A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

doi:10.1016/j.cjche.2021.09.013

Chinese Journal of Chemical Engineering ›› 2022, Vol. 51 ›› Issue (11): 199-215.DOI: 10.1016/j.cjche.2021.09.013

A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

Guoxiao Cai^1,2, Wei Xiong¹, Susu Zhou¹, Pingle Liu¹, Yang Lv¹, Fang Hao¹, Hean Luo¹, ChangYi Kong²

1. College of Chemical Engineering, National & Local United Engineering Research Centre for Chemical Process Simulation and Intensification, Xiangtan University, Xiangtan 411105, China;
2. Department of Environment and Energy System, Graduate School of Science and Technology, Shizuoka University, 3-5-1 Johoku, Naka-ku, Hamamatsu 432-8561, Japan

Received:2021-06-15 Revised:2021-08-30 Online:2023-01-18 Published:2022-11-18
Contact: Pingle Liu,E-mail:liupingle@xtu.edu.cn;Fang Hao,E-mail:haofang.happy@163.com
Supported by:
This work was supported by the National Natural Science Foundation of China (21908185, 22178294), Project of Hunan Provincial Natural Science Foundation of China (2021JJ30663), Project of Hunan Provincial Education Department (19B572, 20B547), Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization, and National Department of Education Engineering Research Centre for Chemical Process Simulation and Optimization.

A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

Guoxiao Cai^1,2, Wei Xiong¹, Susu Zhou¹, Pingle Liu¹, Yang Lv¹, Fang Hao¹, Hean Luo¹, ChangYi Kong²

1. College of Chemical Engineering, National & Local United Engineering Research Centre for Chemical Process Simulation and Intensification, Xiangtan University, Xiangtan 411105, China;
2. Department of Environment and Energy System, Graduate School of Science and Technology, Shizuoka University, 3-5-1 Johoku, Naka-ku, Hamamatsu 432-8561, Japan

通讯作者: Pingle Liu,E-mail:liupingle@xtu.edu.cn;Fang Hao,E-mail:haofang.happy@163.com
基金资助:
This work was supported by the National Natural Science Foundation of China (21908185, 22178294), Project of Hunan Provincial Natural Science Foundation of China (2021JJ30663), Project of Hunan Provincial Education Department (19B572, 20B547), Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization, and National Department of Education Engineering Research Centre for Chemical Process Simulation and Optimization.

Abstract

Abstract: Ru and Mo bimetallic catalysts supported on active carbon modified by phosphotungstic acid (PW) were designed and applied in glycerol hydrogenolysis reaction. The physicochemical properties of the catalysts were characterized and the presence of active sites was investigated from the perspective of the glycerol hydrogenolysis performance. The MoO_x is highly selective for the C—O bond cleavage of glycerol molecules, which can reasonably regulate the strong C—C bond cleavage activity of Ru nanoparticles. By using sequential deposition of Ru and Mo supported on mesoporous PW-C, the characterization results show that the combination of isolated low-valence MoO_x with metal Ru particles can form “MoO_x-Ru-PW”, which provides highly catalytic activity toward C—O bond cleavage, selectively producing more C3 alcohols (mainly 1,2(3)-propanediol). The glycerol conversion of 1% Mo/Ru/PW-C catalyst was 59.6%, the selectivity of C3 alcohol was 96.1%, and the selectivity of propanediol (1,2(3)-propanediol) was 94.9%. It is noteworthy that the selectivity of 1,3-propanediol reached 20.7% when the PW was 21.07% (mass). This study provides experimental evidence for the tandem dehydration and hydrogenation mechanism of the multifunctional Mo/Ru/PW-C catalyst.

Key words: Heterogeneous catalysis, Bimetallic catalyst, Glycerol hydrogenolysis, Ruthenium, Molybdenum, Phosphotungstic acid

摘要： Ru and Mo bimetallic catalysts supported on active carbon modified by phosphotungstic acid (PW) were designed and applied in glycerol hydrogenolysis reaction. The physicochemical properties of the catalysts were characterized and the presence of active sites was investigated from the perspective of the glycerol hydrogenolysis performance. The MoO_x is highly selective for the C—O bond cleavage of glycerol molecules, which can reasonably regulate the strong C—C bond cleavage activity of Ru nanoparticles. By using sequential deposition of Ru and Mo supported on mesoporous PW-C, the characterization results show that the combination of isolated low-valence MoO_x with metal Ru particles can form “MoO_x-Ru-PW”, which provides highly catalytic activity toward C—O bond cleavage, selectively producing more C3 alcohols (mainly 1,2(3)-propanediol). The glycerol conversion of 1% Mo/Ru/PW-C catalyst was 59.6%, the selectivity of C3 alcohol was 96.1%, and the selectivity of propanediol (1,2(3)-propanediol) was 94.9%. It is noteworthy that the selectivity of 1,3-propanediol reached 20.7% when the PW was 21.07% (mass). This study provides experimental evidence for the tandem dehydration and hydrogenation mechanism of the multifunctional Mo/Ru/PW-C catalyst.

关键词: Heterogeneous catalysis, Bimetallic catalyst, Glycerol hydrogenolysis, Ruthenium, Molybdenum, Phosphotungstic acid

Guoxiao Cai, Wei Xiong, Susu Zhou, Pingle Liu, Yang Lv, Fang Hao, Hean Luo, ChangYi Kong. A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol[J]. Chinese Journal of Chemical Engineering, 2022, 51(11): 199-215.

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A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

A multi-functional Ru Mo bimetallic catalyst for ultra-efficient C3 alcohols production from liquid phase hydrogenolysis of glycerol

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