SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2024, Vol. 70 ›› Issue (6): 222-233.DOI: 10.1016/j.cjche.2024.03.014

• • 上一篇    下一篇

Porous silica nano-flowers stabilized Pt-Pd bimetallic nanoparticles as heterogeneous catalyst for efficiently synthesizing guaiacol from 2-methoxycyclohexanol

Junbo Feng1,2,4, Junyan Wu1,3, Dongdong Yan1, Yadong Zhang1,3   

  1. 1. School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China;
    2. State Key Laboratory of Coking Coal Exploitation and Comprehensive Utilization, Pingdingshan 467000, China;
    3. Jiyuan Research Institute, Zhengzhou University, Jiyuan 459000, China;
    4. School of Materials and Chemical Engineering, Zhongyuan University of Technology, Zhengzhou 450007, China
  • 收稿日期:2023-11-08 修回日期:2024-03-11 出版日期:2024-06-28 发布日期:2024-08-05
  • 通讯作者: Junbo Feng,E-mail:junbo716@163.com;Yadong Zhang,E-mail:zhangyadong2016@163.com
  • 基金资助:
    This work was financially supported by Natural Science Foundation of Henan Province of China (162300410253) and the Open Research Fund of State Key Laboratory of Coking Coal Exploitation and Comprehensive Utilization, China Pingmei Shen-ma Group (41040220181107-8).

Porous silica nano-flowers stabilized Pt-Pd bimetallic nanoparticles as heterogeneous catalyst for efficiently synthesizing guaiacol from 2-methoxycyclohexanol

Junbo Feng1,2,4, Junyan Wu1,3, Dongdong Yan1, Yadong Zhang1,3   

  1. 1. School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China;
    2. State Key Laboratory of Coking Coal Exploitation and Comprehensive Utilization, Pingdingshan 467000, China;
    3. Jiyuan Research Institute, Zhengzhou University, Jiyuan 459000, China;
    4. School of Materials and Chemical Engineering, Zhongyuan University of Technology, Zhengzhou 450007, China
  • Received:2023-11-08 Revised:2024-03-11 Online:2024-06-28 Published:2024-08-05
  • Contact: Junbo Feng,E-mail:junbo716@163.com;Yadong Zhang,E-mail:zhangyadong2016@163.com
  • Supported by:
    This work was financially supported by Natural Science Foundation of Henan Province of China (162300410253) and the Open Research Fund of State Key Laboratory of Coking Coal Exploitation and Comprehensive Utilization, China Pingmei Shen-ma Group (41040220181107-8).

摘要: Porous silica nano-flowers (KCC-1) immobilized Pt-Pd alloy NPs (Pt-Pd/KCC-1) with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction, using hydrazinium hydroxide as a reducing agent. The as-synthesized silica nanospheres possess radial fibers with a distance of 15 nm, exhibiting a high specific surface area (443.56 m2·g-1). Meanwhile, the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4-6 nm, which exist as metallic Pd and Pt on the surface of monodisperse KCC-1, showing the transfer of electrons from Pd to Pt. The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol. Compared with Pt or Pd single metal supported catalysts, the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2% conversion rate of 2-methoxycyclohexanol and 76.8% selectivity for guaiacol, which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs. Furthermore, turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s-1, showing higher catalytic efficiency than other two monometallic catalysts. Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed. Consequently, the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol, while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green, outstanding and powerful synthetic pathway of guaiacol.

关键词: Supported catalyst, Nanoparticles, Dehydrogenation, 2-Methoxycyclohexanol, Guaiacol

Abstract: Porous silica nano-flowers (KCC-1) immobilized Pt-Pd alloy NPs (Pt-Pd/KCC-1) with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction, using hydrazinium hydroxide as a reducing agent. The as-synthesized silica nanospheres possess radial fibers with a distance of 15 nm, exhibiting a high specific surface area (443.56 m2·g-1). Meanwhile, the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4-6 nm, which exist as metallic Pd and Pt on the surface of monodisperse KCC-1, showing the transfer of electrons from Pd to Pt. The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol. Compared with Pt or Pd single metal supported catalysts, the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2% conversion rate of 2-methoxycyclohexanol and 76.8% selectivity for guaiacol, which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs. Furthermore, turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s-1, showing higher catalytic efficiency than other two monometallic catalysts. Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed. Consequently, the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol, while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green, outstanding and powerful synthetic pathway of guaiacol.

Key words: Supported catalyst, Nanoparticles, Dehydrogenation, 2-Methoxycyclohexanol, Guaiacol