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Probing deactivation by coking in catalyst pellets for dry reforming of methane using a pore network model 被引量:2
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作者 Yu Wang Qunfeng Zhang +3 位作者 Xinlei Liu Junqi Weng Guanghua Ye Xinggui Zhou 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第3期293-303,共11页
Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, w... Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, which prevents this technology from commercialization. In this work, a pore network model is developed to probe the catalyst deactivation by coking in a Ni/Al_(2)O_(3) catalyst pellet for DRM. The reaction conditions can significantly change the coking rate and then affect the catalyst deactivation. The catalyst lifetime is higher under lower temperature, pressure, and CH_(4)/CO_(2) molar ratio, but the maximum coke content in a catalyst pellet is independent of these reaction conditions. The catalyst pellet with larger pore diameter, narrower pore size distribution and higher pore connectivity is more robust against catalyst deactivation by coking, as the pores in this pellet are more difficult to be plugged or inaccessible.The maximum coke content is also higher for narrower pore size distribution and higher pore connectivity, as the number of inaccessible pores is lower. Besides, the catalyst pellet radius only slightly affects the coke content, although the diffusion limitation increases with the pellet radius. These results should serve to guide the rational design of robust DRM catalyst pellets against deactivation by coking. 展开更多
关键词 Deactivation by coking dry reforming of methane Pore network model Diffusion limitation Catalyst pellet
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An Energy Production System Powered by Solar Heat with Biogas Dry Reforming Reactor and Solid Oxide Fuel Cell
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作者 Akira Nishimura Ryotaro Sato Eric Hu 《Smart Grid and Renewable Energy》 CAS 2023年第5期85-106,共22页
In this paper, an energy system consisting of solar collector, biogas dry reforming reactor and solid oxide fuel cell (SOFC) has been proposed. The heat produced from the concentrating solar collector is used to drive... In this paper, an energy system consisting of solar collector, biogas dry reforming reactor and solid oxide fuel cell (SOFC) has been proposed. The heat produced from the concentrating solar collector is used to drive a biogas dry reforming reactor in order to produce H<sub>2</sub> as a fuel for SOFC, in such as system. The aim of this study is to clarify the impact of climate data on the performance of solar collector with various sizes/designs. The temperature of heat transfer fluid produced by the solar collector is calculated by adopting the climate data for Nagoya city in Japan in 2021. The amount of H<sub>2</sub> produced from the biogas dry reforming reactor and the power generated by SOFC were simulated. The results show the temperature of heat transfer fluid (T<sub>fb</sub>) and T<sub>fb</sub> ratio (a) based on the length of absorber (dx) = 1 m have a peak near the noon following the trend of solar intensity (I). Results also revealed that a increases with increase in dx. It is found that the differences of T<sub>fb</sub> and a between dx = 2 m and dx = 3 m are larger than those between dx = 1 m and dx = 2 m. It is revealed that T<sub>fb</sub> and a are higher in spring and summer. dx = 4 m is the optimum length of solar absorber. The amount of H<sub>2</sub> produced from the biogas dry reforming reactor as well as the power generated by SOFC is the highest in August, resulting that it is prefer to produce H<sub>2</sub> and to generate SOFC in summer. 展开更多
关键词 Solar Collector Fluid Temperature Climate Data Biogas dry reforming H2 Production SOFC
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Ni-Co/Mg-Al catalyst derived from hydrotalcite-like compound prepared by plasma for dry reforming of methane 被引量:9
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作者 Huali Long Yan Xu +4 位作者 Xiaoqing Zhang Shijing Hu Shuyong Shang Yongxiang Yin Xiaoyan Dai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第5期733-739,共7页
Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was inves... Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method. 展开更多
关键词 dry reforming of methane Ni-Co bimetallic catalyst cold plasma treatment hydrotalcite-like compound
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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 被引量:6
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作者 Zahra Alipour Mehran Rezaei Fereshteh Meshkani 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第5期633-638,共6页
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 in... 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. 展开更多
关键词 nickel catalyst MgO modifier SYNGAS dry reforming coke formation
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Charge transfer in plasma assisted dry reforming of methane using a nanosecond pulsed packed-bed reactor discharge 被引量:6
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作者 张帅 高远 +2 位作者 孙昊 范喆 邵涛 《Plasma Science and Technology》 SCIE EI CAS CSCD 2021年第6期59-66,共8页
This paper is aimed to investigate the effect of packing material on plasma characteristic from the viewpoint of charge transfer process.Both the charge accumulation and release processes in the dielectric barrier dis... This paper is aimed to investigate the effect of packing material on plasma characteristic from the viewpoint of charge transfer process.Both the charge accumulation and release processes in the dielectric barrier discharge reactor and packed-bed reactor were investigated by measuring voltage and current waveforms and taking ICCD images.The packing material was ZrO2 pellets and the reactors were driven by a parameterized nanosecond pulse source.The quantity of transferred charges in the dielectric barrier discharge reactor was enhanced when decreasing pulse rise time or increasing pulse width(within 150 ns),but reduced when the gas gap was packed with pellets.The quantity of accumulated charges in the primary discharge was larger than the quantity of released charges in the secondary discharges in the dielectric barrier discharge reactor,but they were almost equal in the packed-bed reactor.It indicates that the discharge behavior has been changed from the view of charge transfer process once the gas gap was packed with pellets,and the ICCD images confirmed it. 展开更多
关键词 non-thermal plasma packed-bed reactor dry reforming plasma catalysis charge transfer
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Methane dry reforming on Ni/La_2Zr_2O_7 treated by plasma in different atmospheres 被引量:4
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作者 Honggen Peng Youhe Ma +7 位作者 Wenming Liu Xianglan Xu Xiuzhong Fang Jie Lian Xiang Wang Changqing Li Wufeng Zhou Ping Yuan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2015年第4期416-424,共9页
A series of Ni/La2Zr2O7 pyrochlore catalysts prepared by impregnation method and treated by dielectric barrier discharge(DBD) plasma in different atmospheres and varied sequences were prepared and applied for dry re... A series of Ni/La2Zr2O7 pyrochlore catalysts prepared by impregnation method and treated by dielectric barrier discharge(DBD) plasma in different atmospheres and varied sequences were prepared and applied for dry reforming of methane(DRM). It is found that all of the plasma treated catalysts show evidently improved activity and coke resistance in comparison with the non-plasma treated one. The best performance is achieved on Ni/La2Zr2O7–H2P–C,a catalyst treated in H2 plasma before calcination. TGA-DSC and SEM demonstrate that carbon deposition is significantly suppressed on all of the plasma treated samples. Moreover,XRD and TEM results testify that both Ni O and Ni sizes on the calcined and reduced samples treated by plasma are also decreased,which results in higher Ni metal dispersion on the reduced and used catalysts and enhances the interactions between Ni sites and the support. It is believed that these are the inherent reasons accounting for the promotional effects of plasma treatment on the reaction performance of the Ni/La2Zr2O7 pyrochlore catalysts. 展开更多
关键词 Methane dry reforming Ni-based catalysts Pyrochlore support DBD plasma Coke resistance
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Nickel ferrite spinel as catalyst precursor in the dry reforming of methane:Synthesis,characterization and catalytic properties 被引量:5
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作者 Rafik Benrabaa Hamza Boukhlouf +4 位作者 Axel Lfberg Annick Rubbens Rose-Nelle Vannier Elisabeth Bordes-Richard Akila Barama 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2012年第5期595-604,共10页
Dry reforming of methane by CO2 using nickel ferrite as precursor of catalysts was investigated.Nickel ferrite crystalline particles were prepared by coprecipitation of nitrates with NaOH or ammonia followed by calcin... Dry reforming of methane by CO2 using nickel ferrite as precursor of catalysts was investigated.Nickel ferrite crystalline particles were prepared by coprecipitation of nitrates with NaOH or ammonia followed by calcination,or by hydrothermal synthesis without calcination step.The textural and structural properties were determined by a number of analysis methods,including X-ray diffraction (XRD),Raman spectroscopy and X-ray photoelectron spectroscopy (XPS),among which X-ray diffraction (XRD) was at room and variable temperatures.All synthesized oxides showed the presence of micro or nanoparticles of NiFe2O4 inverse spinel,but Fe2O3 (hematite) was also present when ammonia was used for coprecipitation.The reducibility by hydrogen was studied by temperature-programmed reduction (TPR) and in situ XRD,which showed the influence of the preparation method.The surface area (BET),particle size (Rietveld refinement),as well as surface Ni/Fe atomic ratio (XPS) and the behavior upon reduction varied according to the synthesis method.The catalytic reactivity was investigated using isopropanol decomposition to determine the acid/base properties.The catalytic performance of methane reforming with CO2 was measured with and without the pre-treatment of catalysts under H2 in 650-800 C range.The catalytic conversions of methane and CO2 were quite low but they increased when the catalysts were pre-reduced.A significant contribution of reverse water gas shift reaction accounted for the low values of H2 /CO ratio.No coking was observed as shown by the reoxidation step performed after the catalytic reactions.The possible formation of nickel-iron alloy observed during the study of reducibility by hydrogen was invoked to account for the catalytic behavior. 展开更多
关键词 dry reforming of methane NiFe2O4 spinel hydrothermal synthesis coprecipitation isopropanol decomposition
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Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming 被引量:4
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作者 Wenming Liu Le Li +6 位作者 Sixue Lin Yiwei Luo Zhenghong Bao Yiru Mao Kongzhai Li Daishe Wu Honggen Peng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第2期34-47,共14页
Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two ... Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or hydrogen.The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts.Herein,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(In_(x)Ni@SiO_(2))have been prepared and displayed superior coking resistance for DRM reaction.The sample containing 0.5 wt.%of In loading(In_(0.5)Ni@SiO_(2))shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test.The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In.Both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane.The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases. 展开更多
关键词 Methane dry reforming InNi intermetallic alloy Confinement Coking resistance Utilization of greenhouse gases
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Tuning combined steam and dry reforming of methane for “metgas”production: A thermodynamic approach and state-of-the-art catalysts 被引量:4
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作者 Karam Jabbour 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第9期54-91,I0003,共39页
Nowadays,combined steam and dry reforming of methane(CSDRM)is viewed as a new alternative for the production of high-quality syngas(termed as"metgas",H2:CO of 2.0)suitable for subsequent synthesis of methano... Nowadays,combined steam and dry reforming of methane(CSDRM)is viewed as a new alternative for the production of high-quality syngas(termed as"metgas",H2:CO of 2.0)suitable for subsequent synthesis of methanol,considered as a promising renewable energy vector to substitute fossil fuel resources.Adequate operation conditions(molar feed composition,temperature and pressure)are required for the sole production of"metgas"while achieving high CH4,CO2 and H2O conversion levels.In this work,thermodynamic equilibrium analysis of CSDRM has been performed using Gibbs free energy minimization where;(i)the effect of temperature(range:200-1000℃),(ii)feed composition(stoichiometric ratio as compared to a feed under excess steam or excess carbon dioxide),(iii)pressure(range:1-20 bar)and,(iv)the presence of a gaseous diluent on coke yields,reactivity levels and selectivity towards"metgas"were investigated.Running CSDRM at a temperature of at least 800℃,a pressure of 1 bar and under a feed composition where CO2-H2O/CH4 is around 1.0,are optimum conditions for the theoretical production of"metgas"while minimizing C(S)formation for longer experimental catalytic runs.A second part of this work presents a review of the recent progresses in the design of(principally)Ni-based catalysts along with some mechanistic and kinetic modeling aspects for the targeted CSDRM reaction.As compared to noble metals,their high availability,low cost and good intrinsic activity levels are main reasons for increasing research dedications in understanding deactivation potentials and providing amelioration strategies for further development.Deactivation causes and main orientations towards designing deactivationresistant supported Ni nanoparticles are clearly addressed and analyzed.Reported procedures based on salient catalytic features(i.e.,acidity/basicity character,redox properties,oxygen mobility,metal-support interaction)and recently employed innovative tactics(such as confinement within mesoporous systems,stabilization through core shell structures or on carbide surfaces)are highlighted and their impact on Ni0reactivity and stability are discussed.The final aspect of this review encloses the major directions and trends for improving synthesis/preparation designs of Ni-based catalysts for the sake of upgrading their usage into industrially oriented combined reforming operations. 展开更多
关键词 Combined steam and dry reforming of methane Thermodynamic equilibrium analysis "Metgas"production Nickel-based catalysts Heterogeneous catalysis Structure-activity relationship
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Comparison of dry reforming of methane in low temperature hybrid plasma-catalytic corona with thermal catalytic reactor over Ni/γ-Al_2O_3 被引量:4
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作者 Amin Aziznia Hamid Reza Bozorgzadeh +2 位作者 Naser Seyed-Matin Morteza Baghalha Ali Mohamadalizadeh 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2012年第4期466-475,共10页
In the current study, the hybrid effect of a corona discharge and γ-alumina supported Ni catalysts in CO2 reforming of methane is investigated. The study includes both purely catalytic operation in the temperature ra... In the current study, the hybrid effect of a corona discharge and γ-alumina supported Ni catalysts in CO2 reforming of methane is investigated. The study includes both purely catalytic operation in the temperature range of 923-1023 K, and hybrid catalytic-plasma operation of DC corona discharge reactor at room temperature and ambient pressure. The effect of feed flow rate, discharge power and Ni/γ-Al2O3 catalysts are studied. When CH4/CO2 ratio in the feed is 1/2, the syngas of low Ha/CO ratio at about 0.56 is obtained, which is a potential feedstock for synthesis of liquid hydrocarbons. Although Ni catalyst is only active above 573 K, presence of Ni catalysts in the cold corona plasma reactor (T≤523 K) shows promising increase in the conversions of methane and carbon dioxide. When Ni catalysts are used in the plasma reaction, H2/CO ratios in the products are slightly modified, selectivity to CO increases whereas fewer by-products such as hydrocarbons and oxygenates are formed. 展开更多
关键词 dry reforming of methane synthesis gas hybrid catalyst plasma Ni/γ-Al2O3 discharge power
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Quantitative behavior of vibrational excitation in AC plasma assisted dry reforming of methane 被引量:3
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作者 Jintao Sun Qi Chen +2 位作者 Yuanwei Guo Zili Zhou Yang Song 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第7期133-143,I0005,共12页
Quantitative behavior of non-equilibrium excitation by direct electron impact in low-temperature dry reforming of methane was investigated by integrated studies of experimental validation and kinetic modeling.A plasma... Quantitative behavior of non-equilibrium excitation by direct electron impact in low-temperature dry reforming of methane was investigated by integrated studies of experimental validation and kinetic modeling.A plasma chemistry kinetic mechanism incorporating the reactions involving vibrational excitation of CH4,CO2,H2 and CO molecules as well as the low temperature He/CH4/CO2 conversion pathways was developed and validated.The calculation results showed that at lower E/N values(<150 Td)large population of energized electrons generated in a He/CH4/CO2 discharge resulted in an intensification of vibrational excitation.Despite the large generation of vibration,the vibrationally excited molecules in a 0.5/0.25/0.25 of He/CH4/CO2 discharge mixture were easy to relax,due to the strong coupling of the vibration of different molecules in a gas mixture.The results showed that the moderate levels of the vibrational excitation,such as CO2(v10,11,...,18)and CO(v9,10),presented most efficient in the stimulation of species generation including CO,CH2 O,CH3 OH,C2 H4 and C2 H6.Specifically,under conditions of E/N of 108 Td,14.9%of CO formation was estimated from the recombination of CO2(v)with CH3 and H,CO2(v)+CH3→CH3 O+CO,CO2(v)+H→CO+OH.Also,4.8%of C2 H4 formation was from the recombination reaction CH4(v)+CH→C2 H4+H.These results highlight the strong roles of vibrational states in a complex plasma chemistry system. 展开更多
关键词 Non-equilibrium plasma dry reforming Vibrational excitation Low-temperature chemistry Plasma assisted combustion
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Dry reforming of methane on active and coke resistant Ni/Y_2Zr_2O_7 catalysts treated by dielectric barrier discharge plasma 被引量:3
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作者 Xiuzhong Fang Jie Lian +7 位作者 Kaiwen Nie Xianhua Zhang Yanfeng Dai Xianglan Xu Xiang Wang Wenming Liu Changqing Li Wufeng Zhou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2016年第5期825-831,共7页
In this study, Ni/YZrOcatalysts prepared with impregnation method and treated by dielectric barrier discharge plasma(DBD) in different atmospheres have been investigated for methane dry reforming. It is revealed by H-... In this study, Ni/YZrOcatalysts prepared with impregnation method and treated by dielectric barrier discharge plasma(DBD) in different atmospheres have been investigated for methane dry reforming. It is revealed by H-TPR that plasma treatment can enhance the interaction between Ni O/Ni particles and the YZrOpyrochlore support. Therefore, catalysts with smaller Ni O and Ni grains sizes, higher metallic Ni active surface areas can be achieved, as evidenced by XRD, TEM and Hadsorption-desorption measurements. As a consequence, the plasma-treated catalysts show significantly improved activity, stability and coke resistance, as testified by the TEM and TGA-DSC results. Plasma treatment in H/Ar gas mixture is found to be the best condition to prepare Ni/YZrO, which can be used to obtain a catalyst with the highest activity, stability and most potent coke resistance. It is believed that the smaller Ni grain size and higher metallic Ni active surface area induced by plasma treatment are the inherent reasons accounting for the promoted reaction performance of the Ni/YZrOpyrochlore catalysts. 展开更多
关键词 Plasma treatment Y2Zr2O7 pyrochlore support Supported Ni catalysts Methane dry reforming Coke resistance
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Catalytic performance of cement clinker supported nickel catalyst in glycerol dry reforming 被引量:1
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作者 Hua Chyn Lee Kah Weng Siew +3 位作者 Maksudur R.Khan Sim Yee Chin Jolius Gimbun Chin Kui Cheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第5期645-656,共12页
The paper reports the development of cement clinker-supported nickel (with metal loadings of 5 wt%, 10 wt%, 15 wt% and 20 wt%) catalysts for glycerol dry (CO2) reforming reaction. XRF results showed that CaO const... The paper reports the development of cement clinker-supported nickel (with metal loadings of 5 wt%, 10 wt%, 15 wt% and 20 wt%) catalysts for glycerol dry (CO2) reforming reaction. XRF results showed that CaO constituted 62.0% of cement clinker. The physicochemical characterization of the catalysts revealed 32-folds increment of BET surface area (SBET) with the addition of nickel metal into the cement clinker, which was also corroborated by FESEM images. Significantly, XRD results suggested different types of Ni oxides formation with Ni loading, whilst Ca3SiO5 and Ca2Al0.67Mn0.33FeO5 were the main crystallite species for pure cement clinker. Temperature-programmed reduction analysis yielded three domains of H2 reduction peaks, viz. centered at approximately 750 K referred to as type-Ⅰ peaks, another peaks at 820 K denoted as type-Ⅱ peaks and the highest reduction peaks, type-Ⅲ recorded at above 1000 K. 20 wt% Ni was found to be the best loading with the highest XG and H2 yield, whilst the lowest methanation activity. Syngas with lower H2/CO ratios (0.6 to 1.5) were readily produced from glycerol dry reforming at CO2-to-Glycerol feed ratio (CGR) of unity. Nonetheless, carbon deposit comprised of whisker type (Cv) and graphitic-like type (Cc) species were found to be in majority on 20 wt%Ni/CC catalysts. 展开更多
关键词 cement clinker dry reforming GLYCEROL nickel catalyst SYNGAS
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Interface-directed epitaxially growing nickle ensembles as efficient catalysts in dry reforming of methane 被引量:1
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作者 Ping Wang Song Wei +3 位作者 Shiyi Wang Ronghe Lin Xiaoling Mou Yunjie Ding 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期502-513,I0014,共13页
Supported nickel catalysts are promising candidates for dry reforming of methane, but agglomeration of Ni^(0) and coke deposition hinder the industrial applications. Herein, we report a novel interface-directed synthe... Supported nickel catalysts are promising candidates for dry reforming of methane, but agglomeration of Ni^(0) and coke deposition hinder the industrial applications. Herein, we report a novel interface-directed synthetic approach to construct distinct metal ensembles by carefully tuning the compositions of the carriers. A Zr-Mn-Zn ternary oxide-supported Ni catalyst, together with the respective binary oxide-supported analogues, was synthesized by adopting a sequential co-precipitation and wetness impregnation method. Combined characterization techniques identify distinct catalyst models, including (i) conventional NiO nanoparticles with different sizes on Zr-Mn and Zr-Zn, and (ii) epitaxially growing NiO ensembles of a few nanometers thickness at the periphery of ZnO_(x) particles. These catalysts exhibit divergent responses in the catalytic testing, with the ternary oxide system significantly outperforming the binary analogues. The strong electronic interactions between Mn-Ni increase Ni dispersion and the activity while the stability is strengthened upon Zn addition. Both high activity, high selectivity, and remarkable stability are attained upon co-adding Mn and Zn. The interfaces between Ni and Zr-Mn-Zn rather than the physical contacts of individual oxide-supported analogues through mechanical mixing are keys for the outstanding performance. 展开更多
关键词 Methane dry reforming NICKEL INTERFACE Epitaxial growth Structure-performance relationship
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Photocatalytic dry reforming of methane by rhodium supported monoclinic TiO_(2)-B nanobelts 被引量:1
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作者 Masaru Kushida Akira Yamaguchi Masahiro Miyauchi 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第8期562-571,I0015,共11页
The conversion of methane and carbon dioxide into syngas(dry reforming of methane;DRM)has attracted attention owing to the potential to reuse greenhouse gases.Titanium dioxide(TiO_(2))-based photocatalysts,which have ... The conversion of methane and carbon dioxide into syngas(dry reforming of methane;DRM)has attracted attention owing to the potential to reuse greenhouse gases.Titanium dioxide(TiO_(2))-based photocatalysts,which have been widely commercialized owing to their high efficiency,non-toxicity,and low cost,are strongly desired in DRM.Here,we report a monoclinic-phase TiO_(2)-B nanobelts-supported rhodium(Rh/TiO_(2)-B nanobelts)catalyst that efficiently promotes DRM under ultraviolet light irradiation at low temperatures.Photogenerated holes in the TiO_(2)-B nanobelts were used to oxidize methane,while the electrons were trapped in rhodium to reduce carbon dioxide.Rh/TiO_(2)-B nanobelts exhibited considerably higher durability and activity than Rh-loaded conventional TiO_(2)(anatase and rutile),owing to the lattice and/or surface oxygen reactivity in TiO_(2)-B nanobelts,which was suggested by X-ray photoelectron spectroscopy measurements and photocatalytic performance tests under an atmosphere of methane alone.This study paves the path for the effective utilization of methane by constructing active TiO_(2)-based nanometal photocatalysts. 展开更多
关键词 Photocatalysis dry reforming of methane Greenhouse gas conversion Gas-phase reaction Titanium dioxide TiO_(2)-B
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Utilizing bimetallic catalysts to mitigate coke formation in dry reforming of methane 被引量:1
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作者 Jaylin Sasson Bitters Tina He +3 位作者 Elizabeth Nestler Sanjaya D.Senanayake Jingguang G.Chen Cheng Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第5期124-142,共19页
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... 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. 展开更多
关键词 dry reforming of methane Carbon dioxide Bimetallic catalysts Coke formation Catalyst stability
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Modeling and optimization of methane dry reforming over Ni-Cu/Al_2O_3 catalyst using Box-Behnken design 被引量:1
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作者 Seyedeh Molood Masoom Nataj Seyed Mehdi Alavi Golshan Mazloom 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2018年第5期1475-1488,共14页
In this work the effects of the contents of nickel (5, 7.5, 10 wt%) and copper (0, 1, 2 wt%) and reac- tion temperature (650, 700, 750 ℃) on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry re... In this work the effects of the contents of nickel (5, 7.5, 10 wt%) and copper (0, 1, 2 wt%) and reac- tion temperature (650, 700, 750 ℃) on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry reforming were evaluated using Box-Behnken design in order to optimize methane conversion, H_2/CO ratio and the catalyst deactivation. Different catalysts were prepared by co-impregnation method and characterized by XRD, BET, H_2-TPR, FESEM and TG/DTA analyses. The results revealed that copper addi- tion improved the catalyst reducibility. Promoted catalyst with low amounts of Cu gave higher activity and stability with high resistance to coke deposition and agglomeration of active phase especially during the reaction. However catalysts with high amounts of Cu were less active and rather deactivated due to the active sites sintering as well as Ni covering by Cu-enriched phase. The optimal conditions were de- termined by desirability function approach as 10 wt% of Ni, 0.83 wt% of Cu at 750℃. CH_4 conversion of 95.1%, H_2/CO ratio of 1 and deactivation of 1.4% were obtained experimentally under optimum conditions, which were in close agreement with the values oredicted hv the developed model. 展开更多
关键词 Methane dry reforming Copper addition Ni-based catalyst SYNGAS Box-Behnken design
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Characterization of La-promoted Ni/Al_2O_3 catalysts for hydrogen production from glycerol dry reforming 被引量:1
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作者 Kah Weng Siew Hua Chyn Lee +1 位作者 Jolius Gimbun Chin Kui Cheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第1期15-21,共7页
In the current paper, dry(CO2)-reforming of glycerol, a new reforming route, was carried out over alumina(Al2O3)-supported, non-promoted and lanthanum-promoted nickel(Ni) catalysts. Both sets of catalysts were synthes... In the current paper, dry(CO2)-reforming of glycerol, a new reforming route, was carried out over alumina(Al2O3)-supported, non-promoted and lanthanum-promoted nickel(Ni) catalysts. Both sets of catalysts were synthesized via a wet co-impregnation procedure. Physicochemical characterization of the catalysts showed that the promoted catalyst possessed smaller metal crystallite size, hence higher metal dispersion compared to the virgin Ni/Al2O3catalyst. This was also corroborated by the surface images captured by the FESEM analysis. From temperature-programmed calcination analysis, the derivative weight profiles revealed two peaks, which represent a water elimination peak at a temperature range of 373 to 473 K followed by nickel nitrate decomposition from 473 to 573 K. In addition, BET surface area measurements gave 85.0 m2 g-1for the non-promoted Ni catalyst, whilst the promoted catalysts showed an average of 1% to 6% improvement depending on the La loadings. Significantly, reaction studies at 873 K showed that glycerol dry reforming successfully produced H2. The 2%La-Ni/Al2O3catalyst, which possessed the largest BET surface area, gave an optimum H2generation(9.70%) at a glycerol conversion of 24.5%. 展开更多
关键词 Ni catalysts dry reforming lanthanide promotion reaction kinetics
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Regeneration of C_4H_(10) dry reforming catalyst by nonthermal plasma
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作者 Y.S.Mok E.Jwa Y.J.Hyun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第3期394-402,共9页
Carbon deposition via coke formation is one of the critical problems causing catalyst deactivation during the reforming of hydrocarbons. An effort was made to regenerate the catalyst (Ni/γ-alumina) by oxidation met... Carbon deposition via coke formation is one of the critical problems causing catalyst deactivation during the reforming of hydrocarbons. An effort was made to regenerate the catalyst (Ni/γ-alumina) by oxidation methods. Two approaches were carded out for the regeneration of the deactivated catalyst. The first one involves the plasma treatment of the deactivated catalyst in the presence of dry air over a temperature range of 300-500℃, while the second one only the thermal treatment in the same temperature range. The performance of the regenerated catalyst was evaluated in terms of C4H10 and CO2 conversions and the physicochemical characteristics were examined using a surface area analyzer, an elemental analyzer, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). It was observed that the carbon deposit (coke) on the catalyst was about 9.89 wt% after reforming C4H10 for 5 h at 540℃. The simple thermal treatment at 400 ℃ reduced carbon content to 6.59 wt% whereas it was decreased to 3.25 wt% by the plasma and heat combination. The specific surface area was fully restored to the original state by the plasma-assisted regeneration at 500℃. As far as the catalytic activity is concerned, the fresh and regenerated catalysts exhibited similar C4H10 and CO2 conversion efficiencies. 展开更多
关键词 dry reforming coke formation REGENERATION PLASMA CATALYST
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Dry Reforming of Ethane over FeNi/Al-Ce-O Catalysts:Composition-Induced Strong Metal-Support Interactions
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作者 Tao Zhang Zhi-Cheng Liu +4 位作者 Ying-Chun Ye Yu Wang He-Qin Yang Huan-Xin Gao Wei-Min Yang 《Engineering》 SCIE EI CAS 2022年第11期173-185,共13页
Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)... Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)effect over FeNi/Al-Ce-O catalysts is revealed via X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(TPR),and energy dispersive X-ray spectroscopy(EDS)elemental mapping.The introduction of Al into Al-Ce-O supports significantly influences the dispersion of surface active components and improves the catalytic performance for DRE over supported FeNi catalysts due to enhancement of the SMSI effect.The catalytic properties,for example,C_(2)H_(6) and CO_(2) conversion,CO selectivity and yield,and turnover frequencies(TOFs),of supported FeNi catalysts first increase and then decrease with increasing Al content,following the same trend as the theoretical effective surface area(TESA)of the corresponding catalysts.The FeNi/Ce-Al_(0.5) catalyst,with 50%Al content,exhibits the best DRE performance under steady-state conditions at 873 K.As observed by with in situ Fourier transform infrared spectroscopy(FTIR)analysis,the introduction of Al not only increases the content of surface Ce3+and oxygen vacancies but also promotes the dispersion of surface active components,which further alters the catalytic properties for DRE over supported FeNi catalysts. 展开更多
关键词 dry reforming of ethane Strong metal-support interaction Carbon dioxide CERIA Oxygen vacancy Reaction mechanism
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