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Utilizing bimetallic catalysts to mitigate coke formation in dry reforming of methane

Journal of Energy Chemistry 2022年第5期31卷 124-142页

作者： Jaylin Sasson Bitters Tina He Elizabeth Nestler Sanjaya D.Senanayake Jingguang G.Chen Cheng Zhang College of Liberal Arts and Sciences Long Island University(Post)BrookvilleNY 11548United States Department of Molecular Biosciences University of Texas at AustinAustinTX 78712United States Chemistry Division Brookhaven National LaboratoryUptonNY 11973United States Department of Chemical Engineering Columbia UniversityNew YorkNY 10027United States

Dry reforming of methane(DRM) involves the conversion of carbon dioxide(CO_(2)) and methane(CH_(4)) into syngas(a mixture of hydrogen, H_(2), and carbon monoxide, CO), which can then be used to produce a wide range of products by means of Fischer–Tropsch synthesis. DRM has gained much attention as a means of mitigating damage from anthropogenic greenhouse gas(GHGs) emissions to the environment and instead utilizing these gases as precursors for value-added chemicals or to synthesize sustainable fuels and chemicals. Carbon deposition or coke formation, a primary cause of catalyst deactivation, has proven to be a major challenge in the development of DRM catalysts. The use of nickel-and cobalt-based catalysts has been extensively explored for DRM for their high activity and low cost but suffer from poor stability due to coke formation that has hindered their commercialization. Numerous articles have reviewed the various aspects of catalyst deactivation and strategies for mitigation, but few has focused on the benefit of bimetallic catalysts for mitigating coke formation. Bimetallic catalysts, often improve the catalytic stability over their monometallic counterparts due to synergistic effects resulting from two metal-tometal interactions. This review will cover DRM literature for various bimetallic catalyst systems, including the effect of supports and promoters, on the mitigation of carbonaceous deactivation.

关键词： Dry reforming of methane Carbon dioxide Bimetallic catalysts coke formation Catalyst stability

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Influence of catalyst support structure on ethene/decene metathesis and coke formation over WO_3/SiO_2 catalyst

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Petroleum Science 2013年第1期10卷 112-119页

作者： Zheng Min Chen Sheng-Li Zhang Jun-Hui Liu Yan Sang Lei You Ju Wang Xiao-Dong State Key Laboratory of Heavy Oil Processing China University of Petroleum

8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-visible diffuse reflectance spectroscopy （DRS） and scanning transmission electron microscopy-high-angle annular dark field （STEM HAADF）. The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure： The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.

关键词： Metathesis WO3/SiO2 catalysts pore structure coke formation

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Inhibition of coke formation in Cracking of 2-Methylpentane on USHY by Addition of Steam

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Chinese Journal of Chemical Engineering 2008年第5期16卷 726-732页

作者：赵迎宪危凤虞影 Ningbo Institute of Technology Zhejiang University Ningbo 315100 China

The effect of steam dilution on the formation of coke and minor products in 2-methylpenatne cracking on ultra stable HY at 673 K has been studied. The results show that steam dilution suppresses the formation of coke and minor aromatic products, but enhances the H/C atomic ratio of coke and the production of di-olefins. This and other evidences suggest that steam dilution enhances the desorption of coke precursors, diolefinic ions and cyclic ions, by inhibiting the further pathological reactions to produce aromatics and polyaromatics. These insights into the chemistry underlying coke formation in hydrocarbon cracking on solid acid catalysts can potentially be applied to the development of additives which inhibit coke formation and control catalyst deactivation.

关键词： 2-methylpentane catalytic cracking coke formation steam dilution inhibition

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Effect of Ni loadings on the activity and coke formation of MgO-modified Ni/Al_2O_3 nanocatalyst in dry reforming of methane

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Journal of Energy Chemistry 2014年第5期23卷 633-638页

作者： Zahra Alipour Mehran Rezaei Fereshteh Meshkani Catalyst and Advanced Materials Research Laboratory Chemical Engineering Department Faculty of Engineering University of Kashan Institute of Nanoscience and Nanotechnology University of Kashan

MgO-modified Ni/Al2O3 catalysts with different Ni loadings were prepared and employed in dry reforming of methane （DRM）. The effect of Ni loadings on the activity and coke formation of Ni/MgO-A1203 catalysts were investigated. The synthesized catalysts were characterized by XRD, N2 adsorption-desorption, SEM, TPO and TPR techniques. The obtained results showed that increasing nickel loading decreased the BET surface area and increased the catalytic activity and amount of deposited carbon. In addition, the effect of gas hourly space velocity （GHSV） and feed ratio were studied.

关键词： nickel catalyst MgO modifier syngas dry reforming coke formation

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Intrinsic properties of active sites for hydrogen production from alcohols without coke formation

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Journal of Energy Chemistry 2013年第3期22卷 436-445页

作者： Zhong He Xianqin Wang Department of Chemical Biological and Pharmaceutical EngineeringNew Jersey Institute of TechnologyNewarkNew Jersey 07102USA

The detailed reaction pathway and coke formation mechanism over Pt/metal oxide nanoparticles during the steam reforming of ethanol （SRE） at 300℃ were studied. The catalysts were prepared by incipient wetness impregnation method and were characterized with CO pulse chemisorption, BET surface measurement, oxygen adsorption, ethanol-TPD, NH3-TPD, and TPO. The SRE activity of the catalysts with steam/ethanol molar ratio of 3/1 was tested using a continuous fixed-bed reactor. Strong interaction between Pt and supports causes lower H2 production temperatures and no C2H4 formation, while weak interaction leads to C2H4 formation and strong bonded CO on Pt particles during ethanol- TPD. H2 production over Pt-based catalysts is mainly resulted from the decomposition and dehydrogenation of ethanol, and decarbonylation of acetaldehyde. Meanwhile, coke can be formed from acetaldehyde, acetone, C2H4 and CO. However, when the interaction between Pt and supports is weak, more coke is formed especially from acetone, C2H4 and CO. When the interaction is strong, no coke formation is observed due to high oxygen storage capacity of the catalyst.

关键词： active sites hydrogen alcohols coke formation Pt interaction

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Overcoming coke formation in high-temperature CO_(2)electrolysis

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Chinese Journal of Catalysis 2022年第12期43卷 2938-2945页

作者： Tongbao Wang Guangtai Han Ziyun Wang Yuhang Wang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123JiangsuChina School of Chemical Sciences University of AucklandAuckland 1010New Zealand

High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical ***,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and *** with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating *** recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode *** investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy *** research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability ***,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.

关键词： High-temperature CO_(2)electroreduction Solid oxide electrochemical cell coke formation Boudouard reaction Stability

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Syngas production from chemical looping reforming of ethanol over iron-based oxygen carriers: Theoretical analysis and experimental investigation

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Chinese Journal of Chemical Engineering 2021年第10期34卷 123-131页

作者： Atif Abdalazeez Wenju Wang Siddig Abuelgasim School of Energy and Power Engineering Nanjing University of Science and TechnologyNanjing 210094China Department of Mechanical Engineering University of KassalaKassalaSudan

Chemical looping reforming(CLR)is a recent trend for syngas production,which has several merits compared to the conventional *** of the most important issues for CLR is to find low-cost material as oxygen carriers,so iron is a promising *** paper contributes to testing the thermodynamic ability of iron-based oxygen carrier for chemical looping reforming of ethanol(CLRE).Iron thermodynamically investigated in temperature 100–1300℃and excess oxygen number(φ)0–*** was found that the temperature andφhave an apparent effect on the gaseous composition produced from the *** in temperature within the range of 100–1300℃enhanced syngas generated and reduced coke formation and ***,increasedφ,particularly at higher temperatures,had also enhanced syngas production as well as reduced coke ***,increasingφfor values beyond one had decreased syngas and not significantly reduced coke ***,an experimental investigation was carried out in a fixed bed reactor for more in-depth verification of iron ability as an oxygen carrier through using magnetite ore(mainly Fe3O4).It found that the effect of temperature on syngas production was consistent with that calculated thermodynamically,as syngas increased with raising the temperature through the CLRE.

关键词： Syngas Chemical looping reforming Iron oxygen carrier Ethanol coke formation Thermodynamic analysis

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Improvement strategies for Ni-based alcohol steam reforming catalysts

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Journal of Energy Chemistry 2023年第11期86卷 447-479,I0010页

作者： Alex Desgagnés Ommolbanin Alizadeh Sahraei Maria C.Iliuta UniversitéLaval Département de Génie Chimique1065 Avenue de la MédecineQuébecQC G1V 0A6Canada

Steam reforming(SR)of fossil methane is already a well-known,documented and established expertise in the industrial sector as it accounts for the vast majority of global hydrogen *** a sustainable development perspective,hydrogen production by SR of biomass-derived feedstock represents a promising alternative that could help to lower the carbon footprint of the traditional *** this regard,bio-alcohols such as methanol,ethanol or glycerol are among the attractive candidates that could serve as green hydrogen carriers as they decompose at relatively low temperatures in the presence of water compared to methane,allowing for improved H_(2)***,significant challenges remain regarding the activity and stability of nickel-based catalysts,which are most widely used in alcohol SR processes due to their affordability and ability to break C–C,O–H and C–H bonds,yet are prone to rapid deactivation primarily caused by coke deposition and metal particle *** this state-of-the-art review,a portfolio of strategies to improve the performance of Ni-based catalysts used in alcohol SR processes is unfolded with the intent of pinpointing the critical issues in catalyst *** examination of the literature reveals that the efforts tackling these recurring issues can be directed at the active metal,either by tuning Ni dispersion and Ni-support interactions or by targeting synergistic effects in bimetallic systems,while others focus on the support,either by modifying acid-base character,oxygen mobility,or by embedding Ni in specific crystallographic *** review provides a very useful tool to orient future work in catalyst development.

关键词： H2 production Alcohol steam reforming Ni-based catalysts Catalyst development Sintering coke formation

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The effect of FER zeolite acid sites in methanol-to-dimethyl-ether catalytic dehydration

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Journal of Energy Chemistry 2017年第3期26卷 406-415页

作者： Enrico Catizzone Alfredo Aloise Massimo Migliori Girolamo Giordano Department of Environmental and Chemical Engineering University of CalabriaVia P.BucciCubo 42aI-87036 RendeCSItaly

In this paper, the effect of acidity of zeolites with FER framework was studied in the methanol dehydration to dimethyl ether reaction, by comparing catalysts with different Si/Al ratios(namely 8, 30 and60). The aim of this work was to investigate how the acid sites concentration, strength, distribution and typology(Br?nsted and Lewis) affect methanol conversion, DME selectivity and coke formation. It was found that the aluminium content affects slightly acid sites strength whilst a relevant effect on acid sites concentration and distribution(Br?nsted/Lewis) was observed as 24% of Lewis sites were found on Alrichest samples, whilst less than 10% of Lewis acid sites were observed on FER at higher Si/Al ratio. All the investigated catalyst samples showed a selectivity toward DME always greater than 0.9 and samples with the lowest Si/Al ratio exhibit the best performances in terms of methanol conversion, approaching the theoretical equilibrium value(around 0.85) at temperatures below 200 °C. Turnover-frequency analysis suggests that this result seems to be related not only to the higher amount of acid sites but also that the presence of Lewis acid sites may play a significant role in converting methanol. On the other hand, the presence of Lewis acid sites, combined with a high acidity, promote the formation of by-products(mainly methane) and coke deposition during the reaction. As final evidence, all the investigated catalysts exhibit very high resistance to deactivation by coke deposition, over 60 h continuous test, and a GC–MS analysis of the coke deposited on the catalyst surface reveals tetra-methyl benzene as main component.

关键词： Methanol dehydration Dimethyl ether Lewis acid sites FER zeolite coke formation

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Studies on accelerated deactivation of ruthenium-promoted alumina-supported alkalized cobalt Fischer-Tropsch synthesis catalyst

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Journal of Natural Gas Chemistry 2011年第1期20卷 65-71页

作者： Shohreh Tehrani Mohamad Irani Ahmad Tavasoli Yadollah Mortazavi Abbas A. Khodadadi Ali Nakhaei Pour Research Institute of Petroleum Industry Department of Chemical Engineering College of Engineering University of Tehran School of Chemistry College of Science University of Tehran

Accelerated deactivation of ruthenium-promoted alumina-supported alkalized cobalt （K-Ru-Co/γ-Al 2 O 3 ） Fischer-Tropsch （FT） synthesis catalyst along the catalytic bed over 120 h of time-on-stream （TOS） was investigated. Catalytic bed was divided into three parts and structural changes of the spent catalysts collected from each catalytic bed after FT synthesis were studied using different techniques. Rapid deactivation was observed during the reaction due to high reaction temperature and low feed flow rates. The physico-chemical properties of the catalyst charged in the Bed #1 of the reactor did not change significantly. Interaction of cobalt with alumina and the formation of CoAl 2 O 4 increased along the catalytic bed. Reducibility percentage decreased by 4.5%, 7.5% and 12.9% for the catalysts in the Beds #1, #2 and #3, respectively. Dispersion decreased by 8.8%, 14.4% and 26.6% for the catalysts in the Beds #1, #2 and #3, respectively. Particle diameter increased by 0.6%, 2.4% and 10.4% for the catalysts in the Beds #1, #2 and #3, respectively, suggesting higher rate of sintering at the last catalytic bed. The amount of coke at the last catalytic bed was significantly higher than those of Beds #1 and #2.

关键词： Fischer-Tropsch synthesis cobalt accelerated deactivation sintering coke formation

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