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Active Fischer-Tropsch synthesis Fe-Cu-K/SiO_2 catalysts prepared by autocombustion method without a reduction step

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Journal of Energy Chemistry 2018年第2期27卷 432-438页

作者： Suthasinee Pengnarapat Peipei Ai Prasert Reubroycharoen Tharapong Vitidsant Yoshiharu Yoneyama noritatsu tsubaki Program in Petrochemistry Faculty of ScienceChulalongkorn University Department of Applied Chemistry School of EngineeringUniversity of Toyama Department of Chemical Technology Faculty of ScienceChulalongkorn University

The purpose of this study was to prepare iron-based catalysts supported on silica by autocombustion method for directly using for Fischer-Tropsch synthesis（FTS） without a reduction step. The effect of different citric acid（CA）：iron nitrate（N） molar ratios and acid types on the FTS performance of catalysts were investigated. The CA：N molar ratios had an important influence on the formation of iron active phases and FTS activity. The iron carbide（FexC）, which is known to be one of the iron active phases, was demonstrated by the X-ray diffraction and X-ray photoelectron spectroscopy. Increasing the CA：N molar ratios up to 0.1 increased CO conversion of catalyst to 86.5%, which was then decreased markedly at higher CA：N molar ratios. An excess of CA resulted in carbon residues covering the catalyst surface and declined FTS activity. The optimal catalyst（CA：N molar ratio = 0.1） achieved the highest CO conversion when compared with other autocombustion catalysts as well as reference catalyst prepared by impregnation method, followed by a reduction step. The autocombustion method had the advantage to synthesize more efficient catalysts without a reduction step. More interestingly, iron-based FTS catalysts need induction duration at the initial stage of FTS reaction even after reduction, because metallic iron species need time to be transformed to FexC. But here, even if without reduction, FexC was formed directly by autocombustion and induction period was eliminated during FTS reaction.

关键词： Fischer-Tropsch synthesis Iron-based catalysts Autocombustion Iron carbide SiO2

Catalytic Oxidation of Dimethyl Ether to Dimethoxymethane over Cs Modified H_3PW_(12)O_(40)/SiO_2 Catalysts

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Journal of Natural Gas Chemistry 2007年第3期16卷 322-325页

作者： Qingde Zhang Yisheng Tan Caihong Yang Yizhuo Han Jun Shamoto noritatsu tsubaki State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 Shanxi China Graduate University of Chinese Academy of Sciences Beijing 100049 China Department of Applied Chemistry University of Toyama Toyama 930-8555 Japan

The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40（40%）/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40（40%）/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40（40%）/SiO2.

关键词： dimethyl ether dimethoxymethane catalytic oxidation Cs modified H3PW12O40/SiO2 XRD

Facilitating efficient photocatalytic hydrogen evolution via enhanced carrier migration at MOF-on-MOF S-scheme heterojunction interfaces through a graphdiyne(C_(n)H_(2n-2))electron transport layer

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Chinese Journal of Structural Chemistry 2023年第12期42卷 11-23页

作者： Fei Jin Bolin Yang Xuanpu Wang Teng Li noritatsu tsubaki Zhiliang Jin School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan750021PR China Department of Applied Chemistry Graduate School of EngineeringUniversity of ToyamaGofuku3190Toyama930-8555Japan

Interface engineering of photocatalysts is an effective way to enhance their photocatalytic *** this work,the MOF-on-MOF strategy was used to construct the ZIF-9(Co)/Cu_(3)BTC_(2) photocatalyst in ***,graph-diyne,possessing an inherent capability to facilitate rapid electron transfer at the interface,has been introduced into the ZIF-9(Co)/Cu_(3)BTC_(2) interface to regulate the interfacial carrier *** photogenerated carrier transfer capability has been significantly enhanced by the interfacial synergy,while retaining the original active sites and high specific surface *** exceptional efficiency performance of the composite catalyst under identical conditions could be attributed to the following two key factors:(i)The interfacial S-scheme hetero-junction in ZIF-9(Co)/Cu_(3)BTC_(2) provides the composite catalyst with strong reduction activity,facilitating the involvement of additional electrons in the reduction reaction through bended bands and an internal electric field.(ii)Carrier dynamics analysis shows that graphdiyne,as an electron transport layer,accelerates the charge migration rate at the S-scheme heterojunction interface through the electron relay *** incorporation of graphdiyne greatly improves the catalytic activity of MOFs and also demonstrates the great potential of graph-diyne in *** work provides a feasible idea for the interface engineering design of graphdiyne in photocatalysts.

关键词： Graphdiyne S-scheme heterojunction MOFs Photocatalytic hydrogen evolution

Tuning the crystallite size of monoclinic ZrO_(2) to reveal critical roles of surface defects on m–ZrO_(2) catalyst for direct synthesis of isobutene from syngas

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Chinese Journal of Chemical Engineering 2021年第7期34卷 211-219页

作者： Xuemei Wu Minghui Tan Bing Xu Shengying Zhao Qingxiang Ma Yingluo He Chunyang Zeng Guohui Yang noritatsu tsubaki Yisheng Tan State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China Department of Applied Chemistry School of EngineeringUniversity of ToyamaGofuku 3190Toyama 930-8555Japan China Petroleum Chemical Industry Federation Beijing 100723China

The effects of crystallite size on the physicochemical properties and surface defects of pure monoclinic ZrO_(2) catalysts for isobutene synthesis were *** prepared a series of monoclinic ZrO_(2) catalysts with different crystallite size by changing calcination temperature and evaluated their catalytic performance for isobutene synthesis from ***_(2) with small crystalline size showed higher CO conversion and isobutene selectivity,while samples with large crystalline size preferred to form dimethyl ether(DME)instead of hydrocarbons,much less to *** defects(ODefects)analyzed by X-ray photoelectron spectroscopy(XPS)provided evidence that more ODefectsoccupied on the surface of ZrO_(2) catalysts with smaller crystalline *** paramagnetic resonance(EPR)and ultraviolet–visible diffuse reflectance(UV–vis DRS)confirmed the presence of high concentration of surface defects and Zr3+on mZrO_(2)-5.9 sample,*** situ diffuse reflectance infrared Fourier transform spectroscopy(in situ DRIFTS)analysis indicated that the adsorption strength of formed formate species on catalyst reduced as the crystalline size *** results suggested that surface defects were responsible for CO activation and further influenced the adsorption strength of surface species,and thus the products distribution *** study provides an in-depth insight for active sites regulation of ZrO_(2) catalyst in CO hydrogenation reaction.

关键词： Syngas Isobutene ZrO_(2)catalyst Crystallite size Surface defects

One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

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Chinese Journal of Chemical Engineering 2021年第8期34卷 101-110页

作者： Ce Du Linet Gapu Chizema Emmerson Hondo Mingliang Tong Qingxiang Ma Xinhua Gao Ruiqin Yang Peng Lu noritatsu tsubaki Zhejiang Provincial Key Lab for Chem.&Bio.Processing Technology of Farm Product School of Biological and Chemical EngineeringZhejiang University of Science and TechnologyHangzhou 310023China Department of Applied Chemistry School of EngineeringUniversity of ToyamaGofuku 3190Toyama 930-8555Japan State Key Laboratory Cultivation Base of Natural Gas Conversion Ningxia UniversityYinchuan 750021China

Light olefins(C_(2)–C_(4))are fundamental building blocks for the manufacture of polymers,chemical intermediates,and *** this work,we realized a composite catalyst,comprising MnxZry oxides and SAPO-34 zeolite,which can convert syngas(CO+H_(2))into light *** oxide catalysts with different Mn/Zr molar ratios were facilely prepared using the coprecipitation method prior to physical mixing with SAPO-34 *** redox properties,surface morphology,electronic state,crystal structure,and chemical elemental composition of the catalysts were examined using H_(2)-TPR,SEM,XPS,XRD,and EDS techniques,*** reactions involved activation of CO and subsequent hydrogenation over the metal oxide catalyst,producing methanol and dimethyl ether as the main reaction intermediates,which then migrated onto SAPO-34 zeolite for light olefins *** of temperature,pressure and reactant gas flow rate on CO conversion and light olefins selectivity were investigated in *** Mn_(1)Zr_(2)/SAPO-34 catalyst(Mn/Zr ratio of 1:2)attained a CO conversion of 10.8%and light olefins selectivity of 60.7%,at an optimized temperature,pressure and GHSV of 380℃,3 MPa and 3000h^(−1) *** findings open avenues to exploit other metal oxides with CO activation capabilities for a more efficient syngas conversion and product selectivity.

关键词： Catalyst C-C coupling CO activation Hydrogenation Light olefins Syngas

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低温甲醇合成研究进展

化工学报 2015年第9期66卷 3333-3340页

作者：石磊张婉莹王玉鑫 tsubaki noritatsu 沈阳化工大学应用化学学院辽宁沈阳110142 Department of Applied Chemistry School of EngineeringUniversity of Toyama

日本学者tsubaki等开创了一种全新的低温甲醇合成反应路径。该路径以含有二氧化碳的合成气为反应原料,使用单一低碳醇（包括甲醇）同时作为催化剂和溶剂,实现了反应原料一氧化碳在低温（443 K）条件下,一步转化率达到70%～100%。原位红... 详细信息

日本学者tsubaki等开创了一种全新的低温甲醇合成反应路径。该路径以含有二氧化碳的合成气为反应原料,使用单一低碳醇（包括甲醇）同时作为催化剂和溶剂,实现了反应原料一氧化碳在低温（443 K）条件下,一步转化率达到70%～100%。原位红外和多种表征手段证明,该反应能够在低温条件下进行,是由于催化剂上吸附的甲酸盐物种可以和多种低碳醇溶剂在低温条件发生酯化反应,生成相对应的甲酸酯。而生成的甲酸酯很容易在低温条件下,铜基催化剂表面,发生加氢反应,生成甲醇和相应的溶剂醇。该种全新的甲醇合成路径克服了常规甲醇合成过程中,甲酸盐必须在高温条件下才能发生加氢反应的关键步骤。同时,还介绍了适用于低温甲醇合成反应的金属Cu/ZnO催化剂制备方法的研究进展。全新的溶胶-凝胶-燃烧法、固相研磨-燃烧法以及甲酸辅助燃烧法直接制备高活性、纳米尺度、高分散的金属Cu/ZnO催化剂,而不需要额外的还原流程。

关键词：催化剂酯化加氢反应动力学低温甲醇合成 Cu/ZnO 原位红外免还原

Synthesis and Characterization of Condensed Polynuclear Aromatic Resin Derived from Ethylene Tar

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China Petroleum Processing & Petrochemical Technology 2012年第4期14卷 42-47页

作者： Wu Mingbo Shi Yangyang Li Shibin Wang Yuwei Tan Minghui Wang Ding Zheng Jingtang tsubaki noritatsu State Key Laboratory of Heavy Oil Processing China University of Petroleum Department of Applied Chemistry School of EngineeringUniversity of ToyamaGofuku 3190Toyama 930-8555Japan

As a kind of low-cost and readily available industrial byproduct, ethylene tar （ET） was for the first time utilized for the preparation of heat-resistant condensed polynuclear aromatic resin （COPNAR）. The basic properties of ET and the resulted COPNAR were characterized by FT-IR, IH-NMR, TGA and elemental analysis. The test results showed that ET with high aromatic content （〉50%） was suitable for the synthesis of COPNAR with superior heat resistance. The average molecular structure of ET was obtained by means of the improved Brown-Ladner method, and the reaction mechanism was considered as an acid-catalyzed positive ion-typed polymerization. Our findings have provided a new route to develop ET into technology-added heat-resistant resins.

关键词： condensed polynuclear aromatic resin ethylene tar 1, 4-benzenedimethanol heat resistance

Al_2O_3改性Co/SiO_2费托合成催化剂的制备及结构表征

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中国石油大学学报（自然科学版） 2009年第5期33卷 148-150,155页

作者：孙晓瑜张燚鲍骏 tsubaki noritatsu 中国石油大学图书馆山东东营257061 日本富山大学工学部中国科学技术大学国家同步辐射实验室安徽合肥230026

采用溶液浸渍法制备不同含量Al2O3的Co/SiO2-Al2O3催化剂。采用程序升温还原(TPR)、X射线衍射(XRD)、物理吸附(BET)以及原位CO吸附红外光谱(DRIFT)对催化剂进行表征。结果表明:Al2O3的添加导致催化剂比表面积稍有下降,但对孔径分布无明... 详细信息

采用溶液浸渍法制备不同含量Al2O3的Co/SiO2-Al2O3催化剂。采用程序升温还原(TPR)、X射线衍射(XRD)、物理吸附(BET)以及原位CO吸附红外光谱(DRIFT)对催化剂进行表征。结果表明:Al2O3的添加导致催化剂比表面积稍有下降,但对孔径分布无明显影响;随着Al2O3负载量的增加,载体表面钴粒子粒径变小,分散度提高,同时还原度逐步降低;Al2O3改性后催化剂表面CO吸附峰位发生蓝移,并且桥式CO吸附峰强度明显增大,说明Al2O3改性后钴催化剂具有更高的表面活性。

关键词：费托合成 Co/SiO2催化剂 Al2O3改性表征

New Chemical and Energy Processes Initiated by Novel Zeolite Capsule Catalysts

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New Chemical and Energy Processes Initiated by Novel Zeolite...