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Molecule configurations modulate packing array and charge transfer in cocrystal engineering

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Science China Chemistry 2024年第2期67卷 512-516页

作者： Shenglong An Mengyuan Qiao Xin Jin Xuanying Chen Jianhua Su Lifang Guo Zhiyun Zhang Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CentreFrontiers Science Center for Materiobiology and Dynamic ChemistryEast China University of Science&TechnologyShanghai200237China

Organic cocrystal as an emerging assembly strategy has received increasing attention in constructing multiple functional materials,through continually screening suitable constituent monomers or changing their stoichiometry ***,the role of molecule configuration in the cocrystal field is rarely explored despite the fascinating potential in regulating the packing *** this study,the N,N′-diphenyl-5,10-dihydrophenazine derivatives(DPPs) with the flexible scaffold and different methyl substitutions are selected as the donors bearing various molecular *** a simple collaborative way,a series of cocrystals based on DPPs and OFN(octafluoronaphthalene) are fabricated,exhibiting two self-adaptive molecular stacking arrays.X-ray crystallographic analysis and theoretical calculation unveil their different π···π interactions and charge transfer characters,leading to the significant emission redshift up to 125 nm compared with individual *** a result,controllable molecule stacking structure,tunable emission,and charge transfer properties can be *** study provides a new perspective to reveal the structure-property relationships at the molecular level by controlling the molecule configuration in cocrystal engineering,contributing to the development of cocrystal theoretical physics and organic functional materials.

关键词： cocrystals molecular configuration self-adaptive packing mode charge transfer

Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

Developing silicon-based photocathodes for CO_(2) conversion

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Science China Chemistry 2024年第6期67卷 1904-1921页

作者： Weijie Zhuang Miao Kan Tao Meng Jinlong Zhang Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Shanghai Engineering research center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai200237China

Photoelectrochemical(PEC)conversion of CO_(2) presents a promising avenue for solar-driven chemical fuel production,with silicon emerging as a cost-effective and high-light-absorbing material pivotal to this *** at exploring opportunities for industrializing PEC CO_(2) reduction(PEC-CO_(2)R)by minimizing reaction energy consumption,enhancing reaction efficiency and selectivity,this review summarizes recent advancements in developing Si-based photocathodes for PEC-CO_(2)*** outlines the fundamental principles,advantages,and limitations of Si photocathodes with key performance *** on this understanding,the strategies to enhance the performance of the PEC-CO_(2)R system,including light absorption,charge separation,and catalytic reactions are categorized as the interfacial modification,active site decoration,and protective layer *** design ideas of this advantageous three-layer structure in promoting the efficiency,stability,and selectivity have been ***,this review scrutinizes the influence of the photocathodic chemical *** review consolidates the mechanism insights and notable breakthroughs of various fuel generation processes within Si-based PEC-CO_(2)R *** this wealth of information offers an up-to-date perspective on the dynamic developments in silicon-based PEC-CO_(2) conversion and underscores the promising pathways toward the sustainable fuel synthesis from pollutant CO_(2).

关键词： photoelectrochemistry solar fuels silicon photocathodes carbon dioxide reduction microenvironment

Nickel-Catalyzed Regiodivergent Acylzincation of Styrenes with Organozincs and CO

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Chinese Journal of Chemistry 2024年第6期42卷 599-604页

作者： Chenglong Wang Ning Liu Xianqing Wu Jingping Qu Yifeng Chen Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237 China Dedicated to the Special Issue of C1 Chemistry.

Transition metal-catalyzed carbometallation of unsaturated hydrocarbons constitutes one of the most efficient synthetic methodologies for the construction of C—C ***,the incorporation of organometallic reagent with the CO gas as a nucleophilic acyl synthon could enable the acylmetallation reaction,which greatly increases the horizon of carbometallation ***,we report a nickel-catalyzed regiodivergent acylzincation of o-cyano cinnamate ester and o-cyano styrene,in which the cyano moiety intramolecularly captures zinc intermediates to trigger the tandem cyclization *** protocol features mild conditions,broad substrate scope and excellent functional group tolerance,thus affording a diverse array of highly functionalized carbocyclic compounds.

关键词： Carbonylation Carbometallation Styrene Nickel Cyclization

β-Receptor blocker enhances the anabolic effect of PTH after osteoporotic fracture

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Bone research 2024年第2期12卷 302-313页

作者： Jie Huang Tong Wu Yi-Rong Jiang Xuan-Qi Zheng Huan Wang Hao Liu Hong Wang Hui-Jie Leng Dong-Wei Fan Wan-Qiong Yuan Chun-Li Song Department of Orthopedics Peking University Third Hospital100191 BeijingChina Beijing Key Laboratory of Spinal Disease 100191 BeijingChina Engineering research center of Bone and joint precision medicine 100191 BeijingChina

The autonomic nervous system plays a crucial role in regulating bone metabolism,with sympathetic activation stimulating bone resorption and inhibiting bone *** found that fractures lead to increased sympathetic tone,enhanced osteoclast resorption,decreased osteoblast formation,and thus hastened systemic bone loss in ovariectomized(OVX)***,the combined administration of parathyroid hormone(PTH)and theβ-receptor blocker propranolol dramatically promoted systemic bone formation and osteoporotic fracture healing in OVX *** effect of this treatment is superior to that of treatment with PTH or propranolol *** vitro,the sympathetic neurotransmitter norepinephrine(NE)suppressed PTH-induced osteoblast differentiation and mineralization,which was rescued by ***,NE decreased the PTH-induced expression of Runx2 but enhanced the expression of Rankl and the effect of PTH-stimulated osteoblasts on osteoclastic differentiation,whereas these effects were reversed by ***,PTH increased the expression of the circadian clock gene Bmal1,which was inhibited by NE-βAR ***1 knockdown blocked the rescue effect of propranolol on the NE-induced decrease in PTHstimulated osteoblast *** together,these results suggest that propranolol enhances the anabolic effect of PTH in preventing systemic bone loss following osteoporotic fracture by blocking the negative effects of sympathetic signaling on PTH anabolism.

关键词： blocker metabolism inhibited

EBSD analysis of grain boundary evolution and dynamic recrystallization of Inconel 625 superalloy at various hot spinning feed rates

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Progress in Natural Science:Materials international 2024年第1期34卷 56-65页

作者： Zhanjie Jing Jiangkun Fan Xudong Liu Yuelin Song Zixiao Wang Kai Cao Yuetan Chen Heng Fu Jianing Zhang Jinshan Li State Key Laboratory of Solidification Processing Northwestern Polytechnical University Chongqing Innovation center Northwestern Polytechnical University National&Local joint Engineering research center for precision Thermoforming Technology of Advanced Metal Materials

Hot spinning can make the material withstand shear stress, so that the shape of the material has a great change,which is one of the main processing methods of nickel-based alloy plate members. Inconel 625 alloy, which has excellent high temperature mechanical properties and can be used as the main candidate material for aerospace applications, needs further study on its hot spinning deformation behavior and deformation mechanism. In this paper, the effect of feed rate on the microstructure evolution of Inconel 625 superalloy was studied by the electron backscattered diffraction technology. The microstructure with necklace-like structures composed of dynamic recrystallization(DRX) grains was observed after hot spinning. It was found that at the low feed rate, the promotion of DRX degree and grain refinement happened, where the grain size reached the trough of 10.99 μm under a feed rate of 300 mm/min. However, with the further feed rate rising, the degree of DRX was suppressed to a certain extent and grain size increased to 14.26 μm. On balance, the feed rate of 300 mm/min was the most efficient condition for grain refinement. Besides, it was revealed that both discontinuous dynamic recrystallization(DDRX) and continuous dynamic recrystallization(CDRX) occurred during hot spinning. DDRX includes the initial grain boundary nucleation by bulging and the annealing twin boundary assisted nucleation, while the CDRX mechanism is related to the continuous subgrain rotation within the deformed grain. DDRX is the main DRX mechanism.

关键词： Inconel 625 superalloy Hot spinning Grain boundary evolution DRX mechanism

Remote copper-catalyzed enantioselective substitution of yne-thiophene carbonates

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Science China Chemistry 2024年第4期67卷 1175-1180页

作者： Hao-Dong Qian Xiang Li Tingrui Yin Wei-Feng Qian Chunhui Zhao Cuiju Zhu Hao Xu CCNU-uOttawa joint research Centre Key Laboratory of Pesticides&Chemical Biology of Ministry of EducationInternational Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China

Here,we describe a strategy for the copper-catalyzed asymmetric heteroarylation of yne-thiophene carbonates with indoles via remote *** key to the success of this strategy lies in the design of the alkynyl group at the ortho-position of the heterocycle thiophene,enabling the formation of a triarylmethane moiety via very remote ***,the concept of remote copper-catalyzed asymmetric transformation extends not only to yne-allylic esters but also to yne-aryl *** reaction readily provides a diverse array of chiral triarylmethanes with high efficiency,enantioselectivity,and excellent functional group ***,facile follow-up transformations underscore their potential utility in the synthesis of various enantioenriched building *** mechanistic studies support the plausibility of the remote substitution pathway.

关键词： remote substitution copper catalyst asymmetric catalysis triaryl methanes

Electrically Driven Nonresonant Single Molecular Switches

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CCS Chemistry 2024年第2期6卷 465-472页

作者： Rui Wang Ajun Tang Zhi Li Yunpeng Li Dahui Qu Hongxiang Li Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237

Electrical switching of a single-molecule junction provides a practical module to perform sophisticated operations in electronic ***,designing an all-electrically-driven molecular switch is a great ***,we experimentally and theoretically investigated the charge transport characteristics of isoindigo(ISO)-molecules at the single-molecule level using the scanning tunneling microscope break junction *** find that the single-molecule junctions of ISO-molecules display bias voltage-driven switching *** switches are realtime,reversible,and nondestructive under low-bias *** results show that the mechanism of the switch is not the transition from nonresonant charge transport to resonant charge transport,but it is the shift of the frontier orbital energy levels of ISO-molecules and the change of the interfacial electronic coupling with bias *** results will advance the design of high-performance bias voltage-driven molecular switches.

关键词： single-molecule junction isoindigo molecular switch bias voltage nonresonant charge transport molecular electronics

Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

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Science China Chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao Yujian Liu Guogang Liu Jinquan Chen Wei Jiang Zhigang Shuai Da-Hui Qu Zhaohui Wang Key Laboratory for Advanced Materials and joint international research Laboratory of precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State Key Laboratory of precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live ***,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap ***,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 10 *** our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(128,200 cm^(-1)mol^(-1)L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently *** femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI *** calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)*** chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence