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Synthesis of lanthanum oxide supported transition metal-based catalysts for clean hydrogen production: The role of reducibility 氧化镧负载过渡金属基清洁制氢催化剂的合成:还原性的作用
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-12 DOI: 10.1016/j.cattod.2025.115277
Wasim Ullah Khan , Dwi Hantoko , Shakeel Ahmed , Ahmed Al Shoaibi , Srinivasakannan Chandrasekar , Mohammad Mozahar Hossain
{"title":"Synthesis of lanthanum oxide supported transition metal-based catalysts for clean hydrogen production: The role of reducibility","authors":"Wasim Ullah Khan ,&nbsp;Dwi Hantoko ,&nbsp;Shakeel Ahmed ,&nbsp;Ahmed Al Shoaibi ,&nbsp;Srinivasakannan Chandrasekar ,&nbsp;Mohammad Mozahar Hossain","doi":"10.1016/j.cattod.2025.115277","DOIUrl":"10.1016/j.cattod.2025.115277","url":null,"abstract":"<div><div>Transition metal-based catalysts containing 20 wt% of nickel, cobalt, iron, and molybdenum doped over lanthanum dioxide (La<sub>2</sub>O<sub>3</sub>) were investigated for clean hydrogen production. The diffraction patterns showed the formation of corresponding metal oxides and their spinel species. The reduction profiles indicated the unique initial reduction temperatures that played a role in the catalytic performance. The activity profiles indicated that nickel-based catalyst (Ni-La) outperformed the rest of the catalysts with an initial activity of 82.3 % that reaches 83.6 % at the end of 170 min time-on-stream. The rest of the catalysts suffered deactivation over time and hence Ni-La turned out to be the active and stable catalyst among the tested catalysts. The high-resolution transition electron microscopy images of the best performing catalyst (Ni-La) revealed the growth of multiwalled carbon nanotubes and carbon formation followed simultaneously tip- as well as base-growth mechanisms.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115277"},"PeriodicalIF":5.2,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143636617","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Operando FT-IR and UV–vis spectroscopic studies emphasise the nature of coke species formed over SSZ-13 zeolite during ethanol-to-hydrocarbons process Operando FT-IR和UV-vis光谱研究强调了SSZ-13沸石在乙醇制烃过程中形成的焦炭物种的性质
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-12 DOI: 10.1016/j.cattod.2025.115274
Karolina A. Tarach , Anna Walczyk , Agata Olszewska , Julia Sobalska , Oliwia Rogala , Kinga Góra-Marek
{"title":"Operando FT-IR and UV–vis spectroscopic studies emphasise the nature of coke species formed over SSZ-13 zeolite during ethanol-to-hydrocarbons process","authors":"Karolina A. Tarach ,&nbsp;Anna Walczyk ,&nbsp;Agata Olszewska ,&nbsp;Julia Sobalska ,&nbsp;Oliwia Rogala ,&nbsp;Kinga Góra-Marek","doi":"10.1016/j.cattod.2025.115274","DOIUrl":"10.1016/j.cattod.2025.115274","url":null,"abstract":"<div><div>This study investigates the conversion of ethanol to higher olefins using protonic chabazite (SSZ-13, SiAl = 8) zeolite, employing advanced FT-IR and UV–vis operando spectroscopic techniques, with concurrent mass spectrometry and gas chromatography examinations of the products. The utilisation of varying ethanol loads facilitates the examination of coke production and its progression relative to the feed quantity. The spectroscopic analysis clarifies the species formed on the catalyst's surface, while mass spectrometry and gas chromatography techniques verify the desorbed products. The counterparts in transforming ethanol and methanol to olefins via the recognised intermediates of the hydrocarbon pool mechanism are identified and examined in detail. Significant value-added information is obtained from in situ FT-IR studies complemented by mass spectrometry examination of the gas phase. The MCR-ALS analysis is utilised in spectroscopic operando investigations and offers significant insights into the findings. Furthermore, these investigations are substantiated by chromatographic examination of coke species obtained from spent catalysts.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115274"},"PeriodicalIF":5.2,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143637597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Iron-doped carbon nanotubes via microwave shock: Recyclability in polypropylene pyrolysis for ORR catalyst manufacturing 微波冲击铁掺杂碳纳米管:聚丙烯热解制备ORR催化剂的可回收性
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-10 DOI: 10.1016/j.cattod.2025.115271
Xi Shen , Zhenyu Zhao , Hong Li , Xin Gao
{"title":"Iron-doped carbon nanotubes via microwave shock: Recyclability in polypropylene pyrolysis for ORR catalyst manufacturing","authors":"Xi Shen ,&nbsp;Zhenyu Zhao ,&nbsp;Hong Li ,&nbsp;Xin Gao","doi":"10.1016/j.cattod.2025.115271","DOIUrl":"10.1016/j.cattod.2025.115271","url":null,"abstract":"<div><div>The recycling and upcycling of waste plastics into high-value products by pyrolysis is a critical challenge caused by its time/energy-consuming problems, which can be overcome by employing microwave-assisted catalytic pyrolysis due to its rapid pyrolysis rates and high product yields. This study presents a facile method for the synthesis of catalysts for microwave-assisted pyrolysis of waste plastics, utilizing the pyrolytic products as raw materials. In this case, a microwave thermal shock strategy is developed to efficiently anchor iron nanoparticles on carbon nanotubes (CNTs). This method recycles a portion of pyrolysis products back into the catalyst pool for plastic transformation into new CNTs, reducing the consumption for preparing additional catalysts. The precursors exposed to 50 W microwave irradiation reaches above 2000 °C within seconds, allowing Fe nanoparticles to be uniformly impregnated within the carbon nanotube matrix. The formed iron-doped CNTs shows high activity for microwave-assisted pyrolysis, generating CNTs with D/G ratios at 0.31. The recycling and reconstruction of CNTs after multiple pyrolysis form a cross-lined network structure, which facilitates electron transition and can be utilized for fabricating electrocatalysts. Nitrogen doping further improves the onset potential to 0.923 V vs. RHE, making them viable candidates for electrocatalytic applications in oxygen reduction reactions. In summary, our findings demonstrate the feasibility of this approach to reactive pyrolysis products that serve as catalysis for microwave-assisted pyrolysis, with the potential to reduce volatile organic compound emissions and capital expenditure in catalyst preparation, offering a greener and more efficient pathway for plastic waste management and catalyst production.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115271"},"PeriodicalIF":5.2,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143621062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optimizing Sorption Enhanced Methanation (SEM) of CO2 with Ni3Fe + LTA 5 A mixtures Ni3Fe + lta5 A混合物对CO2吸附强化甲烷化(SEM)的优化
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-10 DOI: 10.1016/j.cattod.2025.115262
V.D. Mercader, P. Aragüés-Aldea, P. Durán, E. Francés, J. Herguido, J.A. Peña
{"title":"Optimizing Sorption Enhanced Methanation (SEM) of CO2 with Ni3Fe + LTA 5 A mixtures","authors":"V.D. Mercader,&nbsp;P. Aragüés-Aldea,&nbsp;P. Durán,&nbsp;E. Francés,&nbsp;J. Herguido,&nbsp;J.A. Peña","doi":"10.1016/j.cattod.2025.115262","DOIUrl":"10.1016/j.cattod.2025.115262","url":null,"abstract":"<div><div>This study investigates the integration of catalytic CO<sub>2</sub> methanation and water adsorption using a Ni-Fe-based catalyst and LTA 5 A zeolite to enhance methane production via the Sabatier reaction. By mitigating thermodynamic limitations through <em>in situ</em> water removal, the research explores key operational parameters, including temperature, space velocity, and H₂:CO₂ feed ratios, to optimize process performance. The findings highlight that a temperature of 300 °C, a <em>WHSV</em> of 1.50 × 10<sup>4</sup> (STP) mL·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup> (4.86 g<sub>CO2</sub>·g<sub>cat</sub>⁻¹·h⁻¹), and a H₂:CO₂ molar ratio equal to 5:1, result in enhanced methane yields, shifting thermodynamic equilibrium due to water sorption during initial stages. The presence of methane in the feed, representative of a biogas, demonstrated negligible effects on methane yields under optimal conditions, underscoring the method’s feasibility for direct biogas upgrading. While the process achieved significant intensification, challenges such as loss of activity of the bed of solids (catalyst plus water adsorbent) were identified, necessitating further advancements in both catalyst and adsorbent stability, as well as a deeper study on their interaction. The study provides a pathway for scaling up adsorption-enhanced methanation technologies to achieve renewable methane production, addressing the dual goals of carbon management and energy storage.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115262"},"PeriodicalIF":5.2,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143643046","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanochemical vs impregnation synthesis of metal oxides from pyrolyzed MOFs in microwave-assisted methyl levulinate conversion to gamma-valerolactone 微波辅助乙酰丙酸甲酯转化- γ -戊内酯热解mof金属氧化物的机械化学与浸渍合成
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-06 DOI: 10.1016/j.cattod.2025.115260
Lidia López-Gómez , Marina Ronda-Leal , Salvador Pérez-Huertas , Antonio A. Romero , Rafael Luque
{"title":"Mechanochemical vs impregnation synthesis of metal oxides from pyrolyzed MOFs in microwave-assisted methyl levulinate conversion to gamma-valerolactone","authors":"Lidia López-Gómez ,&nbsp;Marina Ronda-Leal ,&nbsp;Salvador Pérez-Huertas ,&nbsp;Antonio A. Romero ,&nbsp;Rafael Luque","doi":"10.1016/j.cattod.2025.115260","DOIUrl":"10.1016/j.cattod.2025.115260","url":null,"abstract":"<div><div>A series of bimetallic oxides (Al<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub>@C) has been synthesized using a metal-organic-framework (NH<sub>2</sub>-UiO-66) as a sacrificial agent by both impregnation and mechanochemical methods. The synthesized materials were used in heterogeneous catalysis for the direct conversion of a promising biomass-based building block, i.e., methyl levulinate to γ-valerolactone (GVL). A complete set of characterization, including N<sub>2</sub> adsorption/desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR) was carried out. The incorporation of aluminum into the catalyst system led to a significant increase in the GVL yield. The conversion rate achieved with the mechanochemistry-based samples doubled that obtained by the impregnation samples. The material prepared via mechanochemistry with the larger Al<sub>2</sub>O<sub>3</sub>/ZrO<sub>2</sub> ratio exhibited the greatest catalytic activity, i.e., 79 % conversion and 87 % selectivity. GVL is considered a promising biomass-derived platform chemical for numerous applications, including bio-materials, fuels or fuel additives, and various chemical intermediates.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115260"},"PeriodicalIF":5.2,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143593644","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Super-dry reforming of methane over surface oxygen mobility enhanced Ni/MgO-Ce/SBA-15 catalysts 甲烷在表面氧迁移率上的超干重整增强了Ni/MgO-Ce/SBA-15催化剂
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-05 DOI: 10.1016/j.cattod.2025.115257
Ho-Ryong Park , Beom-Jun Kim , Su-Jin Ryu , Yukwon Jeon , Sang Soo Lee , Jong-Wook Bae , Hyun-Seog Roh
{"title":"Super-dry reforming of methane over surface oxygen mobility enhanced Ni/MgO-Ce/SBA-15 catalysts","authors":"Ho-Ryong Park ,&nbsp;Beom-Jun Kim ,&nbsp;Su-Jin Ryu ,&nbsp;Yukwon Jeon ,&nbsp;Sang Soo Lee ,&nbsp;Jong-Wook Bae ,&nbsp;Hyun-Seog Roh","doi":"10.1016/j.cattod.2025.115257","DOIUrl":"10.1016/j.cattod.2025.115257","url":null,"abstract":"<div><div>We developed a customized catalyst for the super-dry reforming of methane (S-DRM) reaction, designed to maximize CO<sub>2</sub> utilization compared to the conventional dry reforming of methane (DRM) reaction. The introduction of CeO<sub>2</sub> induced strong metal-support interactions (SMSI) in the Ni/MgO/SBA-15 catalyst, facilitating the high dispersion of Ni particles. Consequently, the crystallite size of metallic Ni (Ni<sup>0</sup>) was reduced, resulting in an increased number of Ni active sites. Furthermore, the incorporation of CeO<sub>2</sub> promoted the formation of oxygen vacancies (OVs), thereby enhancing CO<sub>2</sub> activation and improving the efficiency of the S-DRM reaction. As the CeO<sub>2</sub> content increased, the proportion of SBA-15 decreased, leading to a gradual reduction in surface area. However, at excessive CeO<sub>2</sub> content, a drastic decline in surface area was observed, which also resulted in a decrease in OVs that had previously shown an increasing trend with rising CeO<sub>2</sub> content. These changes could potentially diminish catalyst performance despite the enhanced SMSI. Therefore, maintaining an appropriate ratio of CeO<sub>2</sub>:SBA-15 is crucial for maximizing catalyst performance and ensuring prolonged stability. The optimal catalyst, NMCS250, effectively balanced these factors, exhibiting high Ni dispersion, increased OVs, and basicity, which contributed to excellent catalytic activity and stability. Overall, NMCS250 was identified as the optimal catalyst, demonstrating superior catalytic performance due to its elevated Ni dispersion, increased oxygen vacancies, and basicity.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115257"},"PeriodicalIF":5.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mg-modified Ni-based catalysts prepared by the solution combustion synthesis for dry reforming of methane 溶液燃烧合成甲烷干重整用镁改性镍基催化剂
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-04 DOI: 10.1016/j.cattod.2025.115261
Alua M. Manabayeva , Päivi Mäki-Arvela , Zuzana Vajglová , Mark Martinéz-Klimov , Olha Yevdokimova , Anssi Peuronen , Mika Lastusaari , Teija Tirri , Svetlana A. Tungatarova , Tolkyn S. Baizhumanova , Kaisar Kassymkan , Gulnar N. Kaumenova , Manapkhan Zhumabek , Daulet A. Zhumadullaev , Dinmukhamed Shoganbek , Dmitry Yu. Murzin
{"title":"Mg-modified Ni-based catalysts prepared by the solution combustion synthesis for dry reforming of methane","authors":"Alua M. Manabayeva ,&nbsp;Päivi Mäki-Arvela ,&nbsp;Zuzana Vajglová ,&nbsp;Mark Martinéz-Klimov ,&nbsp;Olha Yevdokimova ,&nbsp;Anssi Peuronen ,&nbsp;Mika Lastusaari ,&nbsp;Teija Tirri ,&nbsp;Svetlana A. Tungatarova ,&nbsp;Tolkyn S. Baizhumanova ,&nbsp;Kaisar Kassymkan ,&nbsp;Gulnar N. Kaumenova ,&nbsp;Manapkhan Zhumabek ,&nbsp;Daulet A. Zhumadullaev ,&nbsp;Dinmukhamed Shoganbek ,&nbsp;Dmitry Yu. Murzin","doi":"10.1016/j.cattod.2025.115261","DOIUrl":"10.1016/j.cattod.2025.115261","url":null,"abstract":"<div><div>In the current work, nickel and magnesia containing catalysts synthesized by solution combustion synthesis (SCS) and impregnation were used for dry reforming of methane (DRM). The present research showcased the difference of two preparation methods and demonstrated the influence of temperature cycling and various duration on the activity of Ni-Mg catalysts (30 min, 10 h, 20 h, 200 h TOS). It was reported that Ni-Mg-Al catalysts exhibited mainly crystalline MgAl<sub>2</sub>O<sub>4</sub> and nickel oxide in both fresh and spent catalysts confirmed by XRD results. As seen from TEM images, nickel particles ranged from 12 to 36 nm. Small metal particles indicate the strong interactions between the metal and the support. Moreover, these particles were localized at the tip of carbon nanotube indicating their activity. According to TPD, for all catalysts large amounts of basic sites and strong interactions between the metal and CO<sub>2</sub> were observed. Ni-Mg-Al obtained with SCS possesses 0.19 wt%·g<sup>−1</sup><sub>Ni</sub> of carbon content, which was much lower than that of Ni-Mg catalyst. It was found that SCS derived Ni-Mg-Al catalyst exhibited higher activity compared to its reduced analogue prepared by impregnation. The former catalyst showed stable performance during 200 h test with a decreasing coking rate. The metal particle size was lower for this spent catalyst in comparison with Ni-Mg-Al tested for 20 h test.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115261"},"PeriodicalIF":5.2,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143562504","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Conversion of dimethyl ether to hydrocarbons catalyzed by Pd-loaded *MRE zeolites 负载pd的*MRE沸石催化二甲醚转化为碳氢化合物
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-01 DOI: 10.1016/j.cattod.2025.115258
Benjamin Niethammer , Foteini Zormpa , Gia Trung Hoang , Nikolaj Aljoscha Slaby , Thomas Anthony Zevaco , Stamatia Karakoulia , Ulrich Arnold , Jörg Sauer
{"title":"Conversion of dimethyl ether to hydrocarbons catalyzed by Pd-loaded *MRE zeolites","authors":"Benjamin Niethammer ,&nbsp;Foteini Zormpa ,&nbsp;Gia Trung Hoang ,&nbsp;Nikolaj Aljoscha Slaby ,&nbsp;Thomas Anthony Zevaco ,&nbsp;Stamatia Karakoulia ,&nbsp;Ulrich Arnold ,&nbsp;Jörg Sauer","doi":"10.1016/j.cattod.2025.115258","DOIUrl":"10.1016/j.cattod.2025.115258","url":null,"abstract":"<div><div>The influence of Pd loading on the conversion of dimethyl ether (DME) to hydrocarbons (DTH) was investigated for *MRE-type zeolite catalysts. Catalysts with different Pd loadings were prepared by incipient wetness impregnation and characterized in terms of morphology, composition and acidity. Co-feeding of H<sub>2</sub> during DME conversion increased the resistance of the Pd/*MRE catalysts to deactivation, which significantly increased their lifetimes and thus conversion capacities. The product spectra show high olefin contents, comprising light olefins and higher olefins in the C<sub>5</sub>–C<sub>11</sub> range, while contents of aromatics are low. H<sub>2</sub> co-feeding reduces the formation of cyclic hydrocarbons and increases the formation of n- and iso-alkanes as well as olefins. Higher Pd loadings slightly decrease olefin production but increase paraffin formation, indicating direct hydrogenation of olefins on Pd nanoparticles. The olefin-rich products offer several possibilities for further processing to fuels and chemicals.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115258"},"PeriodicalIF":5.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143621448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optimizing operational strategies in a non-isothermal bench-scale fixed-bed reactor for CO2 hydrogenation to CH4 combining experimental and modeling and simulation approaches 结合实验和建模仿真方法,优化非等温固定床反应器中CO2加氢制CH4的操作策略
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-01 DOI: 10.1016/j.cattod.2025.115256
Elena Gómez-Bravo, Unai De-La-Torre, José A. González-Marcos, Juan R. González-Velasco, Beñat Pereda-Ayo
{"title":"Optimizing operational strategies in a non-isothermal bench-scale fixed-bed reactor for CO2 hydrogenation to CH4 combining experimental and modeling and simulation approaches","authors":"Elena Gómez-Bravo,&nbsp;Unai De-La-Torre,&nbsp;José A. González-Marcos,&nbsp;Juan R. González-Velasco,&nbsp;Beñat Pereda-Ayo","doi":"10.1016/j.cattod.2025.115256","DOIUrl":"10.1016/j.cattod.2025.115256","url":null,"abstract":"<div><div>The CO<sub>2</sub> methanation reaction is a promising solution for renewable energy storage. However, the process is challenged by thermal management due to its exothermic nature, leading to hot spots that complicate reactor operation and scale-up. This study combines experimental and simulation approaches to optimize the operation of a bench-scale fixed-bed reactor. Experimental results show that reactor wall temperature, flow rate, and nitrogen dilution significantly affect temperature profiles and CO<sub>2</sub> conversion. As a refrigeration strategy, it has been studied the use of pressurized air jackets to improve heat dissipation and stabilize the operation. A dynamic 1D heterogeneous model validated these findings and enabled simulation-based optimization. Non-uniform particle size distributions, metal loading, and SiC dilution strategies effectively mitigated hot spots without compromising CH<sub>4</sub> yield. These results offer critical insights into reactor design, ensuring stable operation and high efficiency.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115256"},"PeriodicalIF":5.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549288","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The role of promoters in enhancing hydrogen production during catalytic decomposition of methane 促进剂在甲烷催化分解过程中促进产氢的作用
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-03-01 DOI: 10.1016/j.cattod.2025.115259
Dwi Hantoko , Wasim Ullah Khan , Ali M. Alomran , Ariel H. Gursida , Mohammed Saud Hammad , Srinivasakannan Chandrasekar , Mohammad M. Hossain
{"title":"The role of promoters in enhancing hydrogen production during catalytic decomposition of methane","authors":"Dwi Hantoko ,&nbsp;Wasim Ullah Khan ,&nbsp;Ali M. Alomran ,&nbsp;Ariel H. Gursida ,&nbsp;Mohammed Saud Hammad ,&nbsp;Srinivasakannan Chandrasekar ,&nbsp;Mohammad M. Hossain","doi":"10.1016/j.cattod.2025.115259","DOIUrl":"10.1016/j.cattod.2025.115259","url":null,"abstract":"<div><div>Catalytic methane decomposition is a promising process for co-production of CO<sub>x</sub> free hydrogen and carbon nanomaterials. In this work, iron-based catalysts, supported on ZSM5, were studied as an active catalyst for methane decomposition and nickel and cobalt were used to boost the methane conversion and catalyst stability. The prepared catalysts were tested at 700 °C with the 9:1 CH<sub>4</sub> to Ar feed ratio under atmospheric pressure in a fixed bed tubular reactor. The diffraction peaks showed the formation of corresponding metal oxides and their combination species. The activity profiles implied that promoted iron-based catalyst (NiFe/ZSM5) outperformed the rest of the catalysts with an initial activity of 81.51 % that remained 75 % at the end of 170 min time-on-stream. The unpromoted (Fe/ZSM5) suffered deactivation over time and hence NiFe/ZSM5 turned out to be the active and stable catalyst among the tested catalysts. The high-resolution transition electron microscopy (HRTEM) images of the best catalyst indicated the growth of multiwalled carbon nanotubes which followed tip-base-growth mechanisms.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"453 ","pages":"Article 115259"},"PeriodicalIF":5.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549289","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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