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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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A critical review towards the causes of the iron-based catalysts deactivation mechanisms in the selective oxidation of hydrogen sulfide to elemental sulfur from biogas

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Journal of Energy Chemistry 2024年第3期90卷 388-411,I0010页

作者： Mostafa Tarek Janaina S.Santos Victor Márquez Mohammad Fereidooni Mohammad Yazdanpanah Supareak praserthdam piyasan praserthdam Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC) Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailan High-Performance Computing Unit(CECC-HCU) Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC)Chulalongkorn UniversityBangkok 10330Thailand

Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low *** various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly *** to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant *** causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this *** focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S.

关键词： Selective oxidation of H_(2)S Iron-based Catalysts Mechanism of deactivation Sulfur or sulfate deposition Transformation of iron species Sintering SDG 7

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Effects of TiO_(2) Support and Cobalt Addition of Ni/TiO_(2) Catalyst in Selective Hydrogenation of Furfural to Furfuryl Alcohol

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Journal of Renewable Materials 2022年第8期10卷 2055-2072页

作者： Kittithad Wonglekha Weerachon Tolek Okorn Mekasuwandumrong Wasu Chaitree piyasan praserthdam Kiat Moon Lee Joongjai Panpranot Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok10330Thailand Department of Chemical Engineering Faculty of Engineering and Industrial TechnologySilpakorn UniversityNakorn Pathom73000Thailand Department of Chemical&Petroleum Engineering Faculty of EngineeringTechnology and Built EnvironmentUCSI UniversityKuala Lumpur56000Malaysia Bio-Circular-Green-Economy Technology&Engineering Center Faculty of EngineeringChulalongkorn UniversityBangkok10330Thailand

An effect of phase compositions(rutile,Rut and anatase,Ant)of TiO_(2)supports on the selective hydrogenation of furfural to furfuryl alcohol was *** 15%wt Ni/TiO_(2)catalysts were prepared by incipient impregnation *** result showed that Ni supported on anatase-rutile mixed phase TiO_(2)(91%Rut and 9%Ant,A2)provided the highest furfuryl alcohol yield at 43.8%due to the relatively strong Ni-TiO_(2)interaction,its appropriate crystallite sizes,and high average pore ***,the effect of cobalt as a promoter on Ni/TiO_(2)-A2 catalysts was *** result showed that the Ni-Co/TiO_(2)-A2 catalysts exhibited poorer catalyst performances compared to the monometallic Ni/TiO_(2),probably because addition of cobalt can lower the reduction temperatures of Ni/TiO_(2)and weaken the metal-support interaction.

关键词： Ni catalyst furfural hydrogenation TiO_(2) furfuryl alcohol cobalt

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Ti-Si composite oxide-supported cobalt catalysts for CO_2 hydrogenation

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Journal of Natural Gas Chemistry 2011年第5期20卷 558-564页

作者： Jakrapan Janlamool piyasan praserthdam Bunjerd Jongsomjit Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University

In the present work, different silica-based supported cobalt （Co） catalysts were synthesized and used for CO2 hydrogenation for methanation. Different supports, such as SSP, MCM-41, TiSSP and TiMCM were used to prepare Co catalysts with 20 wt% Co loading. The supports and catalysts were characterized by means of N2 physisorption, XRD, SEM/EDX, XPS, TPR and CO chemisorption. It is found that after calcination of catalysts, Ti is present in the form of anatase. The introduction of Ti plays important roles in the properties of Co catalysts by：（i） facilitating the reduction of Co oxides species which are strongly interacted with support, （ii） preventing the formation of silicate compounds, and （iii） inhibiting the RWGS reaction. Based on CO2 hydrogenation, the CoTiMCM catalyst exhibites the highest activity and stability.

关键词： CO2 hydrogenation titania-silica cobalt catalysts methanation

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Synergistic Effects of the ZnCl_2-SiCl_4 Modified TiCl_4/MgCl_2/THF Catalytic System on Ethylene/1-Hexene and Ethylene/1-Octene Copolymerizations

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Chinese Journal of Polymer Science 2014年第1期32卷 84-91页

作者： Wanna Phiwkliang Bunjerd Jongsomjit piyasan praserthdam Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University

The copolymerizations of ethylene with 1-hexene or 1-0ctene by using TiC14/MgCI2/THF catalysts modified with different metal halide additives （ZnCI2, SIC14, and the combined ZnC12-SiCl4） were investigated based on catalytic activity and copolymer properties. It was found that the catalyst modified with mixed ZnC12-SiC14 revealed the highest activities for both ethylene/1-hexene and ethylene/1-0ctene copolymerization. The increase in activities was due to the formation of acidic sites by modifying the catalysts with Lewis acids. Based on the FTIR measurements, the characteristic C--O--C peaks of the catalysts modified with metal halide additives were slightly shifted to lower wavenumber when compared to the unmodified catalyst. This showed that the modified catalysts could generate more acid sites in the TiC14/MgC12/THF catalytic system leading to an increase in activities as well as comonomer insertion （as proven by IaC-NMR）. However, Lewis acid- modifications did not affect the microstructure of the copolymers obtained. By comparison on the properties of copolymers prepared with the unmodified catalyst, it was found that polymers with ZnC12 and/or SIC14 modification exhibited a slight decrease in melting temperature, crystallinity and density. It is suggested that these results were obtained based on the different amount of ct-olefins insertion, regardless of the types of Lewis acids and comonomer.

关键词： Ziegler-Natta catalyst Lewis acid Copolymerization of ethylene with a-olefin SIC14 ZnC12.

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Role of support nature (γ-Al_2O_3 and SiO_2-Al_2O_3) on the performances of rhenium oxide catalysts in the metathesis of ethylene and 2-pentene

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Journal of Natural Gas Chemistry 2012年第2期21卷 158-164页

作者： Weena Phongsawat Benjamas Netiworaruksa Kongkiat Suriye Siraprapha Dokjampa piyasan praserthdam Joongjai Panpranot Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University SCG Chemicals CO. Ltd. 1 Siam Cement Rd. Bangsue Bangkok 10800 Thailand

The metathesis of ethylene and 2-pentene was studied as an alternative route for propylene production over Re2O7/γ-Al2O3 and Re2O7/SiO2-Al2O3 catalysts. Both NH3 temperature-programmed desorption （NH3-TPD） and H2 temperature-programmed reduction （H2-TPR） results showed that Re2O7/SiO2-Al2O3 exhibited stronger acidity and weaker metal-support interaction than Re2O7/γ-Al2O3. At 35 60℃, isomerization free metathesis was observed only over Re2O7/γ-Al2O3, suggesting that the formation of metal-carbene metathesis active sites required only weak acidity. Our results suggest that on the Re2O7/SiO2-Al2O3, hydrido-rhenium species （[Re]-H） were formed in addition to the metathesis active sites, resulting in the isomerization of the initial 1-butene product into 2-butenes. A subsequent secondary metathesis reaction between these 2-butenes and the excess ethylene could explain the enhanced yields of propylene observed. The results demonstrate the potential for high yield of propylene from alternative feedstocks.

关键词： metathesis isomerization propylene production 2-pentene rhenium

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Production of propylene from an unconventional metathesis of ethylene and 2-pentene over Re_2O_7/SiO_2-Al_2O_3 catalysts

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Journal of Natural Gas Chemistry 2012年第1期21卷 83-90页

作者： Weena Phongsawat Benjamas Netivorruksa Kongkiat Suriye Siraprapha Dokjampa piyasan praserthdam Joongjai Panpranot Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University SCG Chemicals CO. LTD. 1 Siam Cement Rd. Bangsue Bangkok 10800 Thailand

An unconventional metathesis of ethylene and 2-pentene over Re2O7/SiO2-A1203 catalysts has been studied as an alternative route for the production of propylene. Complete conversion of 2-pentene and propylene yield as high as 88 wt% were obtained under mild reaction conditions at 35 ℃ and atmospheric pressure. Unlike the conventional metathesis of ethylene and 2-butenes in which isomerization is a competing side reaction, the isomerization of 1-butene product from the unconventional metathesis of ethylene and 2-pentene to 2-butenes can further react with excess ethylene in the feed, resulting in additional increase in propylene yield. The secondary metathesis reaction was found to be favored under ethylene/2-pentene （E/2P） molar ratio ≥3 and gas hourly space velocity （GHSV） ≤ 1000 h-1 at the reaction temperature of 35 ℃. No catalyst deactivation was observed during the 455 min time-on-stream under the selected reaction conditions.

关键词： metathesis propylene production 2-pentene rhenium silica-alumina

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Cu/Mg-Al水滑石催化剂用于乙醇的氧化脱氢:乙醇浓度和还原条件的影响

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2020年第3期21卷 218-228页

作者： Piriya PINTHONG piyasan praserthdam Bunjerd JONGSOMJIT Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailand

目的:对现有的乙醇氧化脱氢体系中Mg-Al催化剂进行改进,以期获得更高的收率和产物选择性。创新点:1.制备Cu改性的Mg-Al催化剂用于乙醇氧化脱氢反应,获得了更高的乙醛收率和选择性;***/Mg-Al催化剂制备方法简单,制备价格低廉(无需贵金属)... 详细信息

目的:对现有的乙醇氧化脱氢体系中Mg-Al催化剂进行改进,以期获得更高的收率和产物选择性。创新点:1.制备Cu改性的Mg-Al催化剂用于乙醇氧化脱氢反应,获得了更高的乙醛收率和选择性;***/Mg-Al催化剂制备方法简单,制备价格低廉(无需贵金属),制备条件温和(无需高温高压);***/Mg-Al催化剂在使用前无需预还原。方法:1.采用共沉淀法和浸渍法制备Cu/Mg-Al催化剂;2.通过乙醇氧化脱氢反应对催化剂进行考评,以探究Cu改性、乙醇浓度和催化剂的还原条件对催化活性的影响。结论:1.与Mg-Al催化剂相比,经由Cu改性的Mg-Al催化剂的乙醇氧化脱氢活性显著提高;在350℃,乙醛最大收率为41.8%。2.进料气中水的存在(乙醇浓度下降)会对Cu/Mg-Al的催化性能产生不利影响,使得乙醇转化率和乙醛收率下降;但在高温区间(350~400℃),这个不利影响有所减弱。3.反应前,催化剂在氢气气氛下的还原步骤对Cu/Mg-Al催化活性的影响不明显。

关键词：氧化脱氢乙醇铜 Mg-Al水滑石乙醛催化剂

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POISONING OF ACTIVE SITES ON ZIEGLER-NATTA CATALYST FOR PROPYLENE POLYMERIZATION

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Chinese Journal of Polymer Science 2008年第5期26卷 547-552页

作者： Kitti Tangjituabun Sang Yull Kim Yuichi Hiraoka Toshiaki Taniike Minoru Terano Bunjerd Jongsomjit piyasan praserthdam School of Materials Science Japan Advanced Institute of Science and TechnologyIshikawa 923-1292Japan Department of Chemical Engineering Chulalongkorn UniversityBangkok 10330Thailand

The effects of poisoning materials on catalytic activity and isospecificity of the supported Ziegler-Natta catalyst were investigated.A minor amount of simple structure of Lewis base,i.e.,methanol,acetone,ethyl acetate,was introduced into the catalyst slurry for partial poisoning catalytic active *** was found that the variations in deactivation power were in the order of methanol>acetone>ethyl *** kinetic investigation via stopped-flow polymerization showed that poisoning compounds cau...

关键词： Poisoning material Ziegler-Natta catalyst Stopped-flow propylene polymerization

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NaOH 改性WO_3/SiO_2 催化剂催化2-丁烯和乙烯复分解制丙烯(英文)

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催化学报 2014年第2期35卷 232-241页

作者： Surasa Maksasithorn Damien P. Debecker piyasan praserthdam Joongjai Panpranot Kong- kiat Suriye Sirachaya Kunjara Na Ayudhya Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical EngineeringFaculty of EngineeringChulalongkorn University Institute of Condensed Matter and Nanoscience - Molecules Solids and Reactivity (IMCN/MOST)Université catholique de Louvain SCG Chemicals Co.Ltd

A WO3 /SiO2 catalyst is used in industry to produce propylene from 2-butene and ethylene metathe-sis. Catalysts with various WO3 loading(4% to 10%) were prepared by impregnation and tested for the metathesis of ethene and trans-2-butene. Ion exchange of NaOH onto the WO3/SiO2 catalyst was used to mitigate the acidity of the catalysts in a controlled way. At low WO3 loading, the treatment with large amounts of NaOH resulted in a significant decrease in metathesis activity concomitant with significant W leaching and marked structural changes(XRD, Raman). At higher WO3 loading (6% to 10%), the treatment with NaOH mainly resulted in a decrease in acidity. FT-IR experiments after adsorption of pyridine showed that the Lewis acidic sites were poisoned by sodium. Never-theless, the metathesis activity remained constant after the NaOH treatment. This suggested that the remaining acidity on the catalyst was enough to ensure the efficient formation of the carbene active sites. Interestingly, Na poisoning resulted in some modification of the selectivity. The mitigation of acidity was shown to favor propene selectivity over the formation of isomerization products (cis-2-butene, 1-butene, etc.). Moreover, treatment with NaOH led to a shorter induction period and reduced coke formation on the WO3 /SiO2 catalyst.

关键词：复分解反应氢氧化钠催化剂丁烯丙烯乙烯生产 NaOH

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