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Solar chemical looping reforming of methane combined with isothermal H2O/CO2 splitting using ceria oxygen carrier for syngas production

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Journal of Energy Chemistry 2020年第2期29卷 60-72页

作者： Srirat Chuayboon stéphane abanades Sylvain Rodat Processes Materials and Solar Energy LaboratoryPROMES-CNRSFont-Romeu 66120France Department of Mechanical Engineering King Mongkut's Institute of Technology LadkrabangPrince of Chumphon CampusChumphon 86160Thailand Universite Grenoble Alpes Le-Bourget-du-Lac F-73375France CEA-LJTEN Laboratoire des Systemes Solaires Haute Temperature(LSHT) Grenoble F-38054France

The chemical looping reforming of methane through the nonstoichiometric ceria redox cycle(CeO2/CeO2-δ) has been experimentally investigated in a directly irradiated solar reactor to convert both solar energy and methane to syngas in the temperature range 900–1050 °C. Experiments were carried out with different ceria shapes via two-step redox cycling composed of endothermic partial reduction of ceria with methane and complete exothermic re-oxidation of reduced ceria with H2 O/CO2 at the same operating temperature, thereby demonstrating the capability to operate the cycle isothermally. A parametric study considering different ceria macrostructure variants(ceria packed powder, ceria packed powder mixed with inert Al2 O3 particles, and ceria reticulated porous foam) and operating parameters(methane flow-rate, reduction temperature, or sintering temperature) was conducted in order to unravel their impact on the bed-averaged oxygen non-stoichiometry(δ), syngas yield, methane conversion, and solar reactor performance. The ceria cycling stability was also experimentally investigated to demonstrate repeatable syngas production by alternating the flow between CH4 and H2 O(or CO2). A decrease in sintering temperature of the ceria foam was beneficial for increasing syngas selectivity, methane conversion,and reactor performance. Increasing both CH4 concentration and reduction temperature enhanced δ with the maximum value up to 0.41 but concomitantly favored CH4 cracking reaction. The ceria reticulated porous foam showed better performance in terms of effective heat transfer, due to volumetric absorption of concentrated solar radiation and uniform heating with lower solar power consumption, thereby promoting the solar-to-fuel energy conversion efficiency that reached up to 5.60%. The energy upgrade factor achieved during cycle was up to 1.19. stable patterns in the δ and syngas yield for consecutive cycles with the ceria foam validated material performance stability.

关键词： Chemical looping Methane reforming Ceria structure Concentrated solar power Syngas production H2O/CO2 splitting

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Natural gas pyrolysis in double-walled reactor tubes using thermal plasma or concentrated solar radiation as external heating source

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Journal of Natural Gas Chemistry 2009年第1期18卷 1-8页

作者： stphane abanades stefania Tescari Sylvain Rodat Gilles Flamant Processes Materials and Solar Energy Laboratory (PROMES-CNRS) 7 Rue du Four Solaire 66120 Font-Romeu France

The thermal pyrolysis of natural gas as a clean hydrogen production route is examined. The concept of a double-walled reactor tube is proposed and implemented. Preliminary experiments using an external plasma heating source are carried out to validate this concept. The results point out the efficient CH4 dissociation above 1850 K （CH4 conversion over 90%） and the key influence of the gas residence time. Simulations are performed to predict the conversion rate of CH4 at the reactor outlet, and are consistent with experimental tendencies. A solar reactor prototype featuring four independent double-walled tubes is then developed. The heat in high temperature process required for the endothermic reaction of natural gas pyrolysis is supplied by concentrated solar energy. The tubes are heated uniformly by radiation using the blackbody effect of a cavity-receiver absorbing the concentrated solar irradiation through a quartz window. The gas composition at the reactor outlet, the chemical conversion of CH4, and the yield to H2 are determined with respect to reaction temperature, inlet gas flow-rates, and feed gas composition. The longer the gas residence time, the higher the CH4 conversion and H2 yield, whereas the lower the amount of acetylene. A CH4 conversion of 99% and H2 yield of about 85% are measured at 1880 K with 30% CH4 in the feed gas （6 L/min injected and residence time of 18 ms）, A temperature increase from 1870 K to 1970 K does not improve the H2 yield.

关键词： methane hydrogen thermal cracking plasma concentrated solar energy tubular reactor

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Improving photoreduction of CO2 with water to CH4 in a novel concentrated solar reactor

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Journal of Energy Chemistry 2017年第4期26卷 743-749页

作者： Sisi Han Yinfei Chen stéphane abanades Zekai Zhang Department of Energy Chemical Engineering College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014ZhejiangChina Processes Materialsand Solar Energy LaboratoryPROMES-CNRS(UPR 8521)7 Rue du Four Solaire66120 Font-RomeuFrance

COphotoreduction is an attractive process which allows the storage of solar energy and synthesis of solar fuels. Many different photocatalytic systems have been developed, while the alternative photo-reactors are still insufficiently investigated. In this work, photoreduction of COwith HO into CHwas investigated in a modified concentrating solar reactor, using TiOand Pt/TiOas the catalysts. The TiOand Pt/TiOsamples were extensively characterized by different techniques including powder X-ray diffraction（XRD）, Nadsorption/desorption and UV–vis absorption. The catalytic performance of the TiOand Pt/TiOsamples in the gas phase was evaluated under unconcentrated and concentrated Xe-lamp light and nature solar light with different concentrating ratios. Various parameters of the reaction system and the catalysts were investigated and optimized to maximize the catalytic performance of COreduction system. Compared with the normal light irradiation, the TiOand Pt/TiOsamples show higher photocatalytic activity（about 6–7 times） for reducing COinto CHunder concentrated Xe-lamp light and nature solar light. In the range of experimental light intensity, it is found that the concentration of the light makes it suitable for the catalytic reaction, and increases the utilization efficiency of the TiOand Pt/TiOsamples while does not decrease the quantum efficiency.

关键词： CO2 photoreduction CH4 Concentrating solar reactor Concentrating ratio

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研究流化床内废物焚烧过程中重金属挥发特性的反模型化方法

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环境科学学报 2004年第2期24卷 177-184页

作者：陆继东张步庭黄来沈凯 Gilles Flamant Daniel Gauthier stéphane abanades 华中科技大学煤燃烧国家重点实验室武汉430074 CNRS-IMP BP 5 Odeillo

用反模型化方法研究在流化床焚烧模拟废物过程中重金属 (HM)释放的动力学特性 .该方法包含了出口气体中的HM浓度变化规律 (实验数据 )和一个反应器尺度的模型 .在实验尺度的流化床焚烧反应器内对掺混了金属的模拟废物进行了热处理 ,对... 详细信息

用反模型化方法研究在流化床焚烧模拟废物过程中重金属 (HM)释放的动力学特性 .该方法包含了出口气体中的HM浓度变化规律 (实验数据 )和一个反应器尺度的模型 .在实验尺度的流化床焚烧反应器内对掺混了金属的模拟废物进行了热处理 ,对一种从废物中得到的并掺混有重金属 (Cd ,Pb和Zn)的物质进行了焚烧处理 ,用来模拟城市固体废弃物焚烧过程中的HM释放过程 .在反应器的气体出口安装了在线分析系统 ,该在线分析系统通过用ICP OES连续测量出口气体中的HM相对浓度变化规律能够全面的跟踪金属的挥发过程 .此外 ,还运用并发展了鼓泡床模型 ,应用此模型根据出口气体中的HM浓度和时间关系计算出HM挥发率 .利用反模型化方法可以通过在线分析的结果确定出颗粒尺寸的HM挥发动力学特性 .

关键词：流化床重金属反模型化方法城市固体废弃物动力学反应器大气污染

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Volatilization of heavy metals during incineration of municipal solid wastes

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Journal of Environmental Sciences 2004年第4期16卷 635-639页

作者： SUNLu-shi S.abanades J.D.Lu G.Flamant D.Gauthier stateKeylaboratoryofCoalCombustion HuazhongUniversityofScienceandTechnologyWuhan430074China InstitutdeScienceetdeG6niedesMat6riauxetProc6d6s（CNRS-IMP） BP50deillo66125Font-RomeuCedexFrance

Incineration experiments with MSW, which had been impregnated with heavy metals, were presented to obtain information on the volatilization behavior of the elements cadmium(Cd), lead(Pb), and zinc(Zn) under different conditions. Experiments were carried out in a bubbling fluid bed system connected to a customized inductively coupled plasma optical emission spectroscopy(ICP-OES) for analyzing metals in the flue gas. The results indicated that the combustion temperature, the gas atmosphere, and the chlorine content in the flue gas could affect the volatilization behavior of heavy metals. In the fluidized bed combustion, a large surface area was provided by the bed sand particles, and they may act as absorbents for the gaseous ash-forming compound. Comparer with the metals Cd and Pb, the vaporization of Zn was low. The formation of stable compounds such as ZnO·Al 2O 3 could greatly decrease the metals volatilization. The presence of chlorine would enhance the volatilization of heavy metals by increasing the formation of metal chlorides. However, when the oxygen content was high, the chlorinating reaction was kinetically hindered, which heavy metals release would be delayed.

关键词： municipal solid waste incineration heavy metal emission fluidized bed

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流化床内重金属蒸发特性的动力学模型

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工程热物理学报 2009年第2期30卷 347-349页

作者：刘晶 D Gauthier S abanades G Flamant 郑楚光华中科技大学煤燃烧国家重点实验室 CNRS-PROMES BP 5 Odeillo 66125 Font-Romeu France

在流化床内煤燃烧烟气中重金属浓度的实时监测基础上,发展动力学模型来研究重金属蒸发释放的动力学特性。该方法包括出口烟气中的重金属浓度变化的实验数据和一个反应器尺度的模型。在反应器的气体出口安装了在线分析系统,该在线分析系... 详细信息

在流化床内煤燃烧烟气中重金属浓度的实时监测基础上,发展动力学模型来研究重金属蒸发释放的动力学特性。该方法包括出口烟气中的重金属浓度变化的实验数据和一个反应器尺度的模型。在反应器的气体出口安装了在线分析系统,该在线分析系统可连续测量烟气中的重金属浓度变化规律。将烟气重金属在线分析的实验结果作为模型的输入参数,根据重金属的蒸发率和固体颗粒中重金属浓度的关系得到其蒸发的动力学规律,对于煤得到2级反应动力学规律。

关键词：重金属煤流化床烟气蒸发

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基于烟气重金属浓度在线监测的流化床蒸发动力学模型

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中国电机工程学报 2008年第11期28卷 1-5页

作者：刘晶 S.abanades D.Gauthier G.Flamant 郑楚光煤燃烧国家重点实验室(华中科技大学) 湖北省武汉市430074 CNRS-PROMES BP 50deilloFont-Romeu 66125France

应用改进的电感耦合等离子体发射光谱仪对烟气中重金属的相对浓度进行在线测量,以全面跟踪重金属的释放过程。在烟气重金属浓度实时监测基础上,发展动力学模型来研究重金属蒸发释放的动力学特性。应用矿物质基体氧化铝的实验结果来验证... 详细信息

应用改进的电感耦合等离子体发射光谱仪对烟气中重金属的相对浓度进行在线测量,以全面跟踪重金属的释放过程。在烟气重金属浓度实时监测基础上,发展动力学模型来研究重金属蒸发释放的动力学特性。应用矿物质基体氧化铝的实验结果来验证数学模型的有效性,理论模拟值与实验结果吻合较好。结果表明应用模型,将烟气重金属在线分析的实验结果作为输入参数,可用于预测重金属的蒸发率。根据重金属的蒸发率和固体颗粒中重金属浓度的关系得到其蒸发的动力学规律,对于氧化铝得到1级反应动力学规律。

关键词：重金属蒸发动力学模拟烟气流化床

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烟气中重金属浓度的在线测量

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化工学报 2006年第9期57卷 2185-2188页

作者：刘晶郑楚光陆继东 S.abanades D.Gauthier G.Flamant 华中科技大学煤燃烧国家重点实验室 CNRS-PROMES BP5 Odeillo66125 Font-RomeuFrance

An inductively coupled plasma atomic emission spectrometer （ICP-AES） was developed to continuously measure the heavy metals concentrations in flue gas in order to track the metal release *** system is devoted to the thermal treatment of metal-spiked mineral matrix, coal and municipal solid wastes in fluidized bed （850℃）.This method was used to study the kinetics of heavy metals *** optimum values of the gas flows from the 1200 W power generator were 0.1 L·min -1 for the sample gas and 0.2 L·min -1 for *** the thermal treatment of coal and municipal solid waste,Cd and Pb were released readily,while Zn was released at a lower level than Cd and *** formation of stable compounds such as ZnO·Al2O3 and CdO·Al2O3 from the reaction of heavy metals with fly ash particles could decrease heavy metals *** all cases, the experimental setup was successfully used to monitor the heavy metal release process during coal and solid waste thermal treatment.

关键词：在线测量重金属烟气流化床

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城市垃圾焚烧过程中重金属释放行为的试验研究

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燃烧科学与技术 2003年第6期9卷 516-520页

作者：孙路石陆继东张娟 abanades S Flamant G Gauthier D 华中科技大学煤燃烧国家重点实验室武汉430074 法国国家科学研究中心材料过程研究所

以城市垃圾为研究对象,在流化床试验装置上进行焚烧试验,并采用电感耦合等离子体发射光谱仪在线测量烟气中的重金属浓度,研究不同气氛条件(空气、混合气和氮气)下Cd、Pb及Zn3种重金属的释放特性.试验发现,城市垃圾焚烧过程中,在还原气氛... 详细信息

以城市垃圾为研究对象,在流化床试验装置上进行焚烧试验,并采用电感耦合等离子体发射光谱仪在线测量烟气中的重金属浓度,研究不同气氛条件(空气、混合气和氮气)下Cd、Pb及Zn3种重金属的释放特性.试验发现,城市垃圾焚烧过程中,在还原气氛及HCl存在的情况下,Cd及Pb较易挥发释放,而Zn释放程度较低,且基本不受气氛条件的影响.研究结果对揭示城市垃圾流化床焚烧过程中重金属释放行为有一定的意义.

关键词：城市垃圾焚烧重金属释放流化床

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