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Hydrogen production via chemical looping reforming of coke oven gas

Green Energy & Environment 2021年第5期6卷 678-692页

作者： Kun Yang Zhenhua Gu Yanhui Long Shen Lin Chunqiang Lu Xing Zhu Hua Wang Kongzhai Li State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Kunming University of Science and TechnologyKunming650093China Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming650093China

Coke oven gas(COG)is one of the most important by-products in steel industry,and the conversion of COG to value-added products has attracted much attention from both economic and environmental views.In this work,we use the chemical looping reforming technology to produce pure H_(2) from COG.A series of La1-xSrxFeO_(3)(x?0,0.2,0.3,0.4,0.5,0.6)perovskite oxides were prepared as oxygen carriers for this purpose.The reduction behaviors of La1-xSrxFeO_(3) perovskite by different reducing gases(H_(2),CO,CH4 and the mixed gases)are investigated to discuss the competition effect of different components in COG for reacting with the oxygen carriers.The results show that reduction temperatures of H_(2) and CO are much lower than that of CH4,and high temperatures(>800℃)are requested for selective oxidation of methane to syngas.The co-existence of CO and H_(2) shows weak effect on the equilibrium of methane conversion at high temperatures,but the oxidation of methane to syngas can inhibit the consumption of CO and H_(2).The doping of suitable amounts of Sr in LaFeO_(3) perovskite(e.g.,La0.5Sr0.5FeO_(3))significantly promotes the activity for selective oxidation of methane to syngas and inhibits the formation of carbon deposition,obtaining both high methane conversion in the COG oxidation step and high hydrogen yield in the water splitting step.The La0.5Sr0.5FeO_(3) shows the highest methane conversion(67.82%),hydrogen yield(3.34 mmol g^(-1))and hydrogen purity(99.85%).The hydrogen yield in water splitting step is treble as high as the hydrogen consumption in reduction step.These results reveal that chemical looping reforming of COG to produce pure H_(2) is feasible,and an O_(2)-assistant chemical looping reforming process can further improves the redox stability of oxygen carrier.

关键词： Coke oven gas chemical looping reforming La1-xSrxFeO_(3) Oxygen carrier Hydrogen yield

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

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

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

chemical looping reforming(CLR)is a recent trend for syngas production,which has several merits compared to the conventional manner.One of the most important issues for CLR is to find low-cost material as oxygen carriers,so iron is a promising candidate.This paper contributes to testing the thermodynamic ability of iron-based oxygen carrier for chemical looping reforming of ethanol(CLRE).Iron thermodynamically investigated in temperature 100–1300℃and excess oxygen number(φ)0–4.It was found that the temperature andφhave an apparent effect on the gaseous composition produced from the process.Increases in temperature within the range of 100–1300℃enhanced syngas generated and reduced coke formation and CH4.Whereas,increasedφ,particularly at higher temperatures,had also enhanced syngas production as well as reduced coke formation.However,increasingφfor values beyond one had decreased syngas and not significantly reduced coke deposition.Moreover,an experimental investigation was carried out in a fixed bed reactor for more in-depth verification of iron ability as an oxygen carrier through using magnetite ore(mainly Fe3O4).It found that the effect of temperature on syngas production was consistent with that calculated thermodynamically,as syngas increased with raising the temperature through the CLRE.

关键词： Syngas chemical looping reforming Iron oxygen carrier Ethanol Coke formation Thermodynamic analysis

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Layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers for chemical looping reforming

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Chinese Journal of chemical Engineering 2020年第10期28卷 2668-2676页

作者： Jiangyong Yuan Yannan Zhao Haiwen Xu Chunqiang Lu Kun Yang Xing Zhu Kongzhai Li State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Kunming University of Science and TechnologyKunming 650093China Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming 650093China

A series of layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers were prepared for co-production of syngas and pure hydrogen via chemical looping steam reforming(CLSR).The presence of magnesium-aluminum layered double oxides(Mg Al-LDO)significantly increases the specific surface area of the mixed oxides,reduces the particle size of CeO2-based solid solution and promotes the dispersion of free Fe2O3.When reacting with methane,Mg Al-LDO supported oxygen carrier shows much lower temperature for methane oxidation than the pure CeFe-Zr-O sample,indicating enhanced low-temperature reactivity.Among different Ce-Fe-Zr-O(x)/Mg Al-LDO samples,the Ce-Fe-Zr-O(40 wt%)/Mg Al-LDO sample shows the best performance for the selective oxidation of methane to syngas and the H2 production by water splitting.After a long period of high temperature redox experiment,the Ce-Fe-Zr-O(40 wt%)/Mg Al-LDO oxygen carrier still shows high activity for syngas generation.The comparison on the morphology of the fresh and cycled oxygen carriers indicates that the Mg-Al spinel support still forms a stable skeleton structure with high dispersion of active components on the surface after the long-term cycling,which contributes to excellent redox stability of the Ce-Fe-Zr-O(40 wt%)/Mg Al-LDO oxygen carrier.

关键词： chemical looping reforming Syngas Hydrogen Ce-Fe-Zr-O(x)/MgAl-LDO Oxygen carrier

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Reduction kinetics of SrFeO_(3−δ)/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial oxidation of methane

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Frontiers of chemical Science and Engineering 2022年第12期16卷 1726-1734页

作者： Xinhe Wang Liuqing Yang Xiaolin Ji Yunfei Gao Fanxing Li Junshe Zhang Jinjia Wei State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049China School of chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China Institute of Clean Coal Technology East China University of Science and TechnologyShanghai 200237China Department of chemical and Biomolecular Engineering North Carolina State UniversityRaleighNC 27695USA

chemical looping reforming of methane is a novel and effective approach to convert methane to syngas,in which oxygen transfer is achieved by a redox material.Although lots of efforts have been made to develop high-performance redox materials,a few studies have focused on the redox kinetics.In this work,the kinetics of SrFeO_(3−δ)–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor.During the methane reduction,combustion occurs before the partial oxidation and there exists a transition between them.The weight loss due to combustion increases,but the transition region becomes less inconspicuous as the reduction temperature increased.The weight loss associated with the partial oxidation is much larger than that with combustion.The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n=3(A3 model)with an activation energy of 59.8 kJ∙mol^(‒1).The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law.The partial oxidation is half order with respect to methane pressure.The proposed rate law could well predict the reduction kinetics;thus,it may be used to design and/or analyze a chemical looping reforming reactor.

关键词： chemical looping reforming SrFeO_(3−δ) CaO·MnO nanocomposite reduction kinetics Avrami–Erofeyev model pressure-dependent term

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