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Synthesis of SAPO-34 using metakaolin in the presence of β-cyclodextrin

Journal of Energy Chemistry 2015年第4期24卷 401-406页

作者： Chen Zhang Xuchen Lu Tizhuang Wang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of Sciences (CAS) University of Chinese Academy of Sciences United Research Center for Resource and Materials

SAPO-34 molecular sieves were synthesized by the addition of β-cyclodextrin（β-CD） as crystal growth inhibitor using metakaolin as silicon and aluminum sources. Properties of the obtained samples were characterized by XRD,SEM,N2adsorption–desorption,FTIR,XRF,EDX,NH293-TPD andSi MAS NMR. When β-CD was added,crystal size of the SAPO-34 crystals decreased. Variation of Si content from the crystal center to surface decreased while total Si content hardly changed.29 Si MAS NMR results showed that β-CD contributed to better Si dispersion and decreased the size of Si（4Si） patches. Moreover,the MTO（methanol-to-olefin） process was conducted to investigate the influence of β-CD on catalytic performance. The synthesized sample with molar ratio of β-CD/Al2O3 equaling 0.055 remained active for 610 min while the sample synthesized without β-CD for only 280 min,which indicates that the lifetime of catalyst synthesized with β-CD is greatly prolonged.

关键词： SAPO-34 Metakaolin β-cyclodextrin Acidity MTO process

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Heterojunctioned CuO/Cu_(2)O catalyst for highly efficient ozone removal

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Journal of Environmental Sciences 2023年第3期125卷 340-348页

作者： Guojun Ma Wenxiang Tang AnqiWang Le Zhang Jian Guan Ning Han Yunfa Chen Key Laboratory of Science and Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering Sichuan UniversityChengdu 610065China

In recent years, near surface ozone pollution, has attracted more and more attention,which necessitates the development of high efficient and low cost catalysts. In this work,Cu O/Cu_(2)O heterojunctioned catalyst is fabricated by heating Cu_(2)O at high temperature, and is adopted as ozone decomposition catalyst. The results show that after Cu_(2)O is heated at180℃conversion of ozone increases from 75.2% to 89.3% at mass space velocity 1,920,000cm^(3)/(g·hr) in dry air with 1000 ppm V ozone, which indicates that this heterojunction catalyst is one of the most efficient catalysts reported at present. Catalysts are characterized by electron paramagnetic resonance spectroscopy and ultraviolet photoelectron spectroscopy,which confirmed that the heterojunction promotes the electron transfer in the catalytic process and creates more defects and oxygen vacancies in the Cu O/Cu_(2)O interfaces. This procedure of manufacturing heterostructures would also be applicable to other metal oxide catalysts, and it is expected to be more widely applied to the synthesis of high-efficiency heterostructured catalysts in the future.

关键词： Cu_(2)O Ozone decomposition CuO Heterojunction

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Highly efficient ozone elimination by metal doped ultra-fine Cu_(2)O nanoparticles

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Journal of Environmental Sciences 2023年第12期134卷 108-116页

作者： Anqi Wang Le Zhang Jian Guan Xiaoze Wang Guojun Ma Guijun Fan Hang Wang Ning Han Yunfa Chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Key Laboratory of Science&Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Metallurgical Engineering Xi’an University of Architecture and TechnologyXi’an 710055China

Nowadays,ozone contamination becomes dominant in air and thus challenges the research and development of cost-effective *** this study,metal doped Cu_(2)O catalysts are synthesized via reduction of Cu^(2+)by ascorbic acid in base solutions containing doping metal *** results show that compared with pure Cu_(2)O,the Mg^(2+)and Fe^(2+)dopants enhance the O_(3)removal efficiency while Ni2+depresses the *** specific,Mg-Cu_(2)O shows high O3removal efficiency of 88.4%in harsh environment of 600,000 mL/(g·hr) space velocity and 1500 ppmV O_(3),which is one of the highest in the *** and electron paramagnetic spectroscopy characterization shows higher concentration of crystal defects induced by the Mg^(2+)dopants,favoring the *** in-situ diffuse reflectance Fourier transform infrared spectroscopy shows the intermediate species in the O_(3)degradation process change from O_(2)^(2-)dominant of pure Cu_(2)O to O_(2)^(-)dominant of Mg-Cu2O,which would contribute to the high *** these results show the promising prospect of the Mg-Cu_(2)O for highly efficiency O_(3)removal.

关键词： Ozone catalyst Cu_(2)O Dopant Ultra-fine nanoparticles

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Rational construction of multiple hollow silicalite-1 zeolite with enhanced quasi acidity for robust vapor-phase Beckmann rearrangement

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Nano Research 2023年第5期16卷 7958-7966页

作者： Peng Zhang Xianfeng Yi Changjiu Xia Xinxin Peng Shuai Zhang Chengxiang Li Anmin Zheng Xiaoxin Zhang Yibin Luo Lifeng Cui Fuhong Yu Xingtian Shu State Key Laboratory of Catalytic Materials and Reaction Engineering Research Institute of Petroleum ProcessingSINOPECBeijing 100083China State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics National Center for Magnetic Resonance in WuhanWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071China Shandong Hualu-Hengsheng Chemical Co. Ltd.Dezhou 253024China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Developing efficient and stable zeolites for vapor-phase Beckmann rearrangement of cyclohexanone oxime is still a great challenge to realizeε-caprolactam(CPL)green *** this work,the hierarchical porous silicalite-1 zeolites with multiple hollow structure(S-1-M)are explored by in-situ desilication−recrystallization post-treatment of spongy highway-like zeolites(S-1-S),which are synthesized through silanization synthesis of conventional bulky silicalite-1(S-1).Compared to S-1,S-1-M achieves superior catalytic performance,with improving the CPL selectivity from 85.7%to 94.1%and prolonging the catalyst lifetime from 74 to 126 h at a weight hourly space velocity(WHSV)of 6 h^(−1).Comprehensive physiochemical studies demonstrate that the highly dispersed intracrystalline cavities within S-1-M endow greater mass diffusion and better quasi acidity inducing by the enhanced H-bonds among abundant H-bonded silanols,which is cooperatively responsible for its superior catalytic performance.

关键词： hollow silicalite-1 H-bonded silanols quasi acidity vapor-phase Beckmann rearrangement

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Electrocatalytic Cleavage of C-C Bonds in Lignin Models Using Nonmetallic Catalysts at Ambient Conditions

Chem and Bio Engineering

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Chem and Bio Engineering 2024年第4期1卷 357-365页

作者： Liu, Guangyong Zhai, Ziqi Lu, Yumiao Lu, JunFeng Wang, Yanlei Liang, Shijing He, Hongyan Jiang, Lilong National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou University Fujian Fuzhou350002 China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Zhengzhou450000 China

Lignin, characterized by its amorphous, heavily polymerized structure, is a primary natural source of aromatic compounds, yet its complex constitution poses considerable challenges in its transformation and utilization. Therefore, the selective cleavage of C-C bonds represents a critical and challenging step in lignin degradation, essential for the production of high-value aromatic compounds. In this study, we report a simple electrocatalytic approach for lignin valorization via C-C bond cleavage by developing a nonmetallic electrocatalyst of carbon-based materials. It is found that the hydrophilicity and hydrophobicity of the electrocatalyst have a significant effect on the degradation process. Under mild conditions, the hydrophilic carbon paper exhibits 100% substrate conversion, yielding 97% benzaldehyde and 96% quinone with ionic liquid electrolytes. The mechanism study shows that the carbon catalyst with higher surface defects favors electron transfer in the oxidative cleavage process of C-C bonds. These results signify a substantial advancement in lignin degradation, offering an environmentally friendly, metal-free electrochemical route. © 2024 The Authors. Co-published by Zhejiang University and American Chemical Society.

关键词： Quinone

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CoSe_(2)/MoS_(2) Heterostructures to Couple Polysulfide Adsorption and Catalysis in Lithium-Sulfur Batteries

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Chinese Journal of Chemistry 2021年第5期39卷 1138-1144页

作者： Zihan Shen Qingwen Zhou Huiling Yu Jiaming Tian Man Shi Chaoquan Hu Huigang Zhang Notional Laboratory of Solid State Microstructures College of Engineering and Applied SciencesInstitute of Materials Engineeringand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingJiangsu 210046China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry NanjingJiangsu 211100China

Lithium-sulfur batteries have been regarded as one of most promising next-generation energy storage devices because of their high energy density and low ***,polysulfide shuttling and slow kinetics hinder the practical *** fabricated hierarchically heterostructured CoSe_(2)/MoS_(2) nanoarrays on carbon clothes as the sulfur cathode *** resulting heterostructures facilitate electron conduction and improve electrolyte *** importantly,the composite heterostructures couple the strong poly-sulfide adsorption of CoSe_(2) and high catalytic activity of MoS_(2) to synergistically accelerate polysulfide conversion,demonstrating higher catalytic activity than their individual components.

关键词： Lithium-sulfur batteries Heterostructure Electrocatalyst CoSe_(2) MoS_(2)

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Stimuli-Responsive lonic Liquids and the Regulation of Aggrega-tion Structure and Phase Behavior

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Chinese Journal of Chemistry 2021年第3期39卷 729-744页

作者： Xiao-Qing Yuan Ya-Qin Zhang Zhi-Yong Li Feng Huo Yi-Hui Dong Hong-Yan He Beijing Key Laboratory of lonic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBejling 100190China Dalian National Laboratory for Clean Energy DalianLiaoning 116023China Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chermical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenan 453007China

lonic liquids with stimuli-responsive characteristics are an essential branch in the comprehensive ionic liquids'family,which can meet the controllable and reversible needs in practical applications with different stimulation *** this review,we summarize the recent research progress of these stimuli-responsive ionic liquids,mainly focusing on their chemical structures,properties,responsive mechanism,aggregation structures,and phase behaviors,which were driven by external stimuli,such as CO2,magnetism,light,temperature,redox,and ***,the particular or potential applications of stimuli-responsive ionic liquids are expounded in various fields of science,including catalytic reaction,extraction,separation,nano-material preparation,and gas *** the end,the challenges and strategies of the subject are briefly *** is expected that this review will contribute to the rational design and applications of stimu-liresponsive ionic liquids in the future.

关键词： lonic liquids Stimuli Responsive Aggregation Phase behavior

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Rough-surfaced bimetallic Cu-Pd alloy multicubes as highly effective electrocatalysts for formic acid oxidation and oxygen reduction

Rough-surfaced bimetallic Cu-Pd alloy multicubes as highly e...

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中国化学会第十届全国无机化学学术会议

作者： Dong Chen Linlin Xu Hui Liu Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Center for Mesoscience Institute of Process Engineering Chinese Academy of Sciences

Engineering the morphology of nanomaterials and modifying their electronic structure are effective ways to improve their performance in electrocatalysis. Through combining the co-reduction of Pd and Cu precursors with a digestive ripening process in oleylamine, we synthesized Cu-Pd alloy multicubes with rough surfaces. Benefiting from their alloy and unique rough-surfaced structure, which provides ample edge/corner and step atoms as well as the electronic coupling between Cu and Pd leading to the lower of d-band center, the rough-surfaced Cu-Pd alloy multicubes show much better electrocatalytic performance not only for formic acid oxidation but also for oxygen reduction in comparison with those of spherical Cu-Pd alloy nanoparticles and commercial Pd/C catalyst. In contrast, we confirm that the rough-surfaced Cu-Pd alloy multicubes only exhibit very low Faradaic efficiency（34.3%） for electrocatalytic conversion of carbon dioxide（CO） to carbon monoxide（CO） due to the presence of strong competing hydrogen evolution reaction.

关键词： Multicube Formic acid oxidation Oxygen reduction CO2 reduction

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Excellent Antibacterial Performance of ROS-mediated Cu-doped ZIF-8 and the Mechanism of ROS Generation 18

Excellent Antibacterial Performance of ROS-mediated Cu-doped...

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18th International Conference on Indoor Air Quality and Climate, INDOOR AIR 2024

作者： Chen, Yunfa Zhang, Jingkun Ding, Yan Yin, Hang State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing China Vehicle Emission Control Center Chinese Research Academy of Environmental Sciences Beijing China

ISBN: (纸本)9798331306816

Nowadays, it is necessary to explore efficient antibacterial materials to complement or substitute the conventional antibiotic, to cope with the ever-growing bacterial contamination. Here, a series of Cu-doped ZIF-8 materials are prepared and adopted for disinfection against typical bacteria E. coli and S. aureus in dark. The results show that 5-7 log efficiency can be achieved at a dosage of 15-30 mg mL-1 of 1.35 atomic % Cu doped ZIF-8, and this concentration is also safe as verified by cytotoxicity test. Mechanism investigation shows that Cu(II) is reduced to Cu(I), which would contribute to the effective electron transfer for the reactive oxygen species generation. And these reactive oxygen species would cause oxidative stress and membrane damage on bacteria cells. All these results show the promise of Cu-doped ZIF-8 in the antibacterial applications especially in the environments without any energy input. © 2024 18th Conference of the International Society of Indoor Air Quality and Climate, INDOOR AIR 2024 - Conference Program and Proceedings. All rights reserved.

关键词： Reactive oxygen species

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Ru single atoms induce surface-mediated discharge in Na-O_(2)batteries

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Chinese Chemical Letters 2022年第1期33卷 491-496页

作者： Xin Jin Yangyang Li Shuo Zhang Jiangwei Zhang Zihan Shen Chenlin Zhong Ziqiang Cai Chaoquan Hu Huigang Zhang National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced MicrostructuresCollege of Engineering and Applied SciencesNanjing UniversityNanjing 210093China Dalian National Laboratory for Clean Energy&State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences(CAS)Dalian 116023China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100China

Sodium(Na)O_(2)batteries have high energy density and low ***,high polarization,complex discharge products,and low Coulombic efficiency(CE)lead to poor ***,we proposed an atomically dispersed Ru catalyst on nitrogen-doped graphene for Na-O_(2)*** catalysts enable the discharge to proceed via a surface-mediated route,which leads to uniform deposition of Na_(2-x)O_(2)and low polarization during *** first-principle calculation revealed that Ru-N_(4)complex in the catalyst has strong chemical adsorption to intermediate superoxides,facilitating uniform deposition and enhancing rapid *** contrast,Ru nanoparticles,despite the catalytic activity,induce bulk deposition via a solution-mediated route because the exposed graphene surface shows weak interaction to superoxides,thereby lowering CEs and *** brief,the atomically-dispersed Ru catalyst endows Na-O_(2)batteries with excellent electrochemical properties via a surface-mediated discharge.

关键词： Na-O_(2)batteries Ru single atoms Surface-mediated mechanism Adsorption energy Co-deposition

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