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合成条件对无外部氢气输入时甘油水相氢解反应中Ni/CeO催化性能的影响

Influence of Synthesis Conditions on Catalytic Performance of Ni/CeO in Aqueous-Phase Hydrogenolysis of Glycerol without External Hydrogen Input.

作者信息

Jarauta-Córdoba Clara, García Lucía, Ruiz Joaquín, Oliva Miriam, Arauzo Jesús

机构信息

CIRCE-Energy Resources and Consumption Technology Center, Parque Empresarial Dinamiza, Avda. Ranillas 3D, 1st Floor, 50018 Zaragoza, Spain.

Thermochemical Processes Group (GPT), Aragon Institute of Engineering Research (I3A), Universidad de Zaragoza, Mariano Esquillor S/N, 50018 Zaragoza, Spain.

出版信息

Molecules. 2024 Aug 10;29(16):3797. doi: 10.3390/molecules29163797.

Abstract

The aqueous-phase hydrogenolysis of glycerol was studied in Ni/CeO catalytic systems prepared by incipient wetness impregnation. The operating conditions were 34 bar, 227 ºC, 5 wt.% of glycerol, and a W/m = 20 g catalyst min/g glycerol without a hydrogen supply. The effect of the catalyst preparation conditions on the catalytic activity and physicochemical properties of the catalysts was assessed, particularly the calcination temperature of the support, the calcination temperature of the catalyst, and the Ni content. The physicochemical properties of the catalysts were determined by N adsorption, H-TPR, NH-TPD, and XRD, among other techniques. A relevant increase in acidity was observed when increasing the nickel content up to 20 wt.%. The increase in the calcination temperatures of the supports and catalysts showed a detrimental effect on the specific surface area and acid properties of the catalysts, which were crucial to the selectivity of the reaction. These catalysts notably enhanced the yield of liquid products, achieving global glycerol conversion values ranging from 17.1 to 29.0% and carbon yield to liquids ranging from 12.6 to 24.0%. Acetol and 1,2-propanediol were the most abundant products obtained in the liquid stream.

摘要

在采用初湿浸渍法制备的Ni/CeO催化体系中研究了甘油的水相氢解反应。操作条件为34巴、227℃、5 wt.%的甘油,且在不供应氢气的情况下W/m = 20 g催化剂/分钟/g甘油。评估了催化剂制备条件对催化剂催化活性和物理化学性质的影响,特别是载体的煅烧温度、催化剂的煅烧温度和镍含量。通过N吸附、H-TPR、NH-TPD和XRD等技术测定了催化剂的物理化学性质。当镍含量增加到20 wt.%时,观察到酸度有显著增加。载体和催化剂煅烧温度的升高对催化剂的比表面积和酸性性质产生了不利影响,而这些性质对反应的选择性至关重要。这些催化剂显著提高了液体产物的产率,甘油的总转化率在17.1%至29.0%之间,液体产物的碳产率在12.6%至24.0%之间。丙酮醇和1,2-丙二醇是液流中获得的最主要产物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c104/11357132/d17221b7f9fa/molecules-29-03797-g001.jpg

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