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Journal of Natural Gas Chemistry 2008年第4期17卷 415-418页

作者： Xiaoping Dai Changchun Yu Qiong Wu The Key Laboratory of Catalysis China National Petroleum Corporation China University of Petroleum Beijing 102249 China

Comparison of LaFeO3, La0.8Sr0.2FeO3, and La0.8Sr0.2Fe0.9CO0.1O3 perovskite oxides as oxygen carrier for partial oxidation of methane in the absence of gaseous oxygen was investigated by continuous flow reaction and sequential redox reaction, Methane was oxidized to syngas with high selectivity by oxygen species of perovskite oxides in the absence of gaseous oxygen. The sequential redox reaction revealed that the structural stability and continuous oxygen supply in redox reaction decreased over La0.8Sr0.2Fe0.9Co0. 1O3 oxide, while LaFeO3 and La0.8Sr0.2FeO3 exhibited excellent structural stability and continuous oxygen supply.

关键词： perovskite oxides oxygen carrier methane synthesis gas continuous flow reaction sequential redox reaction

Efficient CO2 to CO conversion at moderate temperatures enabled by the cobalt and copper co-doped ferrite oxygen carrier

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Journal of Energy Chemistry 2020年第7期29卷 123-132,I0005页

作者： Yu Qiu Li Ma Dewang Zeng Min Li Dongxu Cui Yulin Lv Shuai Zhang Rui Xiao Key Laboratory of Energy Thermal conversion and control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 210096JiangsuChina

Chemical looping technology holds great potential on efficient CO2 splitting with much higher CO production and CO2 splitting rate than photocatalytic *** oxygen carrier requires high temperature(typically 850–1000°C)to ensure sufficient redox activity,but the stable and high CO2 conversion is favored at a lower temperature,leading to the degrading on the reaction kinetics as well as the low CO production and CO2 splitting *** this paper,we prepared several ternary spinels and demonstrated their performance for chemical looping CO2 splitting at moderate *** the promotion effect of Cu to cobalt ferrite reduction and reversible phase change of the reduced metals,Cu0.4 Co0.6 Fe2 O4 exhibits high CO2 splitting rate(144.6μmol g–1 min–1)and total CO production(9100μmol g–1)at 650°*** high performance of this earth-abundant spinel material is also consistent in repeated redox cycles,enabling their potential in industrial use.

关键词： Chemical looping oxygen carrier CO2 splitting Ferrite

Ce-Fe-O mixed oxide as oxygen carrier for the direct partial oxidation of methane to syngas

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Journal of Rare Earths 2010年第4期28卷 560-565页

作者：魏永刚王华李孔斋 Faculty of Metallurgy and Energy Engineering Kunming University of Science and Technology

The Ce-Fe-O mixed oxide with a ratio of Ce/Fe=7:3, which was prepared by coprecipitation method and employed as oxygen carrier, for direct partial oxidation of methane to syngas in the absence of gaseous oxygen was explored. The mixed oxide was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM), and the catalytic performances were studied in a fixed-bed quartz reactor and a thermogravimetric reactor, respectively. Approximately 99.4% H2 se...

关键词： Ce-Fe-O mixed oxide oxygen carrier methane lattice oxygen direct partial oxidation syngas rare earths

Application of Fe_2O_3/Al_2O_3 Composite Particles as oxygen carrier of Chemical Looping Combustion

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Journal of Natural Gas Chemistry 2007年第2期16卷 155-161页

作者： Fang He Hua Wang Yongnian Dai Faculty of Materials and Metallurgical Engineering Kunming University of Science and Technology Kunming 650093 Yunnan China Department of Chemical Engineering the University of Adelaide Adelaide 5005 South Australia

Chemical looping combustion （CLC） of carbonaceous compounds has been proposed, in the past decade, as an efficient method for CO2 capture without cost of extra energy penalties. The technique involves the use of a metal oxide as an oxygen carrier that transfers oxygen from combustion air to fuels. The combustion is carried out in a two-step process： in the fuel reactor, the fuel is oxidized by a metal oxide, and in the air reactor, the reduced metal is oxidized back to the original phase. The use of iron oxide as an oxygen carrier has been investigated in this article. Particles composed of 80 wt% Fe2O3, together with Al2O3 as binder, have been prepared by impregnation methods. X-ray diffraction （XRD） analysis reveals that Fe2O3 does not interact with the Al2O3 binder after multi-cycles. The reactivity of the oxygen carrier particles has been studied in twenty-cycle reduction-oxidation tests in a thermal gravimetrical analysis （TGA） reactor. The components in the outlet gas have been analyzed. It has been observed that about 85% of CH4 converted to CO2 and H2O during most of the reduction periods. The oxygen carrier has kept quite a high reactivity in the twenty-cycle reactions. In the first twenty reaction cycles, the reaction rates became slightly higher with the number of cyclic reactions increasing, which was confirmed by the scanning electron microscopy （SEM） test results. The SEM analysis revealed that the pore size inside the particle had been enlarged by the thermal stress during the reaction, which was favorable for diffusion of the gaseous reactants into the particles. The experimental results suggested that the Fe2O3/Al2O3 oxygen carrier was a promising candidate for a CLC system.

关键词： chemical looping combustion iron oxide oxygen carrier CO2 capture

Selective oxidation of methane to syngas using Pr_(0.7)Zr_(0.3)O_(2-δ): Stability of oxygen carrier

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Transactions of Nonferrous Metals Society of China 2015年第4期25卷 1248-1253页

作者：杜云鹏祝星王华魏永刚李孔斋昆明理工大学省部共建复杂有色金属资源清洁利用国家重点实验室昆明650093 昆明理工大学冶金与能源工程学院昆明650093 昆明理工大学冶金节能减排教育部工程研究中心昆明650093

Pr0.7Zr0.3O2-δ solid solution was prepared by co-precipitation method and used as an oxygen carrier in the selective oxidation of methane to syngas(methane/air redox process). The evolution on the physicochemical properties of Pr0.7Zr0.3O2-δ during the redox process was studied by means of X-ray diffraction(XRD), H2 temperature-programmed reduction(H2-TPR), O2temperature-programmed desorption(O2-TPD), Brunauer-Emmett-Teller(BET) surface area measurement and X-ray photoelectron spectroscopy(XPS) technologies. The results indicated that Pr0.7Zr0.3O2-δ solid solution showed the high activity for the methane conversion to syngas with a high CO selectivity in the range of 83.5%-88.1%. Though Pr-Zr solid solution possessed high thermal stability, lattice oxygen was obviously reduced for the recycled sample due to decreased surface oxygen which promoted oxygen vacancies. The increased oxygen vacancies seemed to enhance the oxygen transfer ability in the redox process and provided sufficient oxygen for the methane selective oxidation, resulting in a satisfactory activity. The problem of hot pot was avoided by comparing fresh, aged and recycle sample in the reaction.

关键词： methane selective oxidation oxygen carrier Pr-Zr solid solution syngas stability

Preparation and characterization of Ce_(1-x)Ni_xO_2 as oxygen carrier for selective oxidation methane to syngas in absence of gaseous oxygen

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Journal of Rare Earths 2010年第S1期28卷 357-361页

作者：魏永刚王华李孔斋祝星杜云鹏 Faculty of Metallurgical and Energy Engineering Kunming University of Science and Technology

A citric acid complex method was employed to prepare Ce/Ni mixed oxides with various Ce/Ni ratios useful for selective oxidation methane to syngas in the absence of gaseous oxygen,and the catalytic activity measurement was investigated in a fixed bed reactor at 800 *** prepared oxygen carriers were characterized by various characterization techniques such as TG-DSC,XRD and *** results of TG-DSC indicated that the Ce1-xNixO2 precursor generated a stable phase after the heat-treatment at temperatures above 800 *** XRD characterization suggested that some Ce-Ni solid solution was formed when Ni2+ ions was incorporated into the lattice of CeO2,and it led to the generation of O-vacancy which could improve the oxygen mobility in the lattice of oxygen *** was found that Ce0.8Ni0.2O2 gave the highest activity in the selective oxidation methane to syngas reaction,and the average methane conversion,CO and H2 selectivity reached to 82.31%,82.41% and 87.64%,*** reason could be not only attributed to the fitting amount of NiO dispersed on the CeO2 surface and bulk but also to actual lattice oxygen amount increased in oxygen carrier.

关键词： ceria nickel oxygen carrier selective oxidation methane syngas solid solution rare earths

Evaluation of oxygen uncoupling characteristics of oxygen carrier using micro-fluidized bed thermogravimetric analysis

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Chinese Journal of Chemical Engineering 2021年第4期34卷 408-415页

作者： Lei Liu Zhenshan Li Ye Li Ningsheng Cai Key Laboratory for Thermal Science and Power Engineering of Ministry of Education Department of Energy and Power EngineeringTsinghua UniversityBeijing 100084China

oxygen uncoupling characteristics of a natural manganese ore and a perovskitetype oxide CaMn_(0.5)Ti0_(37)5Fe_(0.125)O_(3)were studied by using a microfluidized bed thermogravimetric analysis(MFBTGA)technology which is based on a realtime mass measurement of fluidizing particles inside a bubbling bed *** chemical stability,kinetics of the oxygen release and uptake reactions and fluidization property were investigated and the experimental data measured by MFBTGA were compared with the results in a regular TGA instrument(TGA Q500).The regular TGA Q500 results show the reactivity of both the manganese ore and perovskite oxide are stable for multi cycles,and the oxygen uncoupling capacity of the manganese ore is~1.2%(mass)which is~2 times higher than that of the perovskite ***,the experimental results from the MFBTGA indicated that there is a serious agglomeration for the manganese ore.A very important finding is that the reaction rate of oxygen release and oxygen uptake of the perovskite oxide measured by the MFBTGA are~2 and~4 times faster than that of testedby the TGA *** can conclude that MFBTGA is a very useful tool to measure the reactivity stability and kinetics of oxygen carriers in highthroughput analysis instead of the regular TGA.

关键词： CO_(2)capture oxygen carrier oxygen uncoupling Fluidized-bed Thermogravimetric analysis Agglomeration

New Insight into the Development of oxygen carrier Materials for Chemical Looping Systems

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Engineering 2018年第3期4卷 343-351页

作者： Zhuo Cheng Lang Qin Jonathan A. Fan Liang-Shih Fan William G. Lowrie Department of Chemical and Biomolecular Engineering The Ohio State University Columbus OH 43210 USA Department of Electrical Engineering Ginzton Laboratory Stanford University Stanford CA 94305 USA

Chemical looping combustion （CLC） and chemical looping reforming （CLR） are innovative technologies for clean and efficient hydrocarbon conversion into power, fuels, and chemicals through cyclic redox reac- tions. Metal oxide materials play an essential role in the chemical looping redox processes. During reduc- tion, the oxygen carriers donate the required amount of oxygen ions for hydrocarbon conversion and product synthesis. In the oxidation step, the depleted metal oxide oxygen carriers are replenished with molecular oxygen from the air while heat is released. In recent years, there have been significant advances in oxygen carrier materials for various chemical looping applications. Among these metal oxide materials, iron-based oxygen carriers are attractive due to their high oxygen-carrying capacity, cost ben- efits, and versatility in applications for chemical looping reactions. Their reactivity can also be enhanced via structural design and modification. This review discusses recent advances in the development of oxy- gen carrier materials and the mechanisms of hydrocarbon conversion over these materials. These advances will facilitate the development of oxygen carrier materials for more efficient chemical looping technology applications.

关键词： Chemical looping oxygen carrier Hydrocarbon conversion Ionic diffusion Mechanism

Chemical-Looping Reforming of Methane Using Iron Based oxygen carrier Modified with Low Content Nickel

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中国化学:英文版 2014年第12期32卷 1271-1280页

作者： Guoqiang Wei Fang He Zhen Huang Kun Zhao Anqing Zheng Haibin Li CAS Key Laboratory of Renewable Energy Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhouGuangdong 510640China

Fe_(2)O_(3)/Al_(2)O_(3) and Fe_(2)O_(3)/Al_(2)O_(3) modified by low content of Ni(below 2%in weight)oxygen carriers were prepared by mechanical mixing and impregnation *** synthesized oxygen carriers were characterized by means of X-ray diffraction(XRD),X-ray fluorescence(XRF),scanning electron microscopy(SEM),BET-surface area and temperature programmed reduction(TPR).Besides,redox cyclic reactivity and the performance of chemical looping reforming of methane of the oxygen carriers were studied in a thermal gravimetrical analysis(TGA)and fixed bed at 850℃.It was observed that the redox reactivity of the oxygen carriers is improved by Ni addition because synergic effect may occur between NiO and Fe_(2)O_(3)/Al_(2)O_(3) to form NiFe_(2)O_(4) and NiAl_(2)O_(4) spinel ***,the improvement was not apparent as Ni addition reached 1 wt%or more because more nickel loaded resulted in methane decomposition into H2 and carbon leading to carbon *** SEM and BET analysis showed that NiFe_(2)O_(4) and NiAl_(2)O_(4) particles dispersed into the pores of the Fe_(2)O_(3)/Al_(2)O_(3) particles in the course of *** addition,the resistance to sintering of the modified samples increased with the Ni addition *** results of successive redox cycles showed that the Ni modified Fe_(2)O_(3)/Al_(2)O_(3) oxygen carriers have good *** integration of reactivity and carbon deposition,the content 1.04 wt%of nickel doping was an optimal amount in the three modified samples.

关键词： methane chemical-looping reforming chemical-looping reforming oxygen carrier iron low content nickel

Waste pulp chemical-looping gasification using Ni-modified electroplating sludge as an oxygen carrier

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Carbon Resources Conversion 2023年第2期6卷 106-115页

作者： Genyang Tang Jing Gu Guoqiang Wei Haoran Yuan Yong Chen Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640China Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou) Guangzhou 511458China University of Chinese Academy of Sciences Beijing 100049China

Waste pulp(WP)is a typical byproduct of paper industry,and Chemical-looping gasification(CLG)as a recently developed technology is highly suited to dispose high-volatile wastes like *** order to make a high-efficiency oxygen carrier(OC)for CLG of WP,the Ni-containing electroplating sludge(NES)was used as the matrix and NiO modification was performed to enhance the hydrogen production in *** resulted in a potentially high-efficiency OC denoted as *** CLG of WP was in a fixed-bed reactor at 850℃by adopting NNES as the OC,injecting 2.4 mL/g(WP)water,and keeping a mass ratio of 1.0 between OC to *** produced 1.73 Nm^(3)/kg syngas that has an LHV of 11.9 MJ/Nm^(3)and a H_(2)/CO ratio of *** 10 redox cycles,the syngas yield did not have obvious decrease,but a certain reduction in the activity of NNES was *** of the spent NNES revealed that it is the Ni agglomeration and inert silicate generation which reduced the activity of NNES.

关键词： Solid waste CLG Waste pulp Electroplating sludge oxygen carrier