用于糠醇加氢的稳定型Rh/羟基磷灰石催化剂：氧化型金属-载体强相互作用在还原条件下的应用

引用本文: 唐海莲, 陈思远, 刘巧云, 白国义, 乔波涛, 刘菲. 用于糠醇加氢的稳定型Rh/羟基磷灰石催化剂：氧化型金属-载体强相互作用在还原条件下的应用[J]. 物理化学学报, 2025, 41(4): 100036. doi: 10.3866/PKU.WHXB202408004 shu

Citation: Hailian Tang, Siyuan Chen, Qiaoyun Liu, Guoyi Bai, Botao Qiao, Fei Liu. Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions[J]. Acta Physico-Chimica Sinica, 2025, 41(4): 100036. doi: 10.3866/PKU.WHXB202408004 shu

用于糠醇加氢的稳定型Rh/羟基磷灰石催化剂：氧化型金属-载体强相互作用在还原条件下的应用

唐海莲 ^{1,2,
,} ,
陈思远 ^2,3, ,
刘巧云 ^2,4, ,
白国义 ^1, ,
乔波涛 ^{2,5,
,} ,
刘菲 ^{2,
,}

1.
天津理工大学化学化工学院, 天津 300384;
2.
中国科学院大连化学物理研究所, 中国科学院催化材料重点实验室, 辽宁大连 116023;
3.
河北大学化学与材料科学学院, 河北保定 071002;
4.
郑州大学化学学院, 郑州 450001;
5.
中国科学院大连化学物理研究所, 催化基础国家重点实验室, 辽宁大连 116023

通讯作者: 唐海莲, E-mail: hltang@email.tjut.edu.cn; 乔波涛, E-mail: bqiao@dicp.ac.cn; 刘菲, E-mail: fei.liu@dicp.ac.cn

基金项目:
国家重点研发计划(2023YFA1506800),国家自然科学基金(21902040,22108259),河北省自然科学基金(B2019201158)资助项目

摘要: 金属-载体强相互作用(SMSI)是多相催化中的一个重要概念，其发生可以显著提高催化剂稳定性并可能调变催化剂性能。然而，由于SMSI效应一般是可逆的，在与其构建的氧化还原条件相反的情况下会发生消退，因此其应用一般需要反应条件与构建条件相同或接近，因而受到限制。本研究报道了在羟基磷灰石负载的Rh催化剂(Rh/HAP)体系上构建的氧化型SMSI(O-SMSI)在还原性环境—糠醇加氢中的应用。通过CO吸附原位漫反射红外傅立叶变换光谱和电镜表征，发现经过500 ℃的高温氧化处理后在Rh/HAP催化剂上形成了O-SMSI效应，该效应伴随着载体对Rh颗粒的包裹行为。在O-SMSI作用下，Rh物种稳定存在于载体表面，其烧结和液相反应下的流失被显著抑制，因此催化剂在循环测试中表现出了稳定的糠醇转换活性和环戊酮选择性。另外，我们还观察到，Rh/HAP体系上的O-SMSI效应及其伴随的包裹行为只是部分可逆而非完全可逆。即使在高达600 ℃的高温还原后，部分SMSI效应仍然保留，确保了催化剂在还原反应中的稳定性。这一发现极大地拓展了SMSI催化剂的应用范围，并为稳定的加氢催化剂的研发提供了新途径。

关键词:

English

Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions

Hailian Tang ^{1,2,
,} ,
Siyuan Chen ^2,3, ,
Qiaoyun Liu ^2,4, ,
Guoyi Bai ^1, ,
Botao Qiao ^{2,5,
,} ,
Fei Liu ^{2,
,}

1.
School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China;
2.
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China;
3.
College of Chemistry and Materials Science, Hebei University, Baoding 071002, Hebei Province, China;
4.
College of Chemistry, Zhengzhou University, Zhengzhou 450001, China;
5.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China

Corresponding author: Hailian Tang, ; Botao Qiao, ; Fei Liu,

Received Date: 04 August 2024
Accepted Date: 02 October 2024
Revised Date: 14 September 2024
Fund Project:
The project was supported by the National Key R&D Program of China (2023YFA1506800), National Natural Science Foundation of China (21902040, 22108259), and Natural Science Foundation of Hebei Province (B2019201158).

Abstract: The strong metal-support interaction (SMSI) is a widely recognized concept in heterogeneous catalysis, known for significantly enhancing catalyst stability and potentially modulating catalytic performance. However, because the SMSI effect is generally reversible, it tends to diminish under redox conditions opposite to those used for its construction. Consequently, its application is typically limited to conditions that are the same or similar to those under which it was formed. Herein, we report the application of oxidative SMSI (O-SMSI) constructed on hydroxyapatite-supported Rh catalyst (Rh/HAP) in a reductive reaction, the hydrogenation of furfuryl alcohol. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and electron microscopy measurements reveal that high-temperature oxidation treatment at 500 ℃ induced the occurrence of O-SMSI on the Rh/HAP catalyst, accompanied by the encapsulation of Rh particles by the support. Upon the O-SMSI, the Rh species were effectively stabilized on the support surface, with significant suppression of sintering and leaching during liquid-phase reactions. As a result, the catalyst showed stable furfuryl alcohol conversion and cyclopentanone selectivity during recycling tests. Furthermore, it was found that the O-SMSI and the associated encapsulation behavior on the Rh/HAP system were only partially reversible rather than completely reversible. Even after high-temperature reduction at up to 600 ℃, a portion of the SMSI effect remains, ensuring the stability of the catalysts in reductive reactions. This discovery greatly expands the application scope of SMSI catalysts and provides a new way to prepare stable hydrogenation catalysts.

Key words:

Oxidative strong metal-support interaction
/ Hydroxyapatite
/ Rh
/ Stability
/ Hydrogenation

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沈阳化工大学材料科学与工程学院沈阳 110142

用于糠醇加氢的稳定型Rh/羟基磷灰石催化剂：氧化型金属-载体强相互作用在还原条件下的应用

通讯作者: 唐海莲, E-mail: hltang@email.tjut.edu.cn; 乔波涛, E-mail: bqiao@dicp.ac.cn; 刘菲, E-mail: fei.liu@dicp.ac.cn

English

Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions

Corresponding author: Hailian Tang, ; Botao Qiao, ; Fei Liu,

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中国化学会秘书处

用于糠醇加氢的稳定型Rh/羟基磷灰石催化剂：氧化型金属-载体强相互作用在还原条件下的应用

通讯作者: 唐海莲, E-mail: hltang@email.tjut.edu.cn; 乔波涛, E-mail: bqiao@dicp.ac.cn; 刘菲, E-mail: fei.liu@dicp.ac.cn

English

Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions

Corresponding author: Hailian Tang, ; Botao Qiao, ; Fei Liu,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs