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Nano Research 2025年第1期18卷 217-224页

作者： Taolue Sun Chen Jian Gang Wang Hui Zhao Guoliang Zhang Zengxi Li Chunshan Li State key laboratory of Mesoscience and Engineering CAS Key Laboratory of Green Process and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Huizhou Institute of Green Energy and Advanced Materials Huizhou 516081China Advanced Energy Science and Technology Guangdong laboratory Huizhou 516081China

Although the nickel-based catalyst is able toexhibit comparative catalytic activity to noble metal formethyl acrylate hydrogenation,it requires strict reactioncondition,which can be improved by regulation ofcoordination *** this study,we constructed akind of Ni single-atom coordinated with N and S(Ni-NSC)through the pyrolysis of organic Ni-based precursors at600℃.The existence and fine structure of Ni single-atom were confirmed by the spherical electron microscopicobservation in combination with the X-ray absorption spectroscopy(XAS)*** addition,the catalytichydrogenation assessment suggested that the as-prepared Ni-NSC catalyst exhibited higher activity and stability than theNi/NSC supported catalyst prepared by incipient wetness impregnation *** remarkable catalytic activity was dueto the high dispersion and density of Ni single-atom and weak adsorption energy of intermediates on these Ni sites.

关键词： methyl acrylate mild hydrogenation Ni single-atom coordination environment adsorption energy

Stability,acidity and interaction properties of [Bmim][SbF_6] coupled with concentrated sulfuric acid

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Science China Chemistry 2017年第9期60卷 1243-1249页

作者： Honghua Zhang Ruixia Liu Ruirui Zhang Feng Huo Zhiqiang Yang Bin He Suojiang Zhang Yanji Wang School of chemical Engineering Hebei University of Technology key laboratory of Green process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of Sciences

ionic liquid coupled with strong acid systems presents considerable promise in some catalytic fields. In the present work, the multiple complex systems composed by 98 wt% concentrated sulfuric acid and [Bmim][SbF6] were investigated in the terms of stability, acidity and interaction properties. It was found that acidolysis of [Bmim][SbF6] occurred in the 98 wt% concentrated sulfuric acid accompanied by HF releasing and SbF6−degrading to [SbF6−y(HSO4)y]−. The species after acidolysis in the multiple complex systems were checked and confirmed by electrospray ionization mass spectrometry (ESI-MS), Fourier transform infrared spectroscopy (FT-IR),1H NMR and19F NMR. Acidity increased slightly with less than 1 wt% [Bmim][SbF6] addition, while decreased with more proportion, which was determined based on the Hammett acidity functions H0, using13C NMR. The strong hydrogen bond S–O–HF of interaction among the multiple complex systems was confirmed by molecular dynamic simulation. © 2017, Science China Press and Springer-Verlag Berlin Heidelberg.

关键词： Electrodeposition Electrospray ionization Fourier transform infrared spectroscopy Hydrogen bonds ionic liquids Mass spectrometry Molecular dynamics Sulfuric acid

A new class of ion-ion interaction: Z-bond

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Science China Chemistry 2015年第3期58卷 495-500页

作者： Kun Dong Suojiang Zhang Qian Wang State key laboratory of Multiphase Complex Systems beijing key laboratory of ionic liquids clean process Institute Process Engineering Chinese Academy of Sciences

The hydrogen-bond interactions in ionic liquids have been simply described by the conventional hydrogen-bond model of A–H···B. Coupling with the strong electrostatic force, however, hydrogen bond between the cation and anion shows particular features in the geometric, energetic, electronic, and dynamic aspects, which is inherently different from that of the conventional hydrogen bond. A general model could be expressed as +[A–H···B]-, in which A and B represent heavy atoms and "+" and "–" represent the charges of the cation containing A atom and anion containing B atom, respectively. Because the structure shows a "zig-zag" motif, this coupling interaction is defined here as the Z-bond. The new model could be generally used to describe the interactions in ionic liquids, as well as bio-systems involved in ions, ionic reaction, and ionic materials.

关键词： ionic liquid interaction hydrogen bond Z-bond

Novel ionic liquid based electrolyte for double layer capacitors with enhanced high potential stability

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Science China Chemistry 2016年第5期59卷 547-550页

作者： Lan Zhang Kun Dong Shimou Chen Suojiang Zhang beijing key laboratory of ionic liquids clean chemical process State Key Laboratory of Multiphase Complex SystemsInstitute of Process and EngineeringChinese Academy of SciencesBeijing 100190China

Developing electrolyte with high electrochemical stability is the most effective way to improve the energy density of double layer capacitors(DLCs), and ionic liquid is a promising choice. Herein, a novel ionic liquid based high potential electrolyte with a stabilizer, succinonitrile, was proposed to improve the high potential stability of the DLC. The electrolyte with 7.5 wt% succinonitrile added has a high ionic conductivity of 41.1 m S cm^(-1) under ambient temperature, and the DLC adopting this electrolyte could be charged to 3.0 V with stable cycle ability even under a discharge current density of 6 A g^(-1). Moreover, the energy density could be increased by 23.4% when the DLC was charged to 3.0 V compared to that charged to 2.7 V.

关键词： double layer capacitor ionic liquid electrolyte high potential succinonitrile

Thermodynamics at microscales: 3D→2D, 1D and 0D

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Green Energy & Environment 2020年第3期5卷 251-258页

作者： Kun Dong Feng Huo Suojiang Zhang State key laboratory of Multiphase Complex Systems Beijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China

Today, the laws of traditional thermodynamics are facing challenges when science is growing rapidly toward the microscale-world, even quantum hypothesis. In this work, the thermodynamics of nano-confinement and quantu... 详细信息

关键词： Thermodynamics Confinement Quantum scale Entropy Reduced dimension

Highly selective and stable hydrogenation of heavy aromatic-naphthalene over transition metal phosphides

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Science China Chemistry 2015年第4期58卷 738-746页

作者： Muhammad Usman Dan Li Chunshan Li Suojiang Zhang beijing key laboratory of ionic liquids clean process State Key Laboratory of Multiphase Complex SystemsInstitute of Process Engineering University of Chinese Academy of Sciences

The present study reports a highly selective and stable catalytic approach for producing tetralin, an important chemical, solvent, and H2 storage material. Transition metal phosphides （MOP, Ni2P, Co2P, and Fe2P） were prepared by wet impregnation and temperature-programmed reduction and characterized by X-ray diffraction （XRD）, energy dispersive X-ray spectroscopy （EDX）, EDX mapping, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, brunauer-emmett- teller （BET）, temperature-programmed desorption of ammonia （NH3-TPD）, and fourier transform infrared spectroscopy of pyridine （pyridine-FTIR）. Of all the transition metal phosphides MoP was formed at a lower reduction temperature, which resuited in smaller particle size that enhanced the overall surface area of the catalyst. The existence of weak, moderate, and Lewis acidic sites over MoP were responsible for its high tetralin selectivity （90%） and stability during the 100 h reaction on-stream in a fixed-bed reactor.

关键词： coal tar naphthalene transition metal phosphides selective hydrogenation tetralin

Synthesis of spherical nano-ZSM-5 zeolite with intergranular mesoporous for alkylation of ethylbenzene with ethanol to produce m-diethylbenzene

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Chinese Journal of chemical Engineering 2024年第3期67卷 298-309页

作者： Siyue Wang Jinhong Li Qingxin Xu Shengjie Song Yu'ni Jiang Lidong Chen Xin Shi Weiguo Cheng Faculty of Chemistry and chemical Engineering Liaoning Normal UniversityDalian 110629China beijing key laboratory of ionic liquids clean process Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to develop efficient and stable heterogeneous ***,the spherical nano-ZSM-5 zeolite with abundant intergranular mesoporous is synthesized by the seed-mediated growth method for alkylation of EB with ethanol to produce *** results show that the spherical nano-ZSM-5 zeolite exhibits better stability and higher alkylation activity at a lower temperature than those of commercial micropore *** then,the spherical nano-ZSM-5 is further modified by La_(2)O_(3) through acid treatment followed by immersion *** acid treatment causes nano-ZSM-5 to exhibit the increased pore size but decreased the acid sites,and subsequent La_(2)O_(3) loading reintroduces the weak acid *** a result,the HNO_(3)-La_(2)O_(3)-modified catalyst exhibits a slight increase in EB conversion and DEB yield in comparison with unmodified one,and meanwhile,it still maintains high m-DEB *** catalyst after acid treatment achieves higher catalytic stability besides maintaining the high alkylation activity of EB with *** present study on the spherical nano-HZSM-5 zeolite and its modification catalyst with excellent alkylation ability provides new insights into the production of mDEB.

关键词： Zeolite Modification Alkylation reaction m-diethylbenzene Catalyst Fixed-bed

Pebax/TSIL blend thin film composite membranes for CO_2 separation

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Science China Chemistry 2016年第5期59卷 538-546页

作者： Zhongde Dai Lu Bai Karoline Navik Hval Xiangping Zhang Suojiang Zhang Liyuan Deng Department of chemical Engineering Norwegian University of Science and TechnologyTrondheim 7491Norway beijing key laboratory of ionic liquids clean process Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

In this study a thin film composite （TFC） membrane with a Pebax/Task-specific ionic liquid （TSIL） blend selective layer was prepared. Defect-flee Pebax/TSIL layers were coated successfully on a polysulfone ultrafiltration porous support with a poly- dimethylsiloxane （PDMS） gutter layer. Different parameters in the membrane preparation （e.g. concentration, coating time） were investigated and optimized. The morphology of the membranes was studied by scanning electron microscopy （SEM）, while the thermal properties and chemical structures of the membrane materials were investigated by thermo-gravimetric ana- lyzer （TGA）, differential scanning calorimetry （DSC） and Fourier transform infrared spectroscopy （FTIR）. The CO2 separation performance of the membrane was evaluated using a mixed gas permeation test. Experimental results show that the incorpora- tion of TSIL into the Pebax matrix can significantly increase both C02 permeance and CO2/N2 selectivity. With the presence of water vapor, the membrane exhibits the best CO2/N2 selectivity at a relative humidity of around 75%, where a CO2 permeance of around 500 GPU and a CO2/N2 selectivity of 46 were documented. A further increase in the relative humidity resulted in higher CO： permeance but decreased COIN2 selectivity. Experiments also show that CO2 permeance decreases with a CO2 partial pressure increase, which is considered a characteristic in facilitated transport membranes.

关键词： CO2 capture thin film composite membrane task specific ionic liquids Pebax post combustion

Angstrom science:Exploring aggregates from a new viewpoint

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Green Energy & Environment 2016年第1期1卷 75-78页

作者： Suojiang Zhang Feng Huo beijing key laboratory of ionic liquids clean process State Key Laboratory of Multiphase Complex SystemInstitute of Process EngineeringChinese Academy of Sciences

A small aggregate is composed of several or tens of molecules or ions, with at least one dimension in the range from a few to dozens of angstroms. Here, we named such aggregate system as Angstrom Aggregates(AA). AA with the specific size in angstrom meter might possess unique structure activity relationship. Unlike molecular level, nano system and the bulk, AA, an aggregate in angstrom scale is firstly proposed,its arrangement in order, electronic effect, surface interaction, confinement effect, is still unclear. However, recently, the structure and activity relationship of such aggregate in angstrom scale has attracted increasing interest in many areas, such as in ionic liquids, aqueous solution,catalytic system, and bio-system. As the physical and chemical propeties of AA strongly depends on its structure, the in situ characterizzation technique combined with theoretical methods should be developed to understand the exact interaction between the component of the clusters, the assembly formations, the special features, and the reaction activities. It has great scientific meaning to detect, represent and regulate the structure and function of AA precisely, facilitating in its application. A systematic and thorough research on AA in angstrom scale will promote the development of fundamental science and the progress of technology significantly.

关键词： Angstom science Aggregates Aqueous system Bio-system ionic liquids

Sub/supercritical carbon dioxide induced phase switching for the reaction and separation in ILs/methanol

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Green Energy & Environment 2016年第2期1卷 144-148页

作者： Jiayu Xin Dongxia Yan Ruimei Cao Xingmei Lu Huixian Dong Suojiang Zhang beijing key laboratory of ionic liquids clean process State Key Laboratory of Multiphase Complex System Institute of Process Engineering Chinese Academy of Sciences

Separation of products from ionic liquid(IL) solvents is one of the main challenges that hinder their utilizations. In this study, the production of γ-valerolactone(GVL) by selective hydrogenation of α-angelica lactone(AL) and separation of the products from the IL solvent were carried out by using subcritical CO_2 as a "switch" at room temperature. After the mixture was separated into two phases by subcritical CO_2, AL and nano Pd/C catalyst were only found in the lower IL-rich phase, GVL was produced with quantitative yield and enriched in the upper methanolrich phase. Pure GVL can be obtained by depressurizing to release CO_2 and evaporation to remove methanol of the upper phase, the lower phase containing IL, catalyst and methanol can be recycled for the next reaction. The strategy may provide a new approach to produce and separate products from IL solvents at mild conditions.

关键词： Separation ionic liquids Selective hydrogenation Mild condition Subcritical CO2