点协同作用降低了乙醇中C—H键断裂的活化能垒，同时增强了氢吸附和H—H键耦合能力，使得Pd/Cu-MFI催化剂获得更高的乙醇转化率和乙醛产率。

关键词: 乙醇, 脱氢, Pd-Cu单原子催化剂, 电子转移, 氢

Abstract:

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.

Key words: Ethanol, Dehydrogenation, Pd-Cu single-atom catalyst, Electron transfer, Hydrogen

冯乐乐, 白雪莹, 庞纪峰, 曹宏晨, 刘晓艳, 罗文豪, 杨小峰, 吴鹏飞, 郑明远. 单原子Pd促进的Cu催化剂用于乙醇脱氢[J]. 物理化学学报, 2025, 41(9), 100100. doi: 10.1016/j.actphy.2025.100100

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 Phys. -Chim. Sin. 2025, 41(9), 100100. doi: 10.1016/j.actphy.2025.100100

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100100

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I9/100100

图/表 6

参考文献 72

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单原子Pd促进的Cu催化剂用于乙醇脱氢

Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation

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