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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

National Science Review 2024年第2期11卷 155-167页

作者： Peng He Meng-Yang Hu Jin-Hong Li Tian-Zhang Qiao Yi-Lin Lu Shou-Fei Zhu Frontiers Science center for New organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Entropy variances of pure coherent states in the diffusion channel

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Chinese Physics B 2024年第9期33卷 384-388页

作者： Wei-Feng Wu Yong Fang Peng Fu School of Mechanical and Electrical Engineering Chizhou UniversityChizhou 247000China Anhui research center of semiconductor Industry Generic Technology Chizhou 247000China

Using the operator correspondence of the real and fictious modes in the thermo entangled state representation, wesolve the quantum master equation describing the diffusion channel and obtain the Kraus operator-sum representation ofits analytical solution. we find that the pure coherent states evolve into the new mixed thermal superposed states in thediffusion channel. Also, we investigate the statistical properties of the initial coherent states and their entropy evolutions inthe diffusion channel, and find that the entropy evolutions are only related to the decay time and without the amplitudes ofthe initial coherent states.

关键词： entangled state representation diffusion channel coherent state entropy evolution

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Investigation of operation and degradation mechanisms in ZnTeSe blue quantum-dot light-emitting diodes by identifying recombination zone

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Nano research 2024年第7期17卷 6527-6533页

作者： Oul Cho Sujin Park Hogeun Chang Jiwhan Kim Jaekwon Kim Sungwoo Kim Taehyung Kim Jeonghun Kwak Department of Electrical and Computer Engineering Inter-university Semiconductor Research Centerand Soft Foundry InstituteSeoul National UniversitySeoul 08826Republic of Korea Material research center Samsung Advanced Institute of TechnologySuwonGyeonggi-do 16419Republic of Korea

ZnTeSe quantum dots(QDs),recognized as promising eco-friendly blue electroluminescent emitters,remain under-explored in light-emitting diode(LED)***,to elucidate the operation and degradation mechanisms of ZnTeSe blue QD-LEDs,stacked ZnTeSe QD layers with discernable luminescence are designed by varying Te doping concentrations,and the recombination zones(RZs)of the blue QD-LEDs are *** RZs are identified near the hole-transport layer(HTL),confirmed by angular-dependent electroluminescence measurements and optical *** addition,in order to investigate carrier dynamics in the process of recombination,the transient electroluminescence(tr-EL)signals of the dichromatic QD-LEDs are *** a result,it is inferred that the RZ initially formed near the electron-transport layer(ETL)due to the high injection barriers of ***,due to the fast electron mobility,the RZ shifts toward the HTL as the operating current *** the device lifetime tests,the RZ remains stationary while the photoluminescence(PL)corresponding to the RZ undergoes a substantial decrease,indicating that the degradation is accelerated by the concentrated *** this study contributes to a deeper understanding of the operational mechanisms of ZnTeSe blue QD-LEDs.

关键词： quantum dots light-emitting diodes degradation recombination zones carrier dynamics

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Azocalixarenes: a scaffold of universal excipients with high efficiency

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Science China Chemistry 2024年第5期67卷 1697-1706页

作者： Yu-Xin Yue Yi-Lin Lin Meng-Meng Chen Han-Wen Tian Rong Ma Ze-Han Wang Fang-Yuan Chen Yu-Chen Pan Dong-Sheng Guo College of Chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Functional Polymer Materials(Ministry of Education)Frontiers Science Center for New Organic MatterCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin 300071China

Excipients are important components of pharmaceutical preparations that affect their quality, safety, and efficacy. Macrocyclic receptors are a family of supramolecular excipients with several advantages, including molecular-level protection, small sizes,fast kinetics of host-guest recognition, and modular construction. With the continuous advances in the medical field, personalized and precision medicine requires the development of excipients with low dosages, integrated modifying effects, universality,and controlled release. To meet these requirements, we have developed a new family of macrocyclic excipients based on calixarenes by integrating their covalent(broad chemical design space) and noncovalent(wide range of substrates) ***, azocalixarenes(Azo CAs) were designed, showing high binding affinities to a broad spectrum of active pharmaceutical ingredients(APIs), selectivity to interferents, and responsiveness to hypoxic microenvironments. Due to their highly efficient and controllable recognition, Azo CAs serve as low-dose excipients for 30 APIs. Molecular encapsulation by Azo CAs results in the integrated modification of the physicochemical properties of APIs, including solubility, stability, bioavailability,and biocompatibility. Moreover, Azo CAs can be reduced by azoreductases overexpressed in hypoxic microenvironments,leading to the controlled release of APIs. Collectively, Azo CA excipients have broad application prospects for a series of diseases such as enteritis, arthritis, stroke, cancer, bacterial infection and kidney injury, with diverse therapeutic modalities,including chemotherapy, photodynamic therapy, photothermal therapy, immunotherapy, boron neutron capture therapy, radiotherapy, fluorescence imaging, and their combinations.

关键词： supramolecular chemistry host-guest systems excipient calixarene molecular recognition

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Core-Shell semiconductor-Graphene Nanoarchitectures for Efficient Photocatalysis:State of the Art and Perspectives

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Nano-Micro Letters 2024年第12期16卷 553-588页

作者： Jinshen Lan Shanzhi Qu Xiaofang Ye Yifan Zheng Mengwei Ma Shengshi Guo Shengli Huang Shuping Li Junyong Kang Engineering research center of Micro-Nano Optoelectronic Materials and Devices Ministry of EducationFujian Key Laboratory of Semiconductor Materials and ApplicationsCI Center for OSEDDepartment of PhysicsXiamen UniversityXiamen 361005People’s Republic of China

semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and structural stability that limit the *** core-shell semiconductorgraphene(CSSG)nanoarchitectures may address these issues due to their unique structures with exceptional physical and chemical *** review explores recent advances of the CSSG nanoarchitectures in the photocatalytic *** starts with the classification of the CSSG nanoarchitectures by the ***,the construction methods under internal and external driving forces were introduced and compared with each ***,the physicochemical properties and photocatalytic applications of these nanoarchitectures were discussed,with a focus on their role in *** ends with a summary and some perspectives on future development of the CSSG nanoarchitectures toward highly efficient photocatalysts with extensive *** harnessing the synergistic capabilities of the CSSG architectures,we aim to address pressing environmental and energy challenges and drive scientific progress in these fields.

关键词： Core-shell semiconductor-graphene Nanoarchitecture Photocatalysis Driving force Interface

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Selective nickel-electrocatalyzed benzylic C-H oxygenation of functionalized alkyl arenes

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Chinese Chemical Letters 2024年第2期35卷 396-401页

作者： Shunyao Tang Siyi Wang Dongmei Zhang Xinxing Zhang Guang Yang Yanwei Wang Youai Qiu State Key Laboratory of Elemento-organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China College of Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (RECAST)Frontiers Science Center for New Organic MatterNankai UniversityTianjin 300071China

Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities,such as free carboxylic acid, aldehyde, halogen(including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp^(3))–H bonds,and short-lived reactive intermediates(aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode(BUME) with nano-electrospray ionization mass spectrometry.

关键词： Electrochemical C-H oxidation Functionalized alkyl arenes Paired nickel-electrocatalysis H_(2)O oxidation Ketones

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Bacteriophages assisted bacteria to facilitate soil multifunctionality under organochlorine pesticide contamination

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Science China Technological Sciences 2024年第10期67卷 3116-3128页

作者： ZHAO DuoKai CHAO HuiZhen BALCAZAR Jose Luis WU ShiMao ZHENG XiaoXuan WU YunLing YUAN ShuJian SUN MingMing HU Feng Soil Ecology Lab Jiangsu Collaborative Innovation Center for Solid Organic Waste Resource Utilization and Jiangsu Key Laboratory for Solid Organic Waste UtilizationNanjing Agriculture University J.F.Blumenbach Institute of Zoology and Anthropology University of G?ttingen Catalan Institute for Water research (ICRA) University of Girona College of Environmental and Resource Sciences Zhejiang University

As the most abundant living entities in the environment, viruses have been well recognized as crucial members in sustaining biogeochemical cycling. However, the significance of viruses in soil ecosystem multifunctionality remains under-explored. In this study, we used metagenomics and meta-viromics analysis to investigate the role of soil viruses in soil ecosystem functions under heavy, light, and no organochlorine pesticides(OCPs) contamination. In the three types of soil samples collected, lightcontaminated soils supported the highest level of multifunctionality, followed by heavy-contaminated soils and clean ***, our results revealed a positive correlation between bacterial community evenness and multifunctionality index(p research could potentially translate phage communities and related ecological processes into artificial methods for application in soil pollution remediation or ecological restoration.

关键词： soil ecosystem multifunctionality viruses auxiliary metabolic genes organochlorine pesticides contamination

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Iridium-Catalyzed Asymmetric Hydrogenation of Dialkyl Imines

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CCS Chemistry 2024年第4期6卷 905-911页

作者： Zheng Wang Xin-Yi Yang Yue Xu Qi-Lin Zhou State Key Laboratory and Institute of Elemento-organic Chemistry College of ChemistryFrontiers Science Center for New Organic MatterNankai UniversityTianjin 300071

Asymmetric hydrogenation of dialkyl imines to chiral amines is difficult because the two alkyls of imines are so similar in spatial and electronic structure that chiral catalysts are difficult to distinguish between *** this study,we described an asymmetric hydrogenation of dialkyl imines by a chiral iridium catalyst containing spiro phosphine-amine-phosphine *** precisely adjusting the chiral pocket of catalyst,a highly efficient catalyst was *** this catalyst,a variety of dialkyl imines were hydrogenated to chiral amines with high yield and enantioselectivity.

关键词： spiro PNP ligand iridium catalyst enantioselective hydrogenation dialkyl imines chiral amines

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Complete kinetic model for esterification reaction of lauric acid with glycerol to synthesize glycerol monolaurate

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Chinese Journal of Chemical Engineering 2024年第6期70卷 211-221页

作者： Han-Qiao Hu Yue Zhang Ming Fan Yong Cai Guang-Wen Chu Liang-Liang Zhang research center of the Ministry of Education for High Gravity Engineering and Technology Beijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Petrochemical research Institute China National Petroleum CorporationBeijing 102206China

Glycerol monolaurate(GML)is a widely used industrial chemical with excellent emulsification and antibacterial *** direct esterification of glycerol with lauric acid is the main method to synthesize *** this work,the kinetic process of direct esterification was systematically studied using p-toluenesulfonic acid as catalyst.A complete kinetic model of consecutive esterification reaction has been established,and the kinetic equation of acid catalysis was *** isomerization reactions of GML and glycerol dilaurate were *** was found that the reaction was an equilibrium reaction and the reaction rate was faster than the esterification *** kinetic equations of the consecutive esterification reaction were obtained by experiments as k_(1)=(276+92261Xcat)exp(-37720/RT)and k_(2)=(80+4413Xcat)exp(-32240/RT).The kinetic results are beneficial to the optimization of operating conditions and reactor design in GML production process.

关键词： Glycerol monolaurate p-Toluenesulfonic acid Esterification Kinetics Mass transfer

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Recent Advances in Patterning Strategies for Full‑Color Perovskite Light‑Emitting Diodes

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Nano-Micro Letters 2024年第3期16卷 99-137页

作者： Gwang Heon Lee Kiwook Kim Yunho Kim Jiwoong Yang Moon Kee Choi Graduate School of semiconductor Materials and Devices Engineering Center for Future Semiconductor Technology(FUST)Ulsan National Institute of Science and Technology(UNIST)Ulsan 44919Republic of Korea Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology(DGIST)Daegu 42988Republic of Korea Energy Science and Engineering research center Daegu Gyeongbuk Institute of Science and Technology(DGIST)Daegu 42988Republic of Korea Department of Materials Science and Engineering Ulsan National Institute of Science and Technology(UNIST)Ulsan 44919Republic of Korea center for Nanoparticle research Institute for Basic Science(IBS)Seoul 08826Republic of Korea

Metal halide perovskites have emerged as promising light-emitting materials for next-generation displays owing to their remarkable material characteristics including broad color tunability,pure color emission with remarkably narrow bandwidths,high quantum yield,and solution *** recent advances have pushed the luminance efficiency of monochromic perovskite light-emitting diodes(PeLEDs)to their theoretical limits,their current fabrication using the spincoating process poses limitations for fabrication of full-color *** integrate PeLEDs into full-color display panels,it is crucial to pattern red–green–blue(RGB)perovskite pixels,while mitigating issues such as cross-contamination and reductions in luminous ***,we present state-of-the-art patterning technologies for the development of full-color ***,we highlight recent advances in the development of efficient ***,we discuss various patterning techniques of MPHs(i.e.,photolithography,inkjet printing,electron beam lithography and laserassisted lithography,electrohydrodynamic jet printing,thermal evaporation,and transfer printing)for fabrication of RGB pixelated *** patterning techniques can be classified into two distinct approaches:in situ crystallization patterning using perovskite precursors and patterning of colloidal perovskite *** review highlights advancements and limitations in patterning techniques for PeLEDs,paving the way for integrating PeLEDs into full-color panels.

关键词： Perovskite Light-emitting diode Full-color display High-resolution patterning Electroluminescence

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