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Ca_(2)MnO_(4)-layered perovskite modified by NaNO_(3)for chemical-looping oxidative dehydrogenation of ethane to ethylene

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Chinese Journal of Chemical Engineering 2024年第4期68卷 53-64页

作者： Weixiao Ding Kun Zhao Shican Jiang Zhen Huang Fang He College of Chemistry and Bioengineering Guilin University of TechnologyGuilin 541006China Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640China School of Chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China

Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox ***,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise *** modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) *** findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.

关键词： Chemical-looping oxidative dehydrogenation ethane Ethylene NaNO_(3)-doped Ca_(2)MnO_(4)redox catalyst Layered perovskites

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Zeolites for the separation of ethylene,ethane,and ethyne

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Frontiers of Chemical Science and Engineering 2024年第9期18卷 137-146页

作者： Binyu Wang Qiang Li Haoyang Zhang Jia-Nan Zhang Qinhe Pan Wenfu Yan State Key Laboratory of Inorganic Synthesis&Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450012China Key Laboratory of Advanced Materials of Tropical Island Resources(Ministry of Education) School of Chemistry and Chemical EngineeringHainan UniversityHaikou 570228China

The cost-effective separation of ethylene(C_(2)H_(4)),ethyne(C_(2)H_(2)),and ethane(C_(2)H_(6))poses a significant challenge in the contemporary chemical *** contrast to the energy-intensive high-pressure cryogenic distillation process,zeolite-based adsorptive separation offers a low-energy *** review provides a concise overview of recent advancements in the adsorptive separation of C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)using zeolites or zeolite-based *** commences with an examination of the industrial significance of these compounds and the associated separation ***,it systematically examines the utilization of various types of zeolites with diverse cationic species in such separation *** then it explores how different zeolitic structures impact adsorption and separation capabilities,considering principles such as cation-πinteraction,π-complexation,and steric separation concerning C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)***,it discusses methods to enhance the separation performance of zeolites and zeolite-based adsorbents,encompassing structural design,modifications,and ion exchange ***,it summarizes current research trends and future directions,highlighting the potential application value of zeolitic materials in the field of C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)separation and offering recommendations for further investigation.

关键词： zeolite ethylene ethane cation-πinteraction π-complexation

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ethane Chemical Looping Oxidative Dehydrogenation to Ethylene over Co_(2)O_(3)(Fe_(2)O_(3),NiO)/LaCoO_(3) Oxygen Carriers

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China Petroleum Processing & Petrochemical Technology 2024年第3期26卷 33-41页

作者： Liang Hao Meng Jinhong Sun Jie Wei Dongkai Shenyang Ligong University Shenyang Liaoning110159 Ecological Environment Protection Comprehensive Administrative Law Enforcement Team FushunLiaoning113006

ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for converting ethane to *** the current study MeO/LaCoO_(3)(MeO=Fe_(2)O_(3),NiO or Co_(2)O_(3))composite metal oxides were prepared via citrate gel and impregnation methods,and used as oxygen carriers for CL-ODH.X-ray diffraction results indicated that all oxygen carriers had a perovskite structure even after eight redox *** a reaction temperature of 650°C,a reaction pressure of 0.1 MPa,and a weight hourly space velocity(WHSV)of 7500 mL/(g·h),ethane conversion over Co_(2)O_(3)/LaCoO_(3) reached 100%and ethylene selectivity reached 60%,both of which were better than corresponding values attained over Fe_(2)O_(3)/LaCoO_(3) and NiO/LaCoO_(3).Ethylene selectivity remained stable for 80 cycles over Co_(2)O_(3)/LaCoO_(3),then decreased gradually after 80 cycles.X-ray photoelectron spectroscopy results and evaluation results indicated that lattice oxygen and O_(2)2-had a direct relationship with ethane conversion and ethylene ***_(2)O_(3)/LaCoO_(3) exhibited a strong capacity to release and absorb oxygen,mainly due to interaction between Co_(2)O_(3) and LaCoO_(3).

关键词： chemical looping oxidative dehydrogenation ethane ethylene oxygen carrier perovskite

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Mn-doped SrCoO_(3-δ) Perovskite Oxides for Ethylene Production via Chemical Looping Oxidative Dehydrogenation of ethane

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China Petroleum Processing & Petrochemical Technology 2024年第3期26卷 53-62页

作者： Li Zhi Liu Linjiao Hao Daijun Ren Xiaohang Shen Fangxia Li Xin Yu Anping Luoyang R&D Center of Technology of Sinopec Engineering(Group)Co.Ltd. Luoyang 471003China

Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers. Inthis study, perovskite-type oxide SrCoO_(3-δ) and B-site Mn ion-doped oxygen carriers (SrCo_(1-x)MnxO_(3-δ), x=0.1, 0.2, 0.3)were prepared and tested for the CL-ODH of ethane. The oxygen-deficient perovskite SrCoO_(3-δ) exhibited high ethyleneselectivity of up to 96.7% due to its unique oxygen vacancies and lattice oxygen migration rates. However, its low ethyleneyield limits its application in the CL-ODH of ethane. Mn doping promoted the reducibility of SrCoO_(3-δ) oxygen carriers,thereby improving ethane conversion and ethylene yield, as demonstrated by characterization and evaluation experiments.X-ray diffraction results confirmed the doping of Mn into the lattice of SrCoO_(3-δ), while X-ray photoelectron spectroscopy(XPS) indicated an increase in lattice oxygen ratio upon incorporation of Mn into the SrCoO_(3-δ) lattice. Additionally, H2temperature-programmed reduction (H2-TPR) tests revealed more peaks at lower temperature reduction zones and a declinein peak positions at higher temperatures. Among the four tested oxygen carriers, SrCo0.8Mn0.2O_(3-δ) exhibited satisfactoryperformance with an ethylene yield of 50% at 710 °C and good stability over 20 redox cycles. The synergistic effect of Mnplays a key role in increasing ethylene yields of SrCoO_(3-δ) oxygen carriers. Accordingly, SrCo0.8Mn0.2O_(3-δ) shows promisingpotential for the efficient production of ethylene from ethane via CL-ODH.

关键词： ethane ethylene perovskite chemical looping oxidative dehydrogenation

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Coupling CO_(2)reduction with ethane aromatization for enhancing catalytic stability of iron-modified ZSM-5

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Journal of Energy Chemistry 2022年第3期31卷 210-217,I0007页

作者： Zhenhua Xie Elaine Gomez Dong Wang Ji Hoon Lee Tiefeng Wang Jingguang G.Chen Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA Chemistry Division Brookhaven National LaboratoryUptonNY 11973USA Department of Chemical Engineering Tsinghua UniversityBeijing100084 BeijingChina

The shale gas revolution and the carbon-neutrality goal are motivating the landscape toward the synthesis of value-added chemicals or fuels from underutilized ethane with the assistance of greenhouse gas CO_(2).Combining ethane aromatization with CO_(2)reduction offers an opportunity to directly produce liquid products for facile separation,storage,and *** the present work,Fe/ZSM-5 catalysts showed promise in the simultaneous CO_(2)reduction and ethane aromatization at atmospheric pressure and 873 *** catalysts were further investigated using X-ray diffraction(XRD)and X-ray absorption fine structure(XAFS)measurements under in-situ conditions,indicating that most of Fe species existed in the form of Fe oxides and a portion of Fe was incorporated into the ZSM-5 framework generating Lewis acid *** types of Fe species remained almost unchanged under reaction conditions,contributing to an enhanced aromatization activity of Fe/*** effects of CO_(2)and steam on the acid sites and in turn aromatization activity were also investigated by transient studies,which exhibited a reversible modification ***,CO_(2)was identified to be critical to enhance coke resistance and in turn catalyst *** work highlights the feasibility of using CO_(2)to assist the upgrading of abundant ethane from shale gas to aromatics over non-precious Fe-based zeolite catalysts.

关键词： ethane CO_(2) Aromatization Fe-modified ZSM-5

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A robust ethane-trapping metal-organic framework for efficient purification of ethylene

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Science China Chemistry 2021年第4期64卷 666-672页

作者： Sisi Jiang Liangying Li Lidong Guo Changhua Song Qiwei Yang Zhiguo Zhang Yiwen Yang Qilong Ren Zongbi Bao Key Laboratory of Biomass Chemical Engineering of the Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

Owing to the similar physicochemical properties between ethane(C_(2)H_(6))and ethylene(C_(2)H_(4)),obtaining polymerization-grade C_(2)H_(4)(≥99.95%pure)is still a tricky problem in the petrochemical ***,we report a robust scandium-based metalorganic framework(Sc BPDC),which is connected by oxygen-rich phenyl ligand with exceptionally high thermal stability(up to873 K)and capacity of C_(2)H_(6)(4.94 mmol/g at 100 k Pa and 283 K),exhibiting superior separation performance of C_(2)H_(6)/C_(2)H_(4) mixture(the IAST selectivity is up to 1.7 at 283 K).Importantly,Sc BPDC can produce 8.96 L/kg C_(2)H_(4) with≥99.99%purity while the C_(2)H_(4)/C_(2)H_(6)(50:50,v/v)as the mixture injection and the low isosteric heat of Sc BPDC(16.4 k J/mol for C_(2)H_(6))validates the facility of adsorbent ***,theoretical calculations demonstrate the C_(2)H_(6) molecules are trapped in the nonpolar pore surface via C–H···πand C–H···O interactions between multiple hydrogen atoms of C_(2)H_(6) and the host framework.

关键词： metal-organic frameworks adsorption separation ethane ethylene

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Numerical investigation of complex chemistry performing in Ptcatalyzed oxidative dehydrogenation of ethane fixed-bed reactors

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Chinese Journal of Chemical Engineering 2020年第3期28卷 793-807页

作者： Zhongfeng Geng Hao Deng Yonghui Li Minhua Zhang Key Laboratory for Green Chemical Technology of Ministry of Education.R&D Center for Petrochemical Technology Tianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China

Ethylene is one of the most important basic chemicals in the modern chemical *** or catalytic cracking of hydrocarbons is the main industrial technologies nowadays,which suffer from equilibriumlimitation and rapid coke *** oxidative dehydrogenation of ethane(ODHE)is considered to be a promising alternative process since it overcomes equilibrium-limitations,avoids catalyst deactivation by coke formation,and decreases the number of side *** this study,particle-resolved 2 D CFD simulations of fixed-beds filled with eggshell catalysts coupled with micro-kinetics of Pt-catalyzed ODHE were performed to understand the effect of operation conditions and catalyst properties on ethylene *** catalyst bed was created by discrete element method(DEM)and the central longitudinal section of the reactor tube was defined as the 2 D simulation *** of the homogeneous and catalytic heterogeneous chemical reactions were described by detailed micro-kinetics within the particle-resolved CFD *** first,the established model of monolith reactors was verified by comparing the simulated results with experimental results reported in ***,the effects of operation conditions and catalyst concentration on the ethylene selectivity in randomly packed beds were *** specific variation of certain operation conditions including inlet flow rate,inlet temperature,pressure,inlet C2 H6/O2 ratio and N2 dilution ratio can effectively increase ethylene *** the reduction of ratio of catalytic active area to geometric area Fcat/georepresenting catalyst properties from 140 to 30 increases the selectivity from 42.2%to 59.3%.This research can provide reference for the industrialization of ODHE process in the future.

关键词： ethane Ethylene Oxidative dehydrogenation Selectivity CFD Fixed-bed

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Visible-light driven room-temperature coupling of methane to ethane by atomically dispersed Au on WO_(3)

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Journal of Energy Chemistry 2021年第10期30卷 195-202,I0006页

作者： Xing Yang Wu Zhiyuan Tang Xiaoxu Zhao Xin Luo Stephen John Pennycook Song Ling Wang China-UK Low Carbon College Shanghai Jiao Tong UniversityShanghai 201306China School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Optoelectronic Materials and Technologies Centre for Physical Mechanics and BiophysicsSchool of PhysicsSun Yat-sen UniversityGuangzhou 510275GuangdongChina Institute Department of Materials Science and Engineering National University of SingaporeSingapore 117575Singapore Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Gold(Au)as co-catalyst is remarkable for activating methane(CH4),especially atomically dispersed Au with maximized exposing active sites and specific electronic ***,singlet oxygen(^(1)O_(2))typically manifests a mild redox capacity with a high selectivity to attack organic ***(PMS)favors to produce oxidative species 102 during the photocatalytic ***,combining atomic Au as co-catalyst and ^(1)O_(2) as oxidant is an effective strategy to selectively convert ***,we synthesized atomically dispersed Au on WO_(3)(Au/WO_(3)),where Au was in the forms of single atoms and *** room temperature,such Au/WO_(3) exhibited enhanced photocata lytic conversion of CH4 to CH3 CH3 with a selectivity,up to 94%,under visible *** radicals-pathway mechanism of CH4 coupling has also been investigated through detection and trapping experiment of active *** calculations further interpret the electronic structure of Au/WO_(3) and tip-enhanced local electric field at the Au sites for promoting CH4 conversion.

关键词： Photocatalysis Single-atom Au Methane ethane Visible light

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The effect of oxidation of ethane to oxygenates on Pt-and Zn-containing LTA zeolites with tunable selectivity

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Journal of Energy Chemistry 2019年第3期28卷 42-48页

作者： Baoyu Liu Su Cheun Oh Huiyong Chen Dongxia Liu School of Chemical Engineering and Light Industry Guangdong University of Technology Department of Chemical and Biomolecular Engineering University of Maryland College Park School of Chemical Engineering Northwest University

Platinum and zinc containing LTA zeolite catalysts with tunable meso/microporosity were prepared by using ligand-metal precursors under hydrothermal condition. These materials were employed for oxidation of ethane to oxygenates using hydrogen peroxides as oxidant under mild reaction condition. The results showed that platinum and zinc loaded LTA zeolites were effective for the partial oxidation of ethane with hydrogen peroxide giving the desired C_2 oxygenates. Moreover, the C_1 oxygenates were also obtained through subsequent C–C bond scission pathways. The over oxidation of ethanol/methanol to acetic acid/formic acid could be inhibited through the introduction of mesoporosity in LTA zeolites. Our findings for oxidation of ethane suggested that the selectivity to the oxidation products such as alcohols and acids could be tailored by tuning the metal species within the LTA zeolites and porosity of catalysts, indicating that a balance between the meso/microporosity and metal species in LTA zeolites can be realized for desirable catalysis by one-pot synthesis of zeolites. In addition, the selectivity to oxygenates can also be tuned by control of the reaction conditions, i.e. concentration of hydrogen peroxide or reaction time.

关键词： Zeolite Hierarchical ethane Porosity

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Design and analysis of dual mixed refrigerant processes for high-ethane content natural gas liquefaction

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Chinese Journal of Chemical Engineering 2021年第1期34卷 354-364页

作者： Ting He Wensheng Lin Institute of Refrigeration and Cryogenics Shanghai Jiao Tong UniversityShanghai 200240China

Recovery and purification of ethane has a significant impact on economic benefit improvement of the high-ethane content natural ***,current LNG-NGL integrated processes mainly focus on conventional natural gas,which are not applicable to natural gas with high ethane *** fill this gap,three dual mixed refrigerant processes are proposed for simulation study of high-ethane content natural gas *** proposed processes are optimized by a combination method of sequence optimization and genetic *** analysis is conducted to evaluate the three processes from the energetic and exergetic points of *** results show that the power consumption of Process 3 which compressing natural gas after distillation is the *** safety or other considerations,some common compositions of the mixed refrigerant may need to be removed under certain *** this,case studies of mixed refrigerant involving six composition combinations are carried out to investigate the effects of refrigerant selection on the process performance.

关键词： Natural gas liquefaction ethane Dual mixed refrigerant cycle Cryogenic distillation Refrigerant selection

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