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Jinan University Achieves Breakthrough in Propylene/Propane Separation
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《China Petroleum Processing & Petrochemical Technology》 SCIE CAS 2021年第3期89-89,共1页
Recently,the research team at the Jinan University(JNU)based on the adsorption/desorption technology over metal-organic frameworks(MOF)for the first time proposes an orthogonal array dynamic screening mechanism to suc... Recently,the research team at the Jinan University(JNU)based on the adsorption/desorption technology over metal-organic frameworks(MOF)for the first time proposes an orthogonal array dynamic screening mechanism to successfully construct the separation mechanism-based frame material(JNU-3),which can be used in adsorptive separation of propylene from propane.MOF is a kind of crystalline porous materials with a definite composition and structure formed by self-assembled metal nodes and organic ligands. 展开更多
关键词 separation propylene definite
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Highly selective separation of propylene/propane mixture on cost-effectively four-carbon linkers based metal-organic frameworks
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作者 Daofei Lv Junhao Xu +9 位作者 Pingjun Zhou Shi Tu Feng Xu Jian Yan Hongxia Xi Zewei Liu Wenbing Yuan Qiang Fu Xin Chen Qibin Xia 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第11期126-134,共9页
The separation of propylene and propane is an important but challenging process,primarily achieved through energy-intensive distillation technology in the petrochemical industry.Here,we reported two natural C4linkers ... The separation of propylene and propane is an important but challenging process,primarily achieved through energy-intensive distillation technology in the petrochemical industry.Here,we reported two natural C4linkers based metal–organic frameworks(MIP-202 and MIP-203)for C_(3)H_(6)/C_(3)H_(8)separation.Adsorption isotherms and selectivity calculations were performed to study the adsorption performance for C_(3)H_(6)/C_(3)H_(8)separation.Results show that C_(3)H_(6)/C_(3)H_(8)uptake ratios(298 K,100 kPa)for MIP-202 and MIP-203 are 2.34 and 7.4,respectively.C_(3)H_(6)/C_(3)H_(8)uptake ratio(303 K,100 k Pa)for MIP-203 is up to50.0.The mechanism for enhanced separation performance of C_(3)H_(6)/C_(3)H_(8)on MIP-203 at higher temperature(303 K)was revealed by the in situ PXRD characterization.The adsorption selectivities of C_(3)H_(6)/C_(3)H_(8)on MIP-202 and MIP-203(298 K,100 k Pa)are 8.8 and 551.4,respectively.The mechanism for the preferential adsorption of C_(3)H_(6)over C_(3)H_(8)in MIP-202 and MIP-203 was revealed by the Monte Carlo simulation.The cost of organic ligands for MIP-202 and MIP-203 was lower than that of organic ligands for those top-performance MOFs.Our work sets a new benchmark for C_(3)H_(6)sorbents with high adsorption selectivities. 展开更多
关键词 propylene propane separation Gas Adsorption Metal-organic frameworks
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State-of-the-art catalysts for direct dehydrogenation of propane to propylene 被引量:32
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作者 Zhong-Pan Hu Dandan Yang +1 位作者 Zheng Wang Zhong-Yong Yuan 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第9期1233-1254,共22页
With growing demand for propylene and increasing production of propane from shale gas,the technologies of propylene production,including direct dehydrogenation and oxidative dehydrogenation of propane,have drawn great... With growing demand for propylene and increasing production of propane from shale gas,the technologies of propylene production,including direct dehydrogenation and oxidative dehydrogenation of propane,have drawn great attention in recent years.In particular,direct dehydrogenation of propane to propylene is regarded as one of the most promising methods of propylene production because it is an on-purpose technique that exclusively yields propylene instead of a mixture of products.In this critical review,we provide the current investigations on the heterogeneous catalysts(such as Pt,CrOx,VOx,GaOx-based catalysts,and nanocarbons)used in the direct dehydrogenation of propane to propylene.A detailed comparison and discussion of the active sites,catalytic mechanisms,influencing factors(such as the structures,dispersions,and reducibilities of the catalysts and promoters),and supports for different types of catalysts is presented.Furthermore,rational designs and preparation of high-performance catalysts for propane dehydrogenation are proposed and discussed. 展开更多
关键词 propane dehydrogenation propylene Heterogeneous catalyst Active site Catalytic mechanism
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Nature of active phase of VO_x catalysts supported on SiBeta for direct dehydrogenation of propane to propylene 被引量:7
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作者 Chong Chen Minglei Sun +3 位作者 Zhongpan Hu Yuping Liu Shoumin Zhang Zhong-Yong Yuan 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第2期276-285,共10页
The VOx catalysts supported on dealuminated Beta zeolite(Si Beta) with varying V loadings(from 0.5 to 10 wt%) are prepared and tested for their catalytic activities in the reaction of direct dehydrogenation of propane... The VOx catalysts supported on dealuminated Beta zeolite(Si Beta) with varying V loadings(from 0.5 to 10 wt%) are prepared and tested for their catalytic activities in the reaction of direct dehydrogenation of propane to propylene(PDH). It is characterized that the VSi Beta catalysts possess different kinds of vanadium species on the Si Beta support, including monomeric or isolated VOx species at a low V loading, and polynuclear VOx species in different polymerization degrees at higher V loadings. The 3 VSi Beta catalyst(V loading is 3 wt%), containing isolated VOx species in monolayer, shows around 40% of propane conversion with 90% of propylene selectivity(reaction conditions: 600 o C, 4000 m L g–1 h–1) which are comparable to VSi Beta catalysts with higher V loadings. The catalytic activity exhibits a good linear relationship with the amount of generated acidic sites, which are derived from the interaction sites between VOx species and Si Beta support, and keeps stable after several regeneration cycles. Thus, as the VOx species directly contact with Si Beta support via V–O–Si bonds, a reactivity enhancement can be achieved. While, the initial valence state of V does not seem to influence the catalytic performance. Moreover, the aggregation degree of VOx species determines the propylene selectivity and deactivation rate, both of which increase as raising the V loading amount. 展开更多
关键词 propane dehydrogenation propylene VOx species SiBeta support Active sites
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Effect of Sr loading on oxydehydrogenation of propane to propylene over Al_2O_3-supported V-Mo catalysts 被引量:2
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作者 Meilana Dharma Putra Saeed M.Al-Zahrani Ahmed E.Abasaeed 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第5期778-782,共5页
Incorporation of strontium into V-Mo alumina-supported catalyst enhanced its performance (increased conversion and selectivity,decreased reducibility and improved stability) in propane oxydehydrogenation to propylene.... Incorporation of strontium into V-Mo alumina-supported catalyst enhanced its performance (increased conversion and selectivity,decreased reducibility and improved stability) in propane oxydehydrogenation to propylene.12.5% Sr loading was shown to be the optimum content to the V-Mo catalyst.The results were supported by various characterization techniques,namely,BET,XRD,SEM,FTIR and TPD. 展开更多
关键词 OXYDEHYDROGENATION STRONTIUM vanadium-molybdenum oxides catalysts propane propylene LOADING
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SEPARATION OF PROPANE FROM PROPANE/NITROGEN MIXTURES USING PDMS COMPOSITE MEMBRANES BY VAPOR PERMEATION 被引量:1
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作者 李继定 《Chinese Journal of Polymer Science》 SCIE CAS CSCD 2009年第5期621-627,共7页
This study deals with polydimethylsiloxane(PDMS)/polyvinylidene fluoride(PVDF) composite membranes for propane separation from propane/nitrogen mixtures,which is relevant to the recovery of propane in petroleum and ch... This study deals with polydimethylsiloxane(PDMS)/polyvinylidene fluoride(PVDF) composite membranes for propane separation from propane/nitrogen mixtures,which is relevant to the recovery of propane in petroleum and chemical industry.The surface and cross-section morphology of PDMS/PVDF composite membranes was observed by scanning electron microscope(SEM).The surface morphology of PDMS/PVDF composite membranes is very dense.There are three layers,the thin dense top layer,finger-like porous middle layer and s... 展开更多
关键词 POLYDIMETHYLSILOXANE Poly(vinylidene fluoride) propane/nitrogen separation Composite membrane Vapor permeation.
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Design and optimization of an integrated process for the purification of propylene oxide and the separation of propylene glycol by-product 被引量:1
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作者 Song Hu Jinlong Li +1 位作者 Qihua Wang Weisheng Yang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第5期111-120,共10页
It is difficult to separate the methanol and hydrocarbons in the propylene oxide(PO)purification process due to their forming azeotrope.As for this,a novel PO separation process,in that the deionized water is employed... It is difficult to separate the methanol and hydrocarbons in the propylene oxide(PO)purification process due to their forming azeotrope.As for this,a novel PO separation process,in that the deionized water is employed as extractant and 1,2-propylene glycol(MPG)that is formed from the PO hydrolysis reaction is recovered,is presented in this work.The salient feature of this process is that both the non-catalyzed reactions of PO hydrolysis to form MPG and dipropylene glycol(DPG)are simultaneously considered and MPG by-product with high purity is obtained in virtue of the deionized water as reflux liquid and side take-off in MPG column.In addition,the ionic liquid(IL)extractant is screened through the conductorlike screening model for segment activity coefficient(COSMO-SAC)and the comparisons of separation efficiency between the IL and normal octane(nC_(8))extractant for the separation of PO and 2-methylpentane are made.With the non-random two-liquid(NRTL)thermodynamic model,the simulation and optimization design for the full flow sheet are performed and the effects of the key operation parameters such as solvent ratio,theoretical stages,feeding stage etc.on separation efficiency are detailedly discussed.The results show that the mass purity and the mass yield of PO can be up to 99.99%and 99.0%,and the condenser duty,reboiler duty and PO loss in the process with IL extractant can be decreased by 69.66%,30.21%and 78.86%compared to ones with nC_(8).The total annual cost(TAC)calculation also suggests that the TAC would be significantly reduced if using IL in replace of nC_(8) for the investigated process.The presented results would provide a useful guide for improving the quality of PO product and the economic efficiency of industrial plant. 展开更多
关键词 propylene oxide purification Ionic liquids separation Extractive distillation HYDROLYSIS 1 2-propylene glycol
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Robust microporous metal-organic framework with high moisture tolerance for efficient separation of propylene from propane 被引量:1
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作者 Shan-Qing Yang Lei Zhou +2 位作者 Bo Xing Ying-Hui Zhang Tong-Liang Hu 《Chinese Journal of Structural Chemistry》 SCIE CAS CSCD 2023年第2期29-34,共6页
Adsorptive separation of propylene(C_(3)H_(6))from propylene/propane(C_(3)H_(8))is desired to replace energy-intensive cryogenic distillation for its energy efficiency,economical viability,and environment friendship.I... Adsorptive separation of propylene(C_(3)H_(6))from propylene/propane(C_(3)H_(8))is desired to replace energy-intensive cryogenic distillation for its energy efficiency,economical viability,and environment friendship.In this work,we report a cupper-based robust microporous metal-organic framework,Cu-Hmpba,constructed by the hard soft acid-base principle using the bifunctional pyridylcarboxylate ligand featuring methyl group,for high-efficient separation of the propylene/propane mixture.Under the synergistic effect of the protective group and hard soft acid base principle,Cu-Hmpba possesses good solvents stability,especially water stability.Cu-Hmpba exhibits the adsorption capacity of C_(3)H_(6)with 2.10 mmol g^(-1)and good equimolar C_(3)H_(6)/C_(3)H_(8)selectivity with 2.24 at ambient conditions.The gas adsorption experiments,IAST selectivity calculations and theoretical calculations comprehensively support the selective adsorption toward C_(3)H_(6)among C_(3)H_(6)/C_(3)H_(8)mixture.Furthermore,it could maintain stable under moisture environment,suggesting its potential for the industrial separation of C_(3)H_(6)/C_(3)H_(8)mixture.The results of experiments and simulations demonstrate that the Cu-Hmpba would be a candidate adsorbent for the separation and purification of light hydrocarbons,and this work provides the insight of syn-thesizing stable MOF materials for separating high-value chemicals. 展开更多
关键词 Metal-organic framework Adsorptive separation propylene/propane separation Energy efficient
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Separation of a C_(3)H_(6)/C_(2)H_(4) mixture using Pebax^(■) 2533/PEG600 blend membranes 被引量:2
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作者 Xi Zhang Xiaodong Wang Wei Huang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第2期192-198,共7页
In industry, ethylene(C_(2)H_(4))/propylene(C_(3)H_(6)) separations are usually performed by a cryogenic process,which is energy intensive. Membrane separation technology is an alternative separation process that save... In industry, ethylene(C_(2)H_(4))/propylene(C_(3)H_(6)) separations are usually performed by a cryogenic process,which is energy intensive. Membrane separation technology is an alternative separation process that saves energy and is efficient. In this study, blend membranes were prepared by doping polyethylene glycol(PEG600) into a poly(ether-block-amide)(Pebax^(■) 2533) matrix and were used to separate the C_(2)H_(4)/C_(3)H_(6) mixture. The PEG 600 and Pebax^(■) 2533 polymers have good compatibility because they share hydrogen bonds. The addition of PEG600 is conducive to the hydrophilicity and the free volume of blend membranes, and it is also conducive to the solubility of C_(2)H_(4) and C_(3)H_(6) in the membranes, which improves the ability of the membranes to separate this gas pair. The Pebax^(■) 2533/PEG600 blend membrane with 15%(mass) PEG600 showed the highest separation performance in our investigated membranes, with a C_(3)H_(6)/C_(2)H_(4) selectivity of 8.9 and a C_(3)H_(6) permeability of 196 barrer(1 barrer = 1.33×10^(14)m^(3)(STP)·m·m^(-2)·s^(-1)·kPa^(-1)) at 238 K and 0.2 MPa, which is higher than that of the Pebax^(■) 2533/NaY-6%(mass) membrane(α_(C_(3)H_(6)/C_(2)H_(4)) =6.5, P_(C_(3)H_(6))=211 barrer) reported in our previous work. It is confirmed that incorporating PEG600 into the Pebax^(■) 2533 matrix to fabricate blend membranes is an efficient strategy for separating light olefins. 展开更多
关键词 Ethylene/propylene separation Blend membranes Pebax^(■)2533 PEG600
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A mini review on oxidative dehydrogenation of propane over boron nitride catalysts
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作者 Zhu Fu De-Zheng Li +5 位作者 Li-Dai Zhou Yu-Ming Li Jia-Wen Guo Yu-Qiao Li Hui-Min Liu Qi-Jian Zhang 《Petroleum Science》 SCIE EI CAS CSCD 2023年第4期2488-2498,共11页
Oxidative dehydrogenation of propane is an attractive route for the synthesis of propylene due to its favorable thermodynamic and kinetic characteristics, however, it is challenging to realize high selectivity towards... Oxidative dehydrogenation of propane is an attractive route for the synthesis of propylene due to its favorable thermodynamic and kinetic characteristics, however, it is challenging to realize high selectivity towards propylene. Recently, it has been discovered that boron nitride (BN) is a promising catalyst that affords superior selectivity towards propylene in oxidative dehydrogenation of propane. Summarizing the progress and unravelling the reaction mechanism of BN in oxidative dehydrogenation of propane are of great significance for the rational design of efficient catalysts in the future. Herein, in this review, the underlying reaction mechanisms of oxidative dehydrogenation of propane over BN are extracted;the developed BN catalysts are classified into pristine BN, functionalized BN, supported BN and others, and the applications of each category of BN catalysts in oxidative dehydrogenation of propane are summarized;the challenges and opportunities on oxidative dehydrogenation of propane over BN are pointed out, aiming to inspire more studies and advance this research field. 展开更多
关键词 Oxidative dehydrogenation of propane Boron nitride propylene Reaction mechanism
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Sub-nanometer Pt_(2)In_(3) intermetallics as ultra-stable catalyst for propane dehydrogenation
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作者 Yanan Xing Guiyue Bi +11 位作者 Xiaoli Pan Qike Jiang Yuanlong Tan Yang Su Leilei Kang Bonan Li Lin Li Aiqin Wang Jingyuan Ma Xiaofeng Yang Xiao Yan Liu Tao Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期304-312,I0009,共10页
Pt-based catalysts are the typical industrial catalysts for propane dehydrogenation(PDH),which still suffer from insufficient lo ng-term durability due to the structu ral instability and coke deposition.A commercial ... Pt-based catalysts are the typical industrial catalysts for propane dehydrogenation(PDH),which still suffer from insufficient lo ng-term durability due to the structu ral instability and coke deposition.A commercial γ-Al_(2)O_(3) supported thermally robust sub-nanometer Pt2In3intermetallic catalyst with atomically ordered structure and rigorously separated Pt single atoms was fabricated,which showed outstanding robustness in 240 h long-term operation at 600℃ with the deactivation rate constant kdas low as0.00078 h^(-1), ranking among the lowest reported values.Based on various in situ characterizations and theoretical calculations,it was proved that the catalyst stability not only resulted from the separated Pt single-atom sites but also significantly affected by the distance of adjacent Pt atoms.An increasing distance to 3.25 A in the Pt_(2)In_(3)could induce a weak π-adsorption configuration of propylene on Pt sites,which facilitated the desorption of propylene and restrained the side reactions like coking. 展开更多
关键词 propane dehydrogenation propylene Pt-In catalyst Intermetallic compounds Pt_(2)ln_(3)
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Mesoporous carbons as metal-free catalysts for propane dehydrogenation: Effect of the pore structure and surface property 被引量:8
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作者 Zhong-Pan Hu Jin-Tao Ren +2 位作者 Dandan Yang Zheng Wang Zhong-Yong Yuan 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第9期1385-1394,共10页
Nanocarbon materials have been used as important metal-free catalysts for various reactions including alkane dehydrogenation.However,clarifying the active sites and tuning the nanocarbon structure for direct dehydroge... Nanocarbon materials have been used as important metal-free catalysts for various reactions including alkane dehydrogenation.However,clarifying the active sites and tuning the nanocarbon structure for direct dehydrogenation have always been significantly challenging owing to the lack of fundamental understanding of the structure and surface properties of carbon materials.Herein,mesoporous carbon materials with different pore ordering and surface properties were synthesized through a soft-templating method with different formaldehyde/resorcinol ratios and carbonization temperatures and used for catalytic dehydrogenation of propane to propylene.The highly ordered mesoporous carbons were found to have higher catalytic activities than disordered and ordered mesoporous carbons,mainly because the highly ordered mesopores favor mass transportation and provide more accessible active sites.Furthermore,mesoporous carbons can provide a large amount of surface active sites owing to their high surface areas,which is favorable for propane dehydrogenation reaction.To control the surface oxygenated functional groups,highly ordered mesoporous carbons were carbonized at different temperatures(600,700,and 800℃).The propylene formation rates exhibit an excellent linear relationship with the number of ketonic C=O groups,suggesting that C=O groups are the most possible active sites. 展开更多
关键词 Mesoporous carbons propane DEHYDROGENATION propylene Metal-free catalysis
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Effect of pH on the catalytic performance of PtSn/B-ZrO2 in propane dehydrogenation 被引量:3
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作者 Zhonghai Ji Dengyun Miao +2 位作者 Lijun Gao Xiulian Pan Xinhe Bao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第4期719-729,共11页
Boron-modified ZrO2(B-ZrO2)was synthesized under various pH values(9,10,and 11)and used as the supports of PtSn catalysts(PtSn/B-ZrO2-x)for non-oxidative dehydrogenation of propane.The NH3-TPD and pyridine IR show tha... Boron-modified ZrO2(B-ZrO2)was synthesized under various pH values(9,10,and 11)and used as the supports of PtSn catalysts(PtSn/B-ZrO2-x)for non-oxidative dehydrogenation of propane.The NH3-TPD and pyridine IR show that only Lewis acid is present and the acid strength increases with the synthesis pH.PtSn/B-ZrO2-10 exhibits the best catalytic performance with an initial propane conversion of 36%and a deactivation rate constant(kd)of 0.0127 h^-1.The XPS results indicate that the electronic properties of Pt and SnOx are affected not only by their interaction but also by the interaction with support.After a careful analysis of the oxygen storage capacity and activity in CO oxidation,it is hypothesized that the interaction between Pt and Sn becomes stronger following the order:PtSn/B-ZrO2-9<PtSn/B-ZrO2-11<PtSn/B-ZrO2-10.The characterization with TPO and Raman on spent catalysts exhibits that more hydrogen deficient coke forms on the support and less coke deposits on the metal surface of PtSn/B-ZrO2-10.The results reveal that the interaction between Pt and Sn is influenced by their respective interaction with the support and a moderate interaction between the metal species and the support is desired. 展开更多
关键词 propane dehydrogenation Platinum-tin propylene SUPPORT Stability
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Modeling-based optimization of a fixed-bed industrial reactor for oxidative dehydrogenation of propane 被引量:5
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作者 Ali Darvishi Razieh Davand +1 位作者 Farhad Khorasheh Moslem Fattahi 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2016年第5期612-622,共11页
An industrial scale propylene production via oxidative dehydrogenation of propane (ODHP) in multi-tubular re- actors was modeled. Multi-tubular fixed-bed reactor used for ODHP process, employing 10000 of small diame... An industrial scale propylene production via oxidative dehydrogenation of propane (ODHP) in multi-tubular re- actors was modeled. Multi-tubular fixed-bed reactor used for ODHP process, employing 10000 of small diameter tubes immersed in a shell through a proper coolant flows. Herein, a theory-based pseudo-homogeneous model to describe the operation of a fixed bed reactor for the ODHP to correspondence olefln over V2O5/γ-Al203 catalyst was presented. Steady state one dimensional model has been developed to identify the operation parameters and to describe the propane and oxygen conversions, gas process and coolant temperatures, as well as other pa- rameters affecting the reactor performance such as pressure. Furthermore, the applied model showed that a double-bed multitubular reactor with intermediate air injection scheme was superior to a single-bed design due to the increasing of propylene selectivity while operating under lower oxygen partial pressures resulting in propane conversion of about 37.3%. The optimized length of the reactor needed to reach 100% conversion of the oxygen was theoretically determined. For the single-bed reactor the optimized length of 11.96 m including 0.5 m of inert section at the entrance region and for the double-bed reactor design the optimized lengths of 5.72 m for the first and 7.32 m for the second reactor were calculated. Ultimately, the use of a distributed oxygen feed with limited number of injection points indicated a significant improvement on the reactor performance in terms of propane conversion and propylene selectivity. Besides, this concept could overcome the reactor run- away temperature problem and enabled operations at the wider range of conditions to obtain enhanced propyl- ene production in an industrial scale reactor. 展开更多
关键词 Fixed-bed reactor Mathematical modeling Oxidative dehydrogenation of propane propylene V2O5/γ-Al203 catalyst OPTIMIZATION
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CrOx supported on high-silica HZSM-5 for propane dehydrogenation 被引量:3
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作者 Zhong-Pan Hu Yansu Wang +1 位作者 Dandan Yang Zhong-Yong Yuan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第8期225-233,I0008,共10页
Industrial propane dehydrogenation(PDH)catalysts generally suffer from low catalytic stability due to the coke formation onto the catalyst surface to cover the active sites.The exploitation of an efficient catalyst wi... Industrial propane dehydrogenation(PDH)catalysts generally suffer from low catalytic stability due to the coke formation onto the catalyst surface to cover the active sites.The exploitation of an efficient catalyst with both high catalytic selectivity and long-term stability toward PDH is of great importance but challenging to make.Herein CrOx supported on high-silica HZSM-5 with a SiO2/Al2O3 ratio of 260(Cr/Z-5(260)is synthesized by a simple wet impregnation method,which exhibits high catalytic activity,good selectivity and excellent stability for PDH.At a weight hourly space velocity(WHSV)of 0.59 h-1,a propylene formation rate of 4.1 mmol g-1cath-1(~32.6% propane conversion and ~94.2% propylene selectivity)can be maintained over the 5%Cr/Z-5(260)catalyst after 50 h time on stream,which is much better than commercial Cr/Al2O3(Catofin process,catalyst life is several hours)at the same reaction conditions.With increasing the WHSV to 5.9 h-1,a high propylene formation rate of 27.9 mmol gcat-1h-1can be obtained over the 5%Cr/Z-5(260)catalyst after 50 h time on stream,demonstrating a very promising PDH catalyst.Characterization results and Na+doping experiments reveal that the Cr species combined with Br?nsted acid sites in Cr/HZSM-5 catalysts are responsible for the high catalytic performance.In particular,the Br?nsted acid sites in HZSM-5 zeolite could increase the propane adsorption and enhance the C–H bond activation.Furthermore,the high surface area and well-defined pores of HZSM-5 zeolite can provide a special environment for the dispersion and stabilization of Cr species,thus guaranteeing high catalytic activity and stability. 展开更多
关键词 propane dehydrogenation ZSM-5 zeolite Chromium oxide propylene BrΦnsted acid sites
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Ultrafine tuning of the pore size in zeolite A for efficient propyne removal from propylene 被引量:1
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作者 Chaohui He Rajamani Krishna +3 位作者 Yang Chen Jiangfeng Yang Jinping Li Libo Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2021年第9期217-221,共5页
The removal of trace propyne(C_(3)H_(4))from propyne/propylene(C_(3)H_(4)/C_(3)H_(6))mixtures is a technical and challenging task during the production of polymer-grade propylene in view of their very similar size and... The removal of trace propyne(C_(3)H_(4))from propyne/propylene(C_(3)H_(4)/C_(3)H_(6))mixtures is a technical and challenging task during the production of polymer-grade propylene in view of their very similar size and physical properties.While some progress has been made,it is still very challenging to use some highly stable and commercially available porous materials via an energy-efficient adsorptive separation process.Herein,we report the ultrafine tuning of the pore apertures in type-A zeolites for the highly efficient removal of trace amounts of C_(3)H_(4)from C_(3)H_(4)/C_(3)H_(6)mixtures.The resulting ion-exchanged zeolite 5 A exhibits a large C_(3)H_(4)adsorption capacity(2.3 mmol g^(-1)under 10^(-4)MPa)and high C_(3)H_(4)/C_(3)H_(6)selectivity at room temperature,which were mainly attributed to the ultrafine-tuned pore size that selectively blocks C_(3)H_(6)molecules,while maintaining the stro ng adsorption of C_(3)H_(4)at low pressure region.High purity of C_(3)H_(6)(>99.9999%)can be directly obtained on this material under ambient conditions,as demonstrated by the experimental breakthrough curves obtained for both 1/99 and 0.1/99.9(V V)C_(3)H_(4)/C_(3)H_(6) mixtures. 展开更多
关键词 Type-A zeolite Ion-exchange Pore tuning Propyne/propylene separation Breakthrough experiments
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The effect of the Ce content on the oxidative dehydrogenation of propane over CrOy-CeO2/γ-Al2O3 catalysts
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作者 Cheng Zuo Man Wu Qingjie Guo 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2020年第12期3035-3043,共9页
A series of CrOy(17.5 wt%)-CeO2(X wt%)/γ-Al2O3 catalysts(X=0,0.5,2,5,8)with various Ce contentswere prepared by a wetness impregnation method and were applied to the dehydrogenation of propane to propylene at 550℃ a... A series of CrOy(17.5 wt%)-CeO2(X wt%)/γ-Al2O3 catalysts(X=0,0.5,2,5,8)with various Ce contentswere prepared by a wetness impregnation method and were applied to the dehydrogenation of propane to propylene at 550℃ and 0.1 MPa.The prepared catalysts were characterized by BET,H2-TPR,O2-TPD,XPS,XRD,SEM-EDS and Raman spectroscopy.Among the prepared catalysts,the 17.5Cr-2Ce/Al catalyst with the largest amount of lattice oxygen exhibited the best catalytic performance for the dehydrogenation of propane to propylene with lattice oxygen.The decreased presence of oxygen defects and reducibility were the factors responsible for the improved dehydrogenation activity of the catalysts.The CeO2 layer could inhibit the evolution of lattice oxygen(O2^−)to electrophilic oxygen species(O2^−),and the oxygen defects on the catalyst surfacewere reduced.The inhibited lattice oxygen evolution prevented the deep oxidation of propane or propylene,the average COx selectivity decreased from 24.41%(17.5Cr/Al)to 5.71%(17.5Cr-2Ce/Al),and the average propylene selectivity increased from 60.15%(17.5Cr/Al)to 85.05%(17.5Cr-2Ce/Al). 展开更多
关键词 OXIDATION SELECTIVITY propane propylene FLUIDIZED-BED Oxygen carrier
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锐钛矿型TiO_(2)负载Ni单原子用于催化丙烷脱氢
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作者 张倩 江训柱 +2 位作者 苏杨 赵阳 乔波涛 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第2期105-113,共9页
丙烯市场需求日益增长,丙烷脱氢(PDH)被认为是最有前途的丙烯定向生产技术之一.作为PDH商业催化剂,贵金属Pt的高成本和CrO_(x)基催化剂的毒性使它们的发展受到限制.镍基催化剂因具有廉价、环保的特点,在多种催化反应的应用中引起了研究... 丙烯市场需求日益增长,丙烷脱氢(PDH)被认为是最有前途的丙烯定向生产技术之一.作为PDH商业催化剂,贵金属Pt的高成本和CrO_(x)基催化剂的毒性使它们的发展受到限制.镍基催化剂因具有廉价、环保的特点,在多种催化反应的应用中引起了研究人员的广泛关注.然而,镍在高温烷烃脱氢反应中的应用较少,目前,保持反应中镍(II)物种的稳定存在仍然是镍基PDH催化剂的主要挑战.近来,单原子催化剂(SAC)在烷烃碳氢键活化过程中表现出优异的催化性能,具有较好的丙烯选择性和出色的稳定性.当镍以单个原子的形式分散在载体上时,它更有可能以带正电的状态存在,但金属单原子的稳定存在是具有挑战性的.本文以锐钛矿型的二氧化钛为载体,采用等体积浸渍法分别制备了0.05 wt%载量的单个原子分散的催化剂(Ni SAC,Ni_(1)/A-TiO_(2))和5 wt%载量的纳米颗粒(NP)催化剂(Ni_(NP)/A-TiO_(2)).结合球差电镜、原位漫反射傅里叶变换红外光谱和X射线吸收光谱等表征结果表明,Ni SAC催化剂主要含有单个Ni原子,以Ni(II)价态孤立地分散在载体上,而Ni_(NP)/A-TiO_(2)催化剂中的Ni物种主要以纳米粒子(1±0.2 nm)的形式存在.在580℃的PDH反应中,Ni_(1)/A-TiO_(2)催化剂表现出较好的本征活性和丙烯选择性,而且比相应的Ni NPs催化剂具有更好的抗积炭稳定性,在Ni_(1)/A-TiO_(2)上得到的丙烯产率约为1.96 molC_(3)H_(6)gNi^(-1)h^(-1),超过NiNP/A-TiO_(2)样品(0.03 molC_(3)H_(6)gNi^(-1)h^(-1))的65倍,Ni SAC催化剂的丙烯时空收率(STYC_(3)H_(6))约为0.2 kg h^(-1) kg_(cat)^(-1),与文献报道的大部分非贵金属催化剂STY值相当(0.02-0.3 kg h^(-1) kg_(cat)^(-1)).还原后的TiO_(2)载体因具有丰富的氧空位(OVs)和配位不饱和的Ti^(3+)表现出一定的活性,而Ni SAC得到了更高的丙烷转化率,但Ni单原子的引入并没有增加OVs和Ti^(3+)的浓度,Ni单原子催化剂的活化能低于纯载体,说明两者的活性位不同.此外,在还原条件下,由于Ni NPs与TiO_(2)载体之间的强相互作用,Ni NPs位点被TiO_(x)覆盖层(~2 nm)包裹,从而显示出较差的反应活性.综上所述,本文报道了Ni单原子催化剂在丙烷直接脱氢反应中比相应的Ni NP催化剂表现出更好的反应性能,体现了具有孤立活性位点的单原子催化剂在丙烷脱氢反应中的优势,为今后探究可用于丙烷脱氢反应的单原子催化剂的制备和应用提供参考. 展开更多
关键词 丙烷脱氢 单原子催化剂 原子利用率 丙烯选择性 稳定性
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实时参数整定的无模型自适应控制算法及其在气体分馏装置的应用
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作者 谷小峰 马庆鲁 +1 位作者 黄文杰 李国庆 《石油炼制与化工》 CAS CSCD 北大核心 2024年第3期97-106,共10页
现有无模型自适应控制(MFAC)算法中,4个模型参数λ,ρ,η,μ在控制过程中保持不变,导致伪偏导对控制进程影响小、算法自适应能弱等问题。利用径向基函数(RBF)神经网络,基于系统的输入和伪偏导,以期望输出与实时输出差值为训练误差的实... 现有无模型自适应控制(MFAC)算法中,4个模型参数λ,ρ,η,μ在控制过程中保持不变,导致伪偏导对控制进程影响小、算法自适应能弱等问题。利用径向基函数(RBF)神经网络,基于系统的输入和伪偏导,以期望输出与实时输出差值为训练误差的实时整定参数,提高了MFAC的自适应能力;进而提出了一种新的离散时间非线性系统紧格式动态线性化MFAC算法(简称BRF-MFAC算法),并通过非线性系统控制案例验证了RBF-MFAC良好的跟踪性能;将其应用于某炼油厂0.3 Mt/a气体分馏装置,相比现有MFAC算法,丙烯塔单输入单输出(SISO)系统丙烯产品纯度达标操作调整次数减少42.4%,多输入多输出(MIMO)系统丙烯产品纯度和产量达标操作调整次数减少78.0%。 展开更多
关键词 过程控制 神经网络 参数估计 气体分馏装置 丙烯塔
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微相分离型聚丙烯热塑性弹性体的力学性能
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作者 刘永超 孙长红 +2 位作者 丁紫阳 孙为云 张磊 《弹性体》 CAS 2024年第1期43-49,共7页
为了制备相畴尺寸均匀、细小,形态结构易控,力学性能稳定的聚丙烯热塑性弹性体(PTPE),设计出了从聚丙烯(PP)与弹性体的均相体系出发,利用在硫化过程中的能效应使之发生微相分离,能效应和熵效应控制组分相畴的尺寸和形态以制备PTPE的原... 为了制备相畴尺寸均匀、细小,形态结构易控,力学性能稳定的聚丙烯热塑性弹性体(PTPE),设计出了从聚丙烯(PP)与弹性体的均相体系出发,利用在硫化过程中的能效应使之发生微相分离,能效应和熵效应控制组分相畴的尺寸和形态以制备PTPE的原理和技术,研究了橡/塑比、橡胶配比、PP相对分子质量、引发剂用量、架桥剂用量、反应温度对样品化学结构和力学性能的影响。结果表明,在125℃反应温度下样品配方为:橡塑质量比为70/30、乙丙橡胶与丁苯质量比为80∶20、引发剂用量为2.14份、架桥剂用量为18.2份时,制得试样的综合力学性能最佳,拉伸强度、100%定伸应力、扯断伸长率、撕裂强度、扯断永久变形分别为11.25 MPa、8.78 MPa、384%、58.5 kN/m、78%。 展开更多
关键词 乙丙弹性体 丁苯弹性体 聚丙烯热塑性弹性体 微相分离
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