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Understanding the catalytic performance and deactivation behaviour of second-promoter doped Pt/WO_(χ)/γ-Al_(2)O_(3) catalysts in the glycerol hydrogenolysis for selective and cleaner production of 1,3-propanediol

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Journal of Energy Chemistry 2024年第7期94卷 486-507页

作者： Rafik Rajjak Shaikh Sittichai Damruang Rais Ahmad Khan Supareak Praserthdam Piyasan Praserthdam Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC) Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailand Department of Chemistry College of ScienceKing Saud UniversityP.O.Box 2455Riyadh 11451Saudi Arabia High-Performance Computing Unit(CECC-HCU) Centre of Excellence on Catalysis and Catalytic Reaction Engineering(CECC)Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailand

The selective aqueous-phase glycerol hydrogenolysis is a promising reaction to produce commercially useful 1,3-propanediol(1,3-PDO).The Pt-WOx bifunctional catalyst can catalyse the glycerol hydrogenol-ysis but the catalyst deactivation via sintering,metal leaching,and coking can predominantly occur in the aqueous phase *** this work,the effect of reaction temperature,pressure and second promoter(Cu,Fe,Rh,Mn,Re,Ru,Ir,Sn,B,and P)on catalytic performance and deactivation behaviour of Pt/WOx/-Al2O3 was *** doped with Rh,Mn,Re,Ru,Ir,B,and P,the second promoter boosts catalytic activity by promoting great dispersion of Pt on support and increasing Pt surface *** increased Bronsted acid sites lead to selective synthesis of 1,3-PDO than 1,2-propanediol(1,2-PDO).The characterization studies of fresh and spent catalysts reveal that the main cause of catalyst deactivation is the Pt sintering,as interpreted based on XRD,CO chemisorption,and TEM *** Pt sintering is affected depending on the second promoter that can either or reduce the interaction between Pt,WO_(χ)/γ and Al_(2)O_(3).As an electron acceptor of Pt in Pt/WO_(χ)/γ-Al_(2)O_(3),Re and Mn as second promoters resulted in increased Pt^(2+) on the catalytic surface,which strengthens the contact between Pt andγ-Al_(2)O_(3) and WO_(χ),resulting in a decrease in Pt *** metal leaching and coking are not affected by the presence of second *** catalyst modified with a second promoter possesses improved catalytic activity and 1,3-PDO production,however the stability continues to remain a *** present work unrav-elled the determining parameters of catalytic activity and deactivation,thus providing a promising pro-tocol toward effective catalysts for glycerol hydrogenolysis.

关键词： glycerol hydrogenolysis 1,3-propanediol Metal-support interaction Second promoter Liquid phase Catalyst deactivation

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Enhanced recycling performance of bimetallic Ir-Re/SiO_(2) catalyst by amberlyst-15 for glycerol hydrogenolysis

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Chinese Journal of Chemical Engineering 2022年第5期35卷 171-181页

作者： Xin Ren Li Leng Yueqiang Cao Jing Zhang Xuezhi Duan Xueqing Gong Jinghong Zhou Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China

Recycling performance of heterogeneous catalysts is of crucial importance especially for a batch reaction *** this work,we demonstrate a strategy for enhancing recycling performance of Ir-Re/SiO_(2) catalyst synergized with amberlyst-15 in glycerol hydrogenolysis to produce 1,*** characterization results reveal that the Re sites in the Ir-Re/SiO_(2) catalyst undergo irreversible segregation and *** hinder the formation of active ReAOH species and thus contribute to a complete and irreversible ***,the introduction of amberlyst-15 into the reactant mixture can restrain the oxidation process of Re sites and favor the formation of ReAOH species,and thus significantly enhance the catalytic recycling *** results demonstrated here could guide the development of excellent bimetallic catalysts with the desirable recycling performances for the reaction.

关键词： glycerol hydrogenolysis Ir-Re/SiO_(2)catalyst Deactivation mechanism Recycling performance Amberlyst-15 promoter

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Thermodynamics of glycerol hydrogenolysis to propanediols over supported copper clusters: Insights from first-principles study

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Science China Chemistry 2013年第6期56卷 763-772页

作者： GUAN Jing WANG XiCheng WANG XiaoYan MU XinDong Key Laboratory of Biofuels Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of Sciences

Copper catalysts supported on metal oxides display unique efficiency and selectivity in catalyzing glycerol hydrogenolysis to propanediols. Understanding the reaction at the molecular level is the key to rational design of better catalysts for propanediol synthesis, which is one of the major challenges for glycerol application in energy. In this work, extensive calculations based on periodic density functional theory were carried out to study thermodynamics of glycerol hydrogenolysis over binary model catalysts, including Cu/ZrO2 and Cu/MgO, with the focus to elucidate the competitive reaction pathways to produce the 1,2-propanediol (1,2-PDO) and 1,3-propanediol (1,3-PDO). Our results suggest that the reaction starts with glycerol dehydration on the metal oxide, followed by sequential hydrogenation over metal centers. Based on our explorations on the stabilities of adsorbed reactants, dehydrated intermediates and hydrogenated species along the reaction channels, the DFT calculations show that the 1,2-PDO formation will dominate in comparison to the 1,3-PDO from thermodynamic viewpoint. This is consistent with our experiments where the Cu catalysts seem to give the 1,2-PDO as a main product. The calculations and experiments also indicate that the Cu/MgO exhibits superior activities than Cu/ZrO2 for the hydrogenolysis of glycerol molecules.

关键词： density functional calculations glycerol hydrogenolysis propanediols copper-based catalysts mechanism

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

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Chinese Journal of Chemical Engineering 2022年第11期51卷 199-215页

作者： Guoxiao Cai Wei Xiong Susu Zhou Pingle Liu Yang Lv Fang Hao Hean Luo ChangYi Kong College of Chemical Engineering National&Local United Engineering Research Centre for Chemical Process Simulation and IntensificationXiangtan UniversityXiangtan 411105China Department of Environment and Energy System Graduate School of Science and TechnologyShizuoka University3-5-1 JohokuNaka-kuHamamatsu 432-8561Japan

Ru and Mo bimetallic catalysts supported on active carbon modified by phosphotungstic acid(PW)were designed and applied in glycerol hydrogenolysis *** physicochemical properties of the catalysts were characterized and the presence of active sites was investigated from the perspective of the glycerol hydrogenolysis *** MoOxis highly selective for the C—O bond cleavage of glycerol molecules,which can reasonably regulate the strong C—C bond cleavage activity of Ru *** using sequential deposition of Ru and Mo supported on mesoporous PW-C,the characterization results show that the combination of isolated low-valence MoOxwith metal Ru particles can form“MoOx-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

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hydrogenolysis of glycerol over HY zeolite supported Ru catalysts

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Journal of Energy Chemistry 2014年第2期23卷 185-192页

作者： Shaohua Jin Zihui Xiao Chuang Li Christopher T.Williams Changhai Liang Laboratory of Advanced Materials and Catalytic Engineering School of Chemical EngineeringDalian University of Technology Department of Chemical Engineering University of South Carolina

An enhanced active and selective catalyst consisting of ruthenium supported on dealuminated HY zeolite has been prepared by a wet im- pregnation method. It was found that BET surface area of Ru/HY catalysts significantly increases after HC1 treatment. This treatment also increases the concentration of strong acid sites in the catalyst. The hydrogenolysis of glycerol over 5 wt% Ru/HY catalyst was investigated at 190-220℃ , an initial H2 pressure of 3-6 MPa, and in 20 wt% glycerol aqueous solution, The results indicate that HC1 treated Ru/HY catalyst shows higher activity compared with the untreated Ru/HY catalyst, and that the glycerol hydrogenolysis efficiency is influenced by the porosity and acidity of the support. A selectivity to 1,2-PDO of 81.3% at a glycerol conversion of 60.1% under 3 MPa H2 pressure and 220 ℃ for 10 h was achieved over the modified Ru/HY catalyst with a 1.0 mol/L HC1 treatment. It has also been shown that a longer reaction time, a higher temperature and a higher H2 pressure have the positive effects on the glycerol hydrogenolysis efficiency of the enhanced Ru/HY.

关键词： ruthenium HY zeolite impregnation modification glycerol hydrogenolysis

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