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3D coarse-grained DPM simulation of the MIP reaction-regeneration loop

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Particuology 2024年第6期89卷 57-66页

作者： Yanhao Ye Shuai Zhang Ji Xu Wei Ge state key laboratory of Mesoscience and engineering(formerly state key laboratory of Multiphase Complex Systems) Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of chemical engineering University of Chinese Academy of SciencesBeijing100049China

The reactor-regenerator loop is the core facility of the maximizing iso-paraffin(MIP)*** the discrete particle method(DPM)simulation can provide detailed information at the particle scale,it has been unable to simulate such a complex loop system due to limitations of coarse-grained(CG)models,computing software,and *** this study,a newly proposed soft-shell CG-DPM model with a CG ratio of up to 800 is used to simulate a 3.5 Mt/a industrial-scale MIP reactor-regenerator *** solid fraction distribution obtained is found to agree well with in-situ *** properties including the distribution of solid fraction,gas and solid velocity,standard derivation of solid fraction with time,temporal distribution of the flow field,and particle residence time distribution are measured in the simulation,which are meaningful to better design and operate such systems in the future.

关键词： Discrete particle method Coarse-grain Maximizing iso-paraffins Full-loop Reaction-regeneration system

Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China Chemistry 2024年第6期67卷 1935-1940页

作者： Ya-Ping Shao Zhuo-Min Chi Yong-Min Liang state key laboratory of Applied Organic Chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor *** method enables the synthesis of diverseβ-orγ-branched aromatic *** mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable ***,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

Porous metal oxides in the role of electrochemical CO_(2) reduction reaction

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Journal of Energy Chemistry 2024年第1期88卷 373-398,I0009页

作者： Ziqi Zhang Jinyun Xu Yu Zhang Liping Zhao Ming Li Guoqiang Zhong Di Zhao Minjing Li Xudong Hu Wenju Zhu Chunming Zheng Xiaohong Sun School of chemical engineering and Technology Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of Materials Science and engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China

The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil *** paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based *** metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction *** tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)*** work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low *** on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.

关键词： CO_(2)reduction Carbon dioxide Transformation Porous metal oxides Electrocatalysis

Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China Chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye key laboratory for chemical Biology of Fujian Province and state key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

Study on flow characteristics and phase holdup in a slurry bubble column coupled with mild agitation Author links open overlay panel

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Particuology 2024年第8期91卷 226-234页

作者： Qingyuan An Jiantao Li Lei Zhang Nailiang Wang Pengfei Zhang Zhenghong Luo Chunxi Lu state key laboratory of High-Efficiency Coal Utilization and Green chemical engineering Ningxia UniversityYinchuan750021China state key laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of Petroleum BeijingBeijing102249China Department of chemical&Biological engineering Monash UniversityVictoria3800Australia

A pilot-scale experimental setup was constructed to investigate the effect of mild agitation on the bubble characteristics and phase holdup in a slurry bubble *** agitation positively impacts the axial uniform distribution of solid holdup,though it shows insignificant influence on the radial *** homogenous regime,mild agitation promotes the coalescence of bubbles,and the effect becomes stronger with increasing agitator *** mild agitation contributes to a decrease in bubble size in heterogeneous flow *** agitation presents a significant effect on the gas holdup by adjusting the bubble size and bubble motion *** modification was introduced to predict the gas holdup considering the effects of mild agitation,a necessary consideration for applications requiring mild *** adapted model predicts gas holdup with a maximum error of 12.9%.

关键词： Slurry bubble column Mild agitation Phase holdup Bubble characteristics

Dielectric nanocomposites with superb high-temperature capacitive performance based on high intrinsic dielectric constant polymer

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Nano Research 2024年第9期17卷 8504-8512页

作者： Ding Ai Yuan Chang Haoliang Liu Chenglong Wu Yao Zhou Yuting Han Hao Yu Bing Xiao Yonghong Cheng Guanglei Wu Zirui Jia state key laboratory of Electrical Insulation and Power Equipment School of Electrical EngineeringXi’an Jiaotong UniversityXi’an 710049China Institute of Materials for Energy and Environment State Key Laboratory of Bio-Fibers and Eco-TextilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China

Advancements in power electronics necessitate dielectric polymer films capable of operating at high temperatures and possessing high energy *** significant strides have been achieved by integrating inorganic fillers into high-temperature polymer matrices,the inherently low dielectric constants of these matrices have tempered the magnitude of *** this work,we report an innovative nanocomposite based on sulfonylated polyimide(SPI),distinguished by the incorporation of sulfonyl groups within the SPI backbone and the inclusion of wide bandgap hafnium dioxide(HfO_(2))*** nanocomposite has demonstrated notable enhancements in thermal stability,dielectric properties,and capacitive performance at elevated *** simulations at both molecular and mesoscopic levels have elucidated the mechanisms behind these improvements,which could be attributed to confined segmental motion,an optimized electronic band structure,and a diminished incidence of dielectric breakdown ascribed to the presence of sulfonyl ***,the SPI-HfO_(2)nanocomposite demonstrates a high charge-discharge efficiency of 95.7%at an elevated temperature of 150℃and an applied electric field of 200 MV/***,it achieves a maximum discharged energy density of 2.71 J/cm^(3),signalling its substantial potential for energy storage applications under extreme conditions.

关键词： dielectric polymer nanocomposites high-temperature high dielectric constant sulfonyl groups energy storage performance

Enhancing alkyne semi-hydrogenation through engineering metal-support interactions of Pd on oxides

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Nano Research 2024年第5期17卷 3707-3713页

作者： Yuefeng Wu Xiaotong Lu Pengfei Cui Wenyu Jia Jun Zhou Yuan Wang Hussain Zahid Yuxin Wu Muhammad Umer Rafique Xiong Yin Baoshan Li Leyu Wang Guolei Xiang state key laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China CAS key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of chemical engineering Beijing University of Chemical TechnologyBeijing 100029China

Supported Pd catalysts show superior activities for olefin productions from alkynes through semi-hydrogenation reactions,but over-hydrogenation into alkanes highly decreases olefin *** phenylacetylene semi-hydrogenation as a model reaction,here we explore the optimization approaches toward better Pd catalysts for alkyne semi-hydrogenation through investigating support effect and metal-support *** results show that the states of Pd with supports can be tuned by varying oxide reducibility,loading ratios,and *** our system,0.06 wt.%Pd on rutile-TiO_(2) nanorods shows the highest activity owing to the synergistic effects of single-atoms and *** reducibility can change the filling degrees of Pd 4d orbitals through varying interfacial bonding strengths,which further affect catalytic activity and selectivity.

关键词： alkyne semi-hydrogenation support effect metal-support interaction Pd catalyst single-atom catalyst

High temperature polyimide nanocomposites containing twodimensional nanofillers for improved thermal stability and capacitive energy storage performance

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Nano Research 2024年第8期17卷 7746-7755页

作者： Ding Ai Yuting Han Zongliang Xie Xi Pang Yuan Chang He Li Chenglong Wu Yonghong Cheng Guanglei Wu state key laboratory of Electrical Insulation and Power Equipment School of Electrical EngineeringXi’an Jiaotong UniversityXi’an 710049China Institute of Materials for Energy and Environment State Key Laboratory of Bio-Fibers and Eco-TextilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China

Future electronic devices toward high integration and miniaturization demand reliable operation of dielectric materials at high electric fields and elevated ***,the electrical deterioration caused by Joule heat generation remains a persistent challenge to ***,the solution-processed polyimide(PI)nanocomposites with unique two-dimensional(2D)alumina nanoplates are *** improvements in the breakdown strength,charge–discharge efficiency and discharged energy density at elevated temperatures have been demonstrated in the composites,owing to simultaneously suppressed conduction loss and increased thermal conductivity upon the incorporation of 2D Al_(2)O_(3) nanofillers possessing excellent dielectric insulation and thermophysical *** predominance of Al_(2)O_(3) nanoplates in enhancing thermal stability and high-temperature capacitive performance over nanoparticles and nanowires is validated experimentally and is further rationalized via finite element ***,the Al_(2)O_(3) nanoplates filled PI nanocomposite exhibits a hightemperature capability up to 200℃ and remarkable efficiency(e.g.≥95% at 200 MV/m)over a wide temperature range,which outperforms commercial dielectric polymers and rivals the state-of-the-art polyimide nanocomposites.

关键词： capacitors polymer nanocomposites high temperature energy storage thermal stability

Preparation and properties of poly(ethylene glycol)-bpoly( 3-acrylamidophenylboronic acid) glucose responsive particles and their hyaluronic acid-based microneedle patches

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Journal of Zhejiang University-Science A(Applied Physics & engineering) 2024年第5期25卷 395-410页

作者： Yichuan HONG Haojie YU Li WANG Xiang CHEN Di SHEN Yu WANG Shuning REN Yudi HUANG Jian YANG state key laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Zhejiang-Russia Joint laboratory of Photo-Electro-Magnetic Functional Materials College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

To overcome the pain and risk of hypoglycemia in insulin administration,glucose-responsive microneedles have been developed by researchers,which could release insulin according to the blood glucose *** designed a kind of particles by a reversible addition-fragmentation chain transfer(RAFT)method containing a phenylboronic acid group as the sensor of glucose and carrier of ***(ethylene glycol)(PEG)-2-(dodecylthio(thiocarbonyl)thio)-2-methylpropionic acid(DDMAT)was synthesized as a macromolecular RAFT agent,which was then reacted with 3-acrylamidophenylboronic acid(AAPBA)to synthesize the block copolymer ***-responsive particles loaded with insulin were prepared by self-assembly based on hydrophilic-hydrophobic *** patches loaded with glucose-responsive particles were prepared using hyaluronic acid as the *** insulin release behavior of the particles in glucose solutions of 0,100,and 400 mg/dL showed significant glucose responsiveness and good *** results of blood glucose control experiments in rats indicate that a single microneedle patch can effectively maintain normal blood glucose for over 7 h.

关键词： Diabetes Hyaluronic acid Phenylboronic acid(PBA) Glucose responsive hydrogel Microneedles