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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

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Nitrogen-doped hierarchically porous carbon spheres for low concentration CO_(2) capture

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Journal of Energy Chemistry 2021年第2期30卷 168-174,I0007页

作者： Yang Li Jing Wang Sisi Fan Fanan Wang Zheng Shen hongmin duan Jinming Xu Yanqiang Huang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China School of Ecological Environment and Urban Construction Fujian University of TechnologyFuzhou 350118FujianChina

Synthesis of spherical carbon beads with effective CO_2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO_2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO_2/N_2(0.5:99.5, v/v).

关键词： Carbon sphere CO_(2)capture Hierarchical porous materials Nitrogen-doped carbon Poly(vinylidene chloride)

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CO_2 methanation over TiO_2–Al_2O_3 binary oxides supported Ru catalysts

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Chinese Journal of Chemical Engineering 2016年第1期24卷 140-145页

作者： Jinghua Xu Qingquan Lin Xiong Su hongmin duan Haoran Geng Yanqiang Huang School of Materials Science and Engineering Shandong University State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences School of Chemistry and Chemical Engineering Yantai University Shandong Applied Research Center of Gold Nanotechnology (Au-SDARC)

TiO_2 modified Al_2O_3 binary oxide was prepared by a wet-impregnation method and used as the support for ruthenium catalyst. The catalytic performance of Ru/TiO_2–Al_2O_3catalyst in CO_2 methanation reaction was investigated. Compared with Ru/Al_2O_3 catalyst, the Ru/TiO_2–Al_2O_3catalytic system exhibited a much higher activity in CO_2 methanation reaction. The reaction rate over Ru/TiO_2–Al_2O_3 was 0.59 mol CO_2·(g Ru)1·h-1, 3.1 times higher than that on Ru/Al_2O_3[0.19 mol CO_2·(gRu)-1·h-1]. The effect of TiO_2 content and TiO_2–Al_2O_3calcination temperature on catalytic performance was addressed. The corresponding structures of each catalyst were characterized by means of H_2-TPR, XRD, and TEM. Results indicated that the averaged particle size of the Ru on TiO_2–Al_2O_3support is 2.8 nm, smaller than that on Al_2O_3 support of 4.3 nm. Therefore, we conclude that the improved activity over Ru/TiO_2–Al_2O_3catalyst is originated from the smaller particle size of ruthenium resulting from a strong interaction between Ru and the rutile-TiO_2 support, which hindered the aggregation of Ru nanoparticles.

关键词： CO2 methanation Supported Ru catalyst TiO2–Al2O3 binary oxide

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The influence of intimacy on the ’iterative reactions’ during OX-ZEO process for aromatic production

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Journal of Energy Chemistry 2019年第8期28卷 60-65,I0003页

作者： Xiaoli Yang Ting Sun Junguo Ma Xiong Su Ruifeng Wang Yaru Zhang hongmin duan Yanqiang Huang Tao Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China University of Chinese Academy of Sciences Beijing 100049China College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610068 Sichuan China

The oxide-zeolite process provides a promising way for one-step production of aromatics from syngas,whereas the reasons for the dramatic effect of intimacy between oxide and zeolite in the composite catalyst on the product selectivity are still unclear. In order to explore the optimal intimacy and the essential influence factors, ZnCrOxcombined with ZSM-5 are employed to prepare the composite catalysts with different distances between the two components by changing the mixing methods. An aromatic selectivity of 74%(with CO conversion to be 16%) is achieved by the composite catalyst when the intimacy is in the range of nanometer. A so-called ‘iterative reactions’ mechanism of intermediates over oxides is then proposed and studied: the intermediate chemical can undergo a hydrogenation reaction on *** the shorter the intermediates stay on oxide, the more of chance for C-C coupling takes place on zeolite to form aromatics. Moreover, the aero-environments of reaction is found to impact on the extent of iterative reaction as well. Therefore, when the intimacy between the two components changes, the extent of iterative reactions vary, resulting in alteration of product distribution. This work provides new insight in understanding the mechanisms during the complex process of OX-ZEO composite catalysis and sheds light to the design of a high-yield catalyst for synthetization of aromatics from syngas.

关键词： OX-ZEO process Intimacy Iterative reactions Reaction aero-environment Diffusion

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THE ROLE OF SURFACE SHELL OF THE YBa_(2)Cu_(3)O_(x) SINGLE CRYSTAL IN HIGH Tc SUPERCONDUCTIVITY

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Chinese Physics Letters 1988年第6期5卷 253-256页

作者： duan hongmin LU Li ZHANG Dianlin Institute of Physics Academia SinicaBeijing

We have measured the susceptibilities of the YBa_(2)Cu_(3)O_(x) single crystals,which were obtained by crushing the original ones to different *** susceptibility decreases rapidly as the size *** indicates that the su... 详细信息

关键词： SUPER

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Catalytic carbon dioxide hydrogenation to methane: A review of recent studies

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Journal of Energy Chemistry 2016年第4期25卷 553-565页

作者： Xiong Su Jinghua Xu Binglian Liang hongmin duan Baolin Hou Yanqiang Huang State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences Dalian Institute of Standardization

Recently, various efforts have been put forward on the development of technologies for the synthesis of methane from CO2 and H-2, since it can offer a solution for renewable H-2 storage and transportation. In parallel, this reaction is considered to be a critical step in reclaiming oxygen within a closed cycle. Over the years, extensive fundamental research works on CO2 methanation have been investigated and reported in the literatures. In this updated review, we present a comprehensive overview of recent publications during the last 3 years. Various aspects on this reaction system are described in detail, such as thermodynamic considerations, catalyst innovations, the influence of reaction conditions, overall catalytic performance, and reaction mechanism. Finally, the future development of CO2 methanation is discussed. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Methanation Carbon dioxide Hydrogenation Ni catalyst Ru catalyst

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Identification of relevant active sites and a mechanism study for reverse water gas shift reaction over Pt/CeO_2 catalysts

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Journal of Energy Chemistry 2016年第6期25卷 1051-1057页

作者： Xiaodong Chen Xiong Su Binglian Liang Xiaoli Yang Xinyi Ren hongmin duan Yanqiang Huang Tao Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

Reverse water gas shift (RWGS) reaction can serve as a pivotal stage in the CO2 conversion processes, which is vital for the utilization of CO2. In this study, RWGS reaction was performed over Pt/CeO2 catalysts at the temperature range of 200-500 degrees C under ambient pressure. Compared with pure CeO2, Pt/CeO2 catalysts exhibited superior RWGS activity at lower reaction temperature. Meanwhile, the calculated TOF and E-a values are approximately the same over these Pt/CeO2 catalysts pretreated under various calcination conditions, indicating that the RWGS reaction is not affected by the morphologies of anchored Pt nanoparticles or the primary crystallinity of CeO2. TPR and XPS results indicated that the incorporation of Pt promoted the reducibility of CeO2 support and remarkably increased the content of Ce 3 + sites on the catalyst surface. Furthermore, the CO TPSR-MS signal under the condition of pure CO2 flow over Pt/CeO 2 catalyst is far lower than that under the condition of adsorbed CO2 with H-2 -assisted flow, revealing that CO2 molecules adsorbed on Ce3+ active sites have difficult in generating CO directly. Meanwhile, the adsorbed CO2 with the assistance of H-2 can form formate species easily over Ce3+ active sites and then decompose into Ce3+-CO species for CO production, which was identified by in-situ FTIR. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B. V. and Science Press. All rights reserved.

关键词： RWGS reaction Pt/CeO2 catalyst Formate intermediate Mechanism

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反应条件对Co/SBA-15催化剂Fischer-Tropsch合成性能的影响

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石油化工 2008年第8期37卷 763-769页

作者：段洪敏徐恒泳中国科学院大连化学物理研究所辽宁大连116023

采用初湿浸渍法制备了 Co/SBA—15催化剂,采用 N_2物理吸附、X 射线衍射和透射电子显微镜等方法对载体和催化剂进行了表征;在小锈钢固定床反应器中,对 Co/SBA—15催化剂的 Fischer—Tropsch 合成性能进行r评价,考察了反应温度、反应压... 详细信息

采用初湿浸渍法制备了 Co/SBA—15催化剂,采用 N_2物理吸附、X 射线衍射和透射电子显微镜等方法对载体和催化剂进行了表征;在小锈钢固定床反应器中,对 Co/SBA—15催化剂的 Fischer—Tropsch 合成性能进行r评价,考察了反应温度、反应压力及合成气空速对 CO 转化率和产物选择性的影响,得到了 CO 转化率与反应温度、反应压力和合成气空速间的定量关系,并给出了数学表达式。实验结果表明,CO 转化率与反应温度呈指数关系、与反应压力呈线性关系、与合成气空速呈反比关系,过高或过低的反应温度、低反应压力和大合成气空速都不利于长链烃的生成。同时考察了反应时间对 Co/SBA-15催化剂 Fischer-Trop-sch 合成性能的影响。随反应时间的延长,CO 转化率降低,产物选择性变化不大,在考察反应温度、反应压力及合成气空速的影响时,可以忽略反应时间的影响。

关键词： Fischer-Tropsch合成合成气一氧化碳钴基催化剂 SBA-15分子筛

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彬长矿区特厚煤层顶水安全开采技术研究

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煤炭科学技术 2015年第11期43卷 22-26,128页

作者：段红民北京天地华泰矿业管理股份有限公司北京100013

为了预防彬长矿区特厚煤层顶水开采时"冒落带与裂缝带"导通洛河组含水层而发生水害事故,在对该矿区内的矿井裂高采高比研究的基础上,利用"三下"采煤规程和相关综放开采导水裂缝带高度公式分别计算预计了该矿区最大导水裂缝带高度,研究... 详细信息

为了预防彬长矿区特厚煤层顶水开采时"冒落带与裂缝带"导通洛河组含水层而发生水害事故,在对该矿区内的矿井裂高采高比研究的基础上,利用"三下"采煤规程和相关综放开采导水裂缝带高度公式分别计算预计了该矿区最大导水裂缝带高度,研究确定了该矿区煤层可采厚度和所适宜的预采顶分层综放或一次采全高综放2种开采工艺,结果表明:若采用预采顶分层综放开采工艺实现顶水安全开采,保证底分层开采厚度不超过7.5 m,顶分层采高应不超过3.5 m。若采用一次采全厚综放工艺时,可据区域主采煤层至洛河组的距离开采时依裂高采高比不大于20来确定合理的采高,严格控制采高,采取间隔放煤方法,严防过度放煤,同时生产中要加强顶板管理,加强矿压监测分析,保证工作面安全顶水开采。

关键词：综放开采顶水开采导水裂缝带特厚煤层

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乙醇浸渍对Co/SBA-15费托合成催化剂性能的影响

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催化学报 2009年第9期30卷 901-906页

作者：段洪敏葛庆杰张微徐恒泳中国科学院大连化学物理研究所辽宁大连116023 中国科学院研究生院北京100049

采用等体积浸渍法分别以乙醇和水为溶剂制备了Co/SBA-15催化剂,通过N2物理吸附、X射线衍射和程序升温还原等方法对催化剂进行了表征,并在固定床反应器中评价了催化剂的费托合成反应性能.结果表明,乙醇浸渍制备的催化剂钴粒子尺寸较小,... 详细信息

采用等体积浸渍法分别以乙醇和水为溶剂制备了Co/SBA-15催化剂,通过N2物理吸附、X射线衍射和程序升温还原等方法对催化剂进行了表征,并在固定床反应器中评价了催化剂的费托合成反应性能.结果表明,乙醇浸渍制备的催化剂钴粒子尺寸较小,金属钴分散度较高,钴粒子与载体之间的相互作用较强,还原温度较高,其费托合成反应活性和高碳烃选择性高于水溶液浸渍制备的催化剂.

关键词：乙醇浸渍钴基催化剂 SBA-15分子筛费托合成孔结构

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