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Chinese Journal of Chemical Engineering 2023年第11期63卷 235-245页

作者： Chang Yang Juping Zhang Jiakai Wang Dongfang li kongzhai li Xing Zhu State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Faculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China

Redox catalysts play a vital role in the interconversion of two significant greenhouse gases,CO_(2)and CH_(4),via chemical looping methane dry reforming technology.Herein,a series of transition metals-alloyed and core-shell structured Ni-M/SiO_(2)@CeO_(2)(M=Fe,Co,Cu,Mn,Zr)redox catalyst were fabricated and evaluated in a gas-solid fixed-bed reactor for cycling CH_(4)partial oxidation(PO_(x))and CO_(2)splitting.The catalysts are composed of spherical SiO_(2)core and CeO_(2)shell,and the highly dispersed Ni alloy nanoparticles are the interlayer between core and shell.The oxygen vacancy concentration of Ni-M/SiO_(2)@CeO_(2)followed the order of Co>Cu>Fe>Mn>Zr,and Ni alloying with transition metals significantly enhanced oxygen storage capacity(OSC).Ni-Co/SiO_(2)@CeO_(2)catalyst with abundant oxygen vacancies and a high OSC showed the lowest temperatures of CH_(4)activation(610℃)and CO_(2)decomposition(590℃),thus demonstrating excellent redox reactivity.The catalyst exhibited superior activity and structural stability in the continuous CH_(4)/CO_(2)redox cycles at 615℃,achieving 87%CH_(4)conversion and 83%CO selectivity.The proposed catalyst shows great potential for the utilization of CH_(4)and CO_(2)in a redox mode,providing a new sight for design redox catalyst in chemical looping or related fields.

关键词： Chemical looping Methane Dry reforming Catalyst Partial Oxidation

Progress and key challenges in catalytic combustion of lean methane

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Journal of Energy Chemistry 2022年第12期75卷 173-215,I0005页

作者： Xiangbo Feng Lei Jiang Danyang li Shaopeng Tian Xing Zhu Hua Wang Chi He kongzhai li Xi’an Key Laboratory of Advanced Photoelectronics Materials and Energy Conversion Device School of ScienceXijing UniversityXi’an 710123ShaanxiChina State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Kunming University of Science and TechnologyKunming 650093YunnanChina Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi'an Jiaotong UniversityXi'an 710049ShaanxiChina National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China

As a primary type of clean energy,methane is also the second most important greenhouse gas after CO_(2)due to the high global warming potential.Large quantities of lean methane(0.1–1.0 vol%)are emitted into the atmosphere without any treatment during coal mine,oil,and natural gas production,thus leading to energy loss and greenhouse effect.In general,it is challenging to utilize lean methane due to its low concentration and flow instability,while catalytic combustion is a vital pathway to realize an efficient utilization of lean methane owing to the reduced emissions of polluting gases(e.g.,NOxand CO)during the reaction.In particular,to efficiently convert lean methane,it necessitates both the designs of highly active and stable heterogeneous catalysts that accelerate lean methane combustion at low temperatures and smart reactors that enable autothermal operation by optimizing heat management.In this review,we discuss the in-depth development,challenges,and prospects of catalytic lean methane combustion technology in various configurations,with particular emphasis on heat management from the point of view of material design combined with reactor configuration.The target is to describe a framework that can correlate the guiding principles among catalyst design,device innovation and system optimization,inspiring the development of groundbreaking combustion technology for the efficient utilization of lean methane.

关键词： Lean methane combustion Catalyst design Heat management Reactor optimization Catalytic mechanism

Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming

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Journal of Energy Chemistry 2022年第2期31卷 34-47页

作者： Wenming liu Le li Sixue lin Yiwei Luo Zhenghong Bao Yiru Mao kongzhai li Daishe Wu Honggen Peng College of Chemistry Key Laboratory of Poyang Lake Environment and Resource UtilizationMinistry of EducationSchool of Resources Environmental and Chemical EngineeringNanchang UniversityNanchang 330031JiangxiChina Chemical Sciences Divison Oak Ridge National LaboratoryOak RidgeTN 37830USA State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina

Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or hydrogen.The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts.Herein,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(In_(x)Ni@SiO_(2))have been prepared and displayed superior coking resistance for DRM reaction.The sample containing 0.5 wt.%of In loading(In_(0.5)Ni@SiO_(2))shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test.The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In.Both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane.The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases.

关键词： Methane dry reforming InNi intermetallic alloy Confinement Coking resistance Utilization of greenhouse gases

Suppressing byproduct formation for high selective CO_(2) reduction over optimized Ni/TiO_(2) based catalysts

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Journal of Energy Chemistry 2022年第9期31卷 465-478,I0013页

作者： Danyang li Ruidong Xu Roong Jien Wong Xing Zhu Dong Tian Lei Jiang Qingjie Guo Hongcun Bai linan Huang Wen liu Hua Wang kongzhai li Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction Ministry of EducationKunming University of Science and TechnologyKunming 650093YunnanChina School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021NingxiaChina Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina

One of the challenges for catalytic CO_(2)reduction is to control product selectivity,and new findings that can modify selectivity would be transformative.Herein,two kinds of TiO_(2)(homemade and commercial)with the same crystal phase but different surface properties are chosen as supports to prepare Ni-based catalysts for CO_(2)reduction,which show distinctly different product selectivity for CO_(2)reduction to CH_(4) or CO,as well as the CO_(2)conversion.The catalysts based on the homemade TiO_(2)support are highly selective for CH_(4) formation,while the latter ones are about 100%selective for CO formation under the same reaction conditions.In addition,the former ones are much active(more than 3 times)than the latter ones.We found that the collaborative contribution of Ti^(3+)and Ni^(2+)species and the electronic metal-support interactions effect maybe the main driving force behind for determining the product selectivity.Methane is almost exclusively produced over the catalysts with abundant Ti^(3+)and Ni^(2+)species and greater electronic metal-support interaction,otherwise,it will give priority to CO generation.The addition of CeO_(2)can reduce the Ni particle size and improve the dispersion of Ni nanoparticles,as well as create more Ti^(3+)species,contributing to the enhancement of CO_(2)conversion,but shows a negligible effect on product selectivity.Furthermore,the in situ DRIFT experiments and kinetic experiments indicate that the CO route is probably involved in the CO_(2)reduction process over the homemade Ni-CeO_(2)/TiO_(2)-CO catalyst with abundant Ti^(3+)and Ni^(2+)species and a strong electronic transform effect.

关键词： CO_(2)reduction Ni-based catalysts TiO_(2)support Product selectivity Surface and interface properties

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

Hydrogen production via chemical looping reforming of coke oven gas

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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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铜基载氧体的焦炉煤气化学链燃烧特性

洁净煤技术 2024年第2期30卷 244-256页

作者：范心瑜卢春强左慧琮李志强江磊李孔斋昆明理工大学冶金与能源工程学院云南昆明650093 冶金节能减排教育部工程研究中心云南昆明650093

焦炉煤气(COG)是炼焦过程产生的主要副产品,含有复杂的气体成分(CO、H_(2)、CH_(4)、CO_(2)),化学链燃烧是一种可实现COG高效转化与高纯CO_(2)捕集的技术。通过溶胶凝胶法制备了一系列x(%)CuO/Ce-Zr-O(x=30、50、70、90)载氧体用于COG... 详细信息

焦炉煤气(COG)是炼焦过程产生的主要副产品,含有复杂的气体成分(CO、H_(2)、CH_(4)、CO_(2)),化学链燃烧是一种可实现COG高效转化与高纯CO_(2)捕集的技术。通过溶胶凝胶法制备了一系列x(%)CuO/Ce-Zr-O(x=30、50、70、90)载氧体用于COG化学链燃烧反应特性研究。XRD表明,x(%)CuO/Ce-Zr-O载氧体物相由CuO和Ce_(0.67)Zr_(0.33)O_(2)固溶体组成。由于Zr^(4+)进入CeO_(2)晶格中,在617 cm^(-1)处出现明显的氧空位Raman特征峰。H_(2)-TPR、CO-TPR、CH_(4)-TPR和COG-TPR结果表明加入Ce-Zr-O固溶体促使铜物种低温释氧能力增强。800℃下,CuO样品CO_(2)捕集率为34%,添加10%Ce_(0.67)Zr_(0.33)O_(2)后CO_(2)捕集率增至100%。经50次氧化还原循环后,CuO样品性能大幅降低,而90CuO/Ce-Zr-O样品的反应性能和物相结构未发生明显变化,表明CuO和Ce_(0.67)Zr_(0.33)O_(2)之间的相互作用增强了铜物种的释氧能力和循环稳定性。此研究有助于拓宽COG利用途径。

关键词：焦炉煤气化学链燃烧循环反应性能 CO_(2)捕集

铁捕集铂族金属的熔渣调控及其捕集机理的理论计算研究

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昆明理工大学学报（自然科学版） 2024年第2期49卷 1-12页

作者：杨泉黄利南李勇江磊吴喜龙赵雨程显名李孔斋贵研资源(易门)有限公司云南玉溪651100 昆明理工大学冶金与能源学院云南昆明650093 昆明理工大学教育部冶金节能减排工程研究中心云南昆明650093

以汽车废催化剂为原料的铂族金属(PGMs)再生利用不仅缓解供需矛盾,而且还能保障国家战略储备金属需求,具有重大战略意义.汽车废催化剂成分复杂,火法捕集PGMs的过程需要进行大量的实验以获得最佳的熔渣,从而提高PGMs的回收率.通过FactSag... 详细信息

以汽车废催化剂为原料的铂族金属(PGMs)再生利用不仅缓解供需矛盾,而且还能保障国家战略储备金属需求,具有重大战略意义.汽车废催化剂成分复杂,火法捕集PGMs的过程需要进行大量的实验以获得最佳的熔渣,从而提高PGMs的回收率.通过FactSage的理论计算对炉渣反应平衡模拟以达到优化炉渣的目的.FactSage计算结果表明,当添加剂CaO、SiO_(2)、Na_(2)CO_(3)和CaF_(2)的添加量分别占汽车废催化剂质量分数的40%、15%、30%和5%时,熔渣的性质最佳,即渣相的完全温度为1 330℃,粘度为1.92 Pa·s.本工作还结合DFT计算对铁捕集汽车废催化剂中PGMs的机理进行了研究.在超过1 390℃的高温条件下,Rh以取代掺杂的类型和δ-Fe形成合金结构.在912~1 390℃的温度区间内,Pd以取代掺杂的方式和γ-Fe形成合金,并只有在该温度区间才能形成Pd-Fe合金.此外,在该温度区间下,大部分Pt被捕集并以取代掺杂的方式和γ-Fe形成合金.当温度低于912℃时,Rh和Pt再次被α-Fe捕集并形成合金.然而,γ-Fe-Pd合金随着温度降低,形成的α-Fe-Pd的合金结构是不稳定的,这就导致Pd会从Fe相中析出,降低Pd的捕集率.总之,本研究为火法捕集PGMs提供了一种高效的炉渣优化方法.

关键词：汽车废催化剂铂族金属回收铁捕集渣设计机理研究

Hydrogen and syngas production from two-step steam reforming of methane using CeO_2 as oxygen carrier

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Journal of Natural Gas Chemistry 2011年第3期20卷 281-286页

作者： Xing Zhu, Hua Wang YonggangWei kongzhai li Xianming Cheng Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction Ministry of Education Faculty of Metallurgical and Energy Engineering Kunming University of Science and Technology Kunming 650093 Yunnan China

CeO2 oxygen carrier was prepared by precipitation method and tested by two-step steam reforming of methane （SRM）. Two-step SRM for hydrogen and syngas generation is investigated in a fixed-bed reactor. Methane is directly converted to syngas at a H2/CO ratio close to 2 ： 1 at a high temperature （above 750 °C） by the lattice oxygen of CeO2; methane cracking is found when the reduction degree of CeO2 was above 5.0% at 850 °C in methane isothermal reaction. CeO2？δ obtained from methane isothermal reaction can split water to generate CO-free hydrogen and renew its lattice oxygen at 700 °C; simultaneously, deposited carbon is selectively oxidized to CO2 by steam following the reaction （C＋2H2O→CO2＋2H2）. Slight deactivation in terms of amounts of desired products （syngas and hydrogen） is observed in ten repetitive two-step SRM process due to the carbon deposition on CeO2 surface as well as sintering of CeO2.

关键词： two-step steam reforming of methane CeO2 hydrogen syngas redox cycle

Effect of Preparation Method on the Structural Characteristics of NiO-ZrO2 Oxygen Carriers for Chemical-looping Combustion

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Chemical Research in Chinese Universities 2019年第6期35卷 1024-1031页

作者： liU Yike LONG Yanhui TANG Yaqin GU Zhenhua li kongzhai School of Material and Metallurgical Engineering Guizhou Institute of TechnologyGuiyang 550003P.R.China Faculty of Metallurgical and Energy Engineering Kunming University of Science ami TechnologyKunming 650093P.R.China State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Kunming University of Science and TechnologyKunming 650093P.R.China Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction Ministry of EducationKunming University of Science and TechnologyKunming 650093P.R.China

Chemical-looping combustion(CLC)offers an effective approach for power generation and CO2 capture.In this work,an NiO-ZrO2 oxygen carrier prepared by three methods was subjected to an optimal reaction temperature test,an optimal flow test and a cyclic redox reaction test to explore the most suitable reaction conditions.Through comparative analysis,it is noted that the coprecipitation method is not suitable for the preparation of this NiO-ZrO2 oxygen carrier,while the oxygen carrier prepared by the mechanical mixing method and solution combustion method obtained a higher CH4 conversion rate and CO2 selectivity.In addition,these two oxygen carriers also showed high stability during successive CLC testing.Therefore,both the mechanical mixing method and the solution combustion method can be used to prepare NiO-ZrO2 oxygen carriers.

关键词： Chemicalooping combustion NiO-ZrO2 oxygen carrier Solution combustion method Mechanical mixing method Coprecipitation method