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Effect of reduction pretreatment on the structure and catalytic performance of Ir-In_(2)O_(3)catalysts for CO_(2) hydrogenation to methanol

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Journal of Environmental Sciences 2024年第6期140卷 2-11页

作者： Changyu Ding Feifei Yang Xue Ye Chongya Yang Xiaoyan Liu yuanlong tan Zheng Shen Hongmin Duan Xiong Su Yanqiang Huang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

In_(2)O_(3)has been found a promising application in CO_(2)hydrogenation to methanol,which is beneficial to the utilization of CO_(2).The oxygen vacancy(O_(v))site is identified as the catalytic active center of this ***,there remains a great challenge to understand the relations between the state of oxygen species in In_(2)O_(3)and the catalytic performance for CO_(2)hydrogenation to *** the present work,we compare the properties of multiple In_(2)O_(3)and Ir-promoted In_(2)O_(3)(Ir-In_(2)O_(3))catalysts with different Ir loadings and after being pretreated under different reduction *** CO_(2)conversion rate of Ir-In_(2)O_(3)is more promoted than that of pure In_(2)O_(3).With only a small amount of Ir loading,the highly dispersed Ir species on In_(2)O_(3)increase the concentration of O_(v)sites and enhance the *** finely tuning the catalyst structure,Ir-In_(2)O_(3)with an Ir loading of 0.16 wt.%and pre-reduction treatment under 300℃exhibits the highest methanol yield of 146 mgCH_(3)OH/(gcat·hr).Characterizations of Raman,electron paramagnetic resonance,X-ray photoelectron spectroscopy,CO_(2)-temperature programmed desorption and CO_(2)-pulse adsorption for the catalysts confirm that more O_(v)sites can be generated under higher reduction temperature,which will induce a facile CO_(2)adsorption and desorption *** performance for methanol production requires an adequate dynamic balance among the surface oxygen atoms and vacancies,which guides us to find more suitable conditions for catalyst pretreatment and reaction.

关键词： Carbon dioxide Hydrogenation Methanol In_(2)O_(3) Fixed-bed Reduction temperature

An Improved Method for Approximating the Infinite-Horizon Value Function of the Discrete-Time Switched LQR Problem

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Journal of Systems Science & Complexity 2024年第1期37卷 22-39页

作者： HOU tan LI yuanlong LIN Zongli Department of Automation Shanghai Jiao Tong UniversityShanghai 200240China Key Laboratory of System Control and Information Processing Ministry of Education of ChinaShanghai 200240China Shanghai Engineering Research Center of Intelligent Control and Management Shanghai 200240China Charles L.Brown Department of Electrical and Computer Engineering University of VirginiaCharlottesvilleVA 22904-4743USA

This paper considers the problem of approximating the infinite-horizon value function of the discrete-time switched LQR *** particular,the authors propose a new value iteration method to generate a sequence of monotonically decreasing functions that converges exponentially to the value *** method facilitates us to use coarse approximations resulting from faster but less accurate algorithms for further value iteration,and thus,the proposed approach is capable of achieving a better approximation for a given computation time compared with the existing *** numerical examples are presented in this paper to illustrate the effectiveness of the proposed method.

关键词： Optimal control switched linear systems switched LQR problem.

SnCl_(2)促进的Pt1/PS-PPh_(2)催化剂高选择性催化高碳烯烃氢甲酰化反应

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Chinese Journal of Catalysis 2024年第5期60卷 316-326页

作者：虞周楠张磊磊谈源龙井日峥曹宏晨楼才溢格日乐王军虎王爱琴张涛中国科学院大连化学物理研究所中国科学院应用催化科学技术重点实验室辽宁大连116023 中国科学院大学北京100049 中国科学院大连化学物理研究所低碳催化技术国家工程研究中心辽宁大连116023 中国科学院大连化学物理研究所穆斯堡尔谱数据中心辽宁大连116023

氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)_(4),HCo(CO)_(3)(PR_(3))和HRh(CO)(PPh_(3))_(2)等配合物作为催化剂.尽管Co基催化剂可以... 详细信息

氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)_(4),HCo(CO)_(3)(PR_(3))和HRh(CO)(PPh_(3))_(2)等配合物作为催化剂.尽管Co基催化剂可以将高碳烯烃、内烯烃以及支链烯烃高选择性地转化为直链醛,但其反应条件(5-30 MPa,140-200℃)较苛刻,且容易发生烯烃加氢等副反应.相比之下,Rh催化剂的活性比Co基催化剂高1-2个数量级,且反应条件较为温和.但Rh储量稀少,价格昂贵,而且对于高碳烯烃氢甲酰化反应,Rh催化剂难以分离和循环使用.因此,研究者开展了其他金属催化剂的研究,其中Pt-Sn催化剂因其出色的区域选择性而备受关注.但目前Pt-Sn催化剂多局限于均相催化体系,而且Sn助剂的作用尚不明确.本文采用商业化三苯基膦嫁接的聚苯乙烯小球为载体,通过浸渍法制备了SnCl_(2)-Pt_(1)/PS-PPh_(2)单原子催化剂,考察了其在长链-烯烃氢甲酰化反应中的催化性能,并研究了Sn的促进作用.首先,以1-己烯氢甲酰化为探针反应,对催化剂的组成以及反应条件进行了优化.当Pt/P/Sn=1/2/5时,催化剂表现出最高的催化活性,在90-120℃和4-6 MPa合成气条件下,催化剂转化频率(TOF)为40 h^(-1),产物醛的正异比>42.随后,考察了催化剂的底物适用性.结果表明,C6-C12的高碳烯烃均可被高选择性地转化为相应的醛(正异比>20).然而,在循环使用实验中,由于SnCl_(2)不能稳定锚定在载体上,第二次循环时催化活性降低.但通过补加SnCl_(2),催化活性可以完全恢复.高压热过滤实验及元素检测结果表明,反应过程中Pt没有流失.X射线吸收光谱(XAFS)表征结果表明,反应后Pt仍以单原子形式存在,说明Pt1/PS-PPh_(2)具有良好的稳定性.通过准原位X-射线吸收谱、Mössbauer谱和红外光谱表征对反应过程中Pt和Sn的电子性质和配位结构进行了研究.结果表明,SnCl_(2)在反应过程中逐渐转化为Sn(dioxane)Cl3-物种(1,4-二氧六环为反应溶剂),并与Pt原子形成Pt-Sn键.当反应体系中没有Sn时,Pt(II)会被合成气过度还原并发生团聚.当没有膦配体时,Pt原子也会发生聚集,而且SnCl_(2)会在Pt(II)的催化作用下发生水解生成SnO.因此Sn(dioxane)Cl3-与膦配体共同抑制了Pt(I)在反应过程中的还原与聚集.最后,通过XAFS表征深入研究了反应机理.分析结果表明,CO在催化剂上具有较强的吸附作用,而H_(2)则可能以异裂的方式在催化剂上被活化.据此提出可能的反应机理:首先,H_(2)在催化剂上活化先形成Pt-H物种;随后,烯烃插入Pt-H,形成Pt-烷基物种;接着,CO迁移并插入,生成Pt-酰基物种;最后,经过还原消除步骤,得到最终的产物醛.综上,本文制备了一种对高碳烯烃氢甲酰化反应具有良好催化性能的SnCl_(2)-Pt1/PS-PPh_(2)单原子催化剂,为低成本非Rh基催化剂的开发提供借鉴.同时,揭示了催化体系中Sn的促进作用,为通过Lewis酸来调控催化剂的性能提供了参考.

关键词：氢甲酰化反应铂-锡催化剂高碳烯烃区域选择性单原子催化剂

Scission of C–O and C–C linkages in lignin over RuRe alloy catalyst

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Journal of Energy Chemistry 2022年第4期31卷 492-499页

作者： Xinxin Li Yangming Ding Xiaoli Pan Yanan Xing Bo Zhang Xiaoyan Liu yuanlong tan Hua Wang Changzhi Li CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Science Beijing 100049China

The performance of lignin depolymerization is basically determined by the interunit C–O and C–C *** C–O bond cleavage strategies have been developed, while the cleavage of C–C bond between the primary aromatic units remains a challenging task due to the high dissociation energy of C–C ***, a multifunctional Ru Re alloy catalyst was designed, which exhibited exceptional catalytic activity for the cleavage of both C–O and C–C linkages in a broad range of lignin model compounds(β-1, a-5, 5–5,β-O-4, 4-O-5) and two stubborn lignins(kraft lignin and alkaline lignin), affording 97.5% overall yield of monocyclic compounds from model compounds and up to 129% of the maximum theoretical yield of monocyclic products based on C–O bonds cleavage from realistic lignin. Scanning transmission electron microscopy(STEM) characterization showed that Ru Re(1:1) alloy particles with hexagonal close-packed structure were homogeneously dispersed on the support. Quasi-in situ X-ray photoelectron spectroscopy(XPS), and X-ray absorption spectroscopy(XAS) indicate that Ru species were predominantly metallic state, whereas Re species were partially oxidized;meanwhile, there was a strong interaction between Ru and Re, where the electron transfer from Re to Ru was occurred, resulting in great improvement on the capability of C–O and C–C bonds cleavage in lignin conversion.

关键词： C–C bonds Ru Re alloy catalyst Lignin depolymerization

氧化还原驱动的高活性Pd/PdO表面界面促进低温甲烷燃烧

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Chinese Journal of Catalysis 2024年第5期60卷 242-252页

作者：谈源龙张亚峰高雅马静远赵晗顾青青苏杨徐晓燕王爱琴杨冰张国旭刘晓艳张涛中国科学院大连化学物理研究所中国科学院航天催化材料重点实验室辽宁大连116023 中国科学院大学北京100049 哈尔滨工业大学化工与化学学院新能源转化与存储关键材料工业和信息化部重点实验室黑龙江哈尔滨150001 中国科学院上海高等研究院上海同步辐射光源上海201204 中国科学院大连化学物理研究所中国科学院洁净能源创新研究院辽宁大连116023 中国科学院大连化学物理研究所催化基础国家重点实验室辽宁大连116023

天然气汽车尾气中尚未充分燃烧的甲烷是一种典型的温室气体之一,其温室效应远超二氧化碳,达到后者的20倍以上.因此,减少甲烷的排放对于有效应对气候变化至关重要.目前,以Pd/Al_(2)O_(3)为基础催化剂的催化燃烧反应,已被证实为减少甲烷... 详细信息

天然气汽车尾气中尚未充分燃烧的甲烷是一种典型的温室气体之一,其温室效应远超二氧化碳,达到后者的20倍以上.因此,减少甲烷的排放对于有效应对气候变化至关重要.目前,以Pd/Al_(2)O_(3)为基础催化剂的催化燃烧反应,已被证实为减少甲烷排放的最为切实可行的技术手段.深入了解钯基催化剂的活性结构不仅有助于合理设计高效的催化体系,还能在很大程度上减少贵金属钯的使用量.然而,在甲烷燃烧反应过程中,由于氧化还原气氛的复杂性,Pd金属的表面容易转变为不同结构,这增加了研究其活性结构的难度.此外,催化剂的制备方法、载体的性质、预处理的气氛以及温度等因素均会对Pd的价态和粒径效应产生影响,使得Pd基催化剂在甲烷燃烧反应中的活性结构至今仍存在争议.为了深入研究这一问题,本文选用商业化的纳米级γ-Al_(2)O_(3)作为载体,采用易于工业化应用的浸渍法制备了Pd/Al_(2)O_(3)催化剂,并研究其在低温(200-400℃)贫燃条件下的活性结构.球差电镜结果表明,催化剂中的Pd纳米颗粒在不同气氛中经800℃高温预处理后呈现出不同的结构特点.氦气处理后的催化剂中,Pd以完全金属态的形式存在;氧气处理后的催化剂中,Pd以PdO的形式存在;甲烷燃烧反应气处理后的催化剂中,PdO大颗粒上存在金属Pd小颗粒,呈现出“荔枝型”Pd/PdO结构.准原位X射线光电子能谱和原位X射线吸收谱等结果表明,“荔枝型”Pd/PdO结构是在甲烷燃烧反应中受氧化还原气氛诱导形成的.该独特的“荔枝型”Pd/PdO结构的催化剂在300℃甲烷燃烧反应中,表现出337.8μmol gPd^(-1) s^(-1)的反应速率,分别是纯金属Pd和PdO型催化剂反应速率的10.7倍和15.5倍.进一步研究表明,无论催化剂中Pd的初始状态为金属态或是氧化态,高活性的“荔枝型”Pd/PdO结构都可以在较低温度(500℃)的长时间(12 h)甲烷燃烧反应中缓慢生成.通过调节预处理气氛中甲烷与氧气的相对浓度,可以实现689.2μmol gPd-1 s^(-1)的反应速率,高于文献已报道的Pd基催化剂在相似反应条件下的活性.密度泛函理论计算结果表明,相对于金属Pd和PdO,甲烷在Pd/PdO界面处表现出最低(0.40 eV)的自由能势垒,这表明由于界面处金属Pd和PdO的协同作用,甲烷断裂第一个C-H键的解离活化过程更容易发生,从而解释了“荔枝型”Pd/PdO结构高催化活性的来源.综上,本文通过先进的球差电镜和原位光谱表征技术,为深入认识甲烷燃烧钯基催化剂活性结构提供了新的角度.研究发现,反应过程中因气氛诱导而生成的高活性结构可能是重要的活性中心,这一观点不仅有助于理解甲烷燃烧反应的机理,而且可以为其他氧化还原催化体系的研究以及工业催化剂的设计制备提供参考.

关键词：原位表征纳米颗粒钯甲烷燃烧界面

Sub-nanometer Pt_(2)In_(3) intermetallics as ultra-stable catalyst for propane dehydrogenation

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能源化学:英文版 2023年第8期83卷 304-312,I0009页

作者： Yanan Xing Guiyue Bi Xiaoli Pan Qike Jiang yuanlong tan Yang Su Leilei Kang Bonan Li Lin Li Aiqin Wang Jingyuan Ma Xiaofeng Yang Xiao Yan Liu Tao Zhang CAS Key Laboratory of Science and Technology on Applied Catalysis ichEMDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China

Pt-based catalysts are the typical industrial catalysts for propane dehydrogenation(PDH),which still suffer from insufficient lo ng-term durability due to the structu ral instability and coke deposition.A commercial γ-Al_(2)O_(3) supported thermally robust sub-nanometer Pt2In3intermetallic catalyst with atomically ordered structure and rigorously separated Pt single atoms was fabricated,which showed outstanding robustness in 240 h long-term operation at 600℃ with the deactivation rate constant kdas low as0.00078 h^(-1), ranking among the lowest reported *** on various in situ characterizations and theoretical calculations,it was proved that the catalyst stability not only resulted from the separated Pt single-atom sites but also significantly affected by the distance of adjacent Pt *** increasing distance to 3.25 A in the Pt_(2)In_(3)could induce a weak π-adsorption configuration of propylene on Pt sites,which facilitated the desorption of propylene and restrained the side reactions like coking.

关键词： Propane dehydrogenation Propylene Pt-In catalyst Intermetallic compounds Pt_(2)ln_(3)

Global practical stabilization of the double integrator system with an imperfect sensor and subject to a bounded disturbance

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Control Theory and Technology 2024年第3期22卷 468-478页

作者： Zhiyuan Zhu yuanlong Li Zongli Lin Department of Automation Shanghai Jiao Tong Universityand Key Laboratory of System Control and Information Processing of Ministry of EducationShanghai 200240China Charles L.Brown Department of Electrical and Computer Engineering University of VirginiaP.0.Box 400743CharlottesvilleVA 22904-4743USA

This paper is concerned with global practical stabilization of the double integrator system with an imperfect sensor and subject to an additive bounded output *** imperfect sensor nonlinearity possesses the nonlinear characteristics of saturation and dead *** of the presence of output dead zone and the additive disturbance,the states cannot be expected to driven into an arbitrarily small neighborhood of the *** solve the global practical stabilization problem,we proposes a low gain-based linear dynamic output feedback law,under which the first state enters and remains in a bounded set whose size is depended on the bound of disturbance and the range of dead zone and the second state enters and remains in a pre-specified arbitrarily small set,both in finite *** results illustrate the effectiveness of our proposed control method.

关键词： Output saturation Disturbance rejection Output dead zone Low gain feedback-Linear output feedback Practical stabilization

Design and performance investigation of modified dual reflector parabolic trough collector with double planar mirrors

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Science China(Technological Sciences) 2024年第3期67卷 902-918页

作者： LI Peijing LIU TaiXiu QIN yuanlong LI JiChao LIU QiBin School of Energy Powerand Mechanical EngineeringNorth China Electric Power University Beijing 226China Institute of Engineering Thermophysics Chinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Department of Thermal Science and Energy Engineering University of Science and Technology of ChinaHefei 230027China

In a typical parabolic trough collector(PTC), sunlight is concentrated at the bottom of the absorber tube. This concentrated solar flux leads to uneven heat distribution, resulting in high local temperatures and significant thermal stress on the absorber *** limitations have restricted the application of PTCs in solar thermochemistry and other fields and have impacted their safe operation. In this study, a new PTC with dual planar mirrors(DPMS) is proposed to homogenize the circumferential solar flux distribution of the absorber tube. A design method and single-objective optimization of the new PTC with a DPMS are proposed,and an uncertainty analysis of the operational and structural parameters is performed. A coupled light-heat-structure numerical model was developed to study the heat transfer performance and structural mechanical properties. The thermodynamic properties of the PTC with DPMS under different boundary conditions were analyzed. The results show that the circumferential temperature difference of the new PTC is within 2.6 K, and the circumferential thermal deformation is within 0.9 mm under typical working conditions(the inlet velocity of the heat transfer fluid is 3 m/s, inlet temperature is 573.15 K, and the direct normal irradiance is 1000 W/m^(2)). Compared with conventional PTCs, the circumferential temperature difference is reduced by 74%–90%, and the maximum thermal deformation along the y-axis is reduced by more than 95% under all working conditions(1–5 m/s, 373.5–675.15 K, 200–1000 W/m^(2)). The new PTC maintains the uniformity of the circumferential solar flux distribution for different operating parameters(sun incident angle of 0°–3°) and installation errors(±3 mm), is suitable for solar energy applications in various fields, and has the potential for large-scale applications.

关键词： solar thermal energy parabolic trough collector secondary reflector solar flux distribution optical optimization

Performance Enhancement of Parabolic Trough Collector by Using Homogenizer and Spiral

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Journal of Thermal Science 2024年第2期33卷 658-674页

作者： LI Peijing LIU Taixiu QIN yuanlong ZHENG Zhimei ZHAO Kai LIU Qibin School of Energy Powerand Mechanical EngineeringNorth China Electric Power UniversityBeijing102206China Institute of Engineering Thermophysics Chinese Academy of SciencesBeijing100190China University of Chinese Academy of Science Beijing100049China Department of Thermal Science and Energy Engineering University of Science and Technology of ChinaHefei230027China Research Institute of Science and Technology of China Three Gorges Group Corporation Beijing100038China

In conventional parabolic trough collectors(PTCs),sunlight is concentrated at the bottom of the absorber tube,resulting in a significant circumferential temperature gradient across the absorber tube,heat loss and thermal deformation,which affects the safety and thermal performance of *** this study,a new receiver with homogenizer and spiral(RHS) is proposed,achieving the optical and thermal synergy to ameliorate the thermal deformation of the absorber tube and enhance thermal efficiency.A plane structure homogenizer is designed to improve uniformity of the concentrated solar flux of absorber tube through second *** combination with the spiral,it improves the optical-thermal efficiency of the PTC by enhancing heat exchange between the fluid and the backlight side of the absorber *** performance of the collector is numerically studied by building a three-dimensional coupled light-thermal-structure *** results show that the thermal deformation of the RHS is reduced by more than 96% and the optical-thermal efficiency is improved by 1.2%-0.63% compared with conventional receivers(CRs) under the same inlet temperature *** proposed receiver is validated to be effective in reducing thermal deformation and improving optical-thermal efficiency.

关键词： parabolic trough collector homogenizer thermal deformation spiral