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Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of Materials Science and Engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic ***,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and *** enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional *** work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

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Function-reversible facets enabling SrTiO_(3)nanocrystals for improved photocatalytic hydrogen evolution

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Frontiers in Energy 2024年第1期18卷 101-109页

作者： Bin WANG Bei AN Xiaoqian LI Shaohua SHEN School of Physics Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter(Ministry of Education)Key Laboratory of Shaanxi for Advanced Materials and Mesoscopic PhysicsXi’an Jiaotong UniversityXi’an 710049China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China

It has been widely reported that,for faceted nanocrystals,the two adjacent facets with different band levels contribute to promoted charge separation,and provide active sites for photocatalytic reduction and oxidation reaction,*** such cases,only one family of facets can be used for photocatalytic hydrogen ***,by using SrTiO_(3)nanocrystals enclosed by{023}and{001}facets as a model photocatalyst,this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all *** photo-deposition experiment of CdS provided direct evidence to demonstrate that the{023}facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles,together with the{001}***,the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen,in contrast to those SrTiO_(3)nanocrystals with only{001}facets deposited by Pt nanoparticles via a photo-deposition method.

关键词： SrTiO_(3)nanocrystals crystal facets photocatalysis hydrogen evolution

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Early Growth Response Gene-1 Deficiency Interrupts TGFβ1 Signaling Activation and Aggravates Neurodegeneration in Experimental Autoimmune Encephalomyelitis Mice

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Neuroscience Bulletin 2024年第3期40卷 283-292页

作者： Yunyi Lan Xinyan Han Fei Huang Hailian Shi Hui Wu Liu Yang Zhibi Hu Xiaojun Wu shanghai key laboratory of Compound Chinese Medicines The Ministry of Education Key Laboratory for Standardization of Chinese MedicinesThe State Administration of TCM Key Laboratory for New Resources and Quality Evaluation of Chinese MedicineInstitute of Chinese Materia MedicaShanghai University of Traditional Chinese MedicineShanghai201203China Central laboratory Shuguang Hospital Affiliated to Shanghai University of Traditional Chinese MedicineShanghai200021China

Early growth response protein 1(Egr-1)triggers the transcription of many genes involved in cell growth,differentiation,synaptic plasticity,and ***,its mechanism in neuronal survival and degeneration is still poorly *** study demonstrated that Egr-1 was down-regulated at mRNA and protein levels in the central nervous system(CNS)of experimental autoimmune encephalomyelitis(EAE)***-1 knockout exacerbated EAE progression in mice,as shown by increased disease severity and incidence;it also aggravated neuronal apoptosis,which was associated with weakened activation of the BDNF/TGFβ1/MAPK/Akt signaling pathways in the CNS of EAE ***,Egr-1 siRNA promoted apoptosis but mitigated the activation of BDNF/TGFβ1/MAPK/Akt signaling in SH-SY5Y *** results revealed that Egr-1 is a crucial regulator of neuronal survival in EAE by regulating TGFβ1-mediated signaling activation,implicating the important role of Egr-1 in the pathogenesis of multiple sclerosis as a potential novel therapy target.

关键词： Early growth response protein 1 Transforming growth factor-beta 1 Multiple sclerosis Experimental autoimmune encephalomyelitis Neurodegeneration

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Multistep continuous flow synthesis of Erlotinib

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Chinese Chemical Letters 2024年第4期35卷 371-375页

作者： Hui Jin Qin Cai Peiwen Liu Yan Chen Derong Wang Weiping Zhu Yufang Xu Xuhong Qian State key laboratory of Bioreactor Engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China

Erlotinib is an orally administered, highly effective, specific epidermal growth factor receptor tyrosine kinase inhibitor, used to treat non-small cell lung cancer and pancreatic cancer. The traditional synthetic methods for Erlotinib exhibit long reaction time and safety concern. Herein, we describe a novel five-step route for the synthesis of Erlotinib in flow. These five steps comprise etherification, nitration, reduction,addition and cyclization reactions. All steps were optimized and converted to continuous flow process,which drastically reduces the reaction time and considerably improves the process safety as well as the total yield. Enabled by five continuous flow units, Erlotinib is efficiently afforded with an E-factor of 38,an overall yield of 83%, and a total residence time of 25.1 min. Majority steps in this process have been optimized for quantitative conversion, which offers the possibility of telescoping the entire process.

关键词： Erlotinib Continuous flow synthesis Microchannel flow reactor Process optimization Continuous nitration Continuous hydrogenation

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Suppression of multistep phase transitions of O3-type cathode for sodium-ion batteries

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Chinese Chemical Letters 2024年第5期35卷 453-458页

作者： Shengyu Zhao Qinhao Shi Wuliang Feng Yang Liu Xinxin Yang Xingli Zou Xionggang Lu Yufeng Zhao Institute for Sustainable Energy&College of Sciences Shanghai UniversityShanghai 200444China State key laboratory of Advanced Special Steel&shanghai key laboratory of Advanced Ferrometallurgy&School of Materials Science and Engineering Shanghai UniversityShanghai 200444China

O3-type layered oxide cathodes have been widely investigated due to their high reversible capacities and sufficient Na+***,such materials usually suffer from complex multistep phase transitions along with drastic volume changes,leading to the unsatisfied cycle ***,we report a Mg/Ti co-doped O3-type NaNi_(0.5)Mn_(0.5)O_(2),which can effectively suppress the complex multistep phase transition and realize a solid-solution reaction within a wide voltage *** is confirmed that,the Mg/Ti co-doping is beneficial to enhance the structural stability and integrity by absorbing micro-strain and ***,the as obtained sample delivers an outstanding cyclic performance(82.3%after 200 cycles at 1 C)in the voltage range of 2.0-4.0 V,and a high discharge capacity of 86.6 mAh/g after 100 cycles within the wide voltage range(2.0-4.5 V),which outperform the existing *** co-doping strategy offers new insights into high performance O3-type cathode for sodium ion batteries.

关键词： Sodium ion batteries Mg/Ti co-doping Phase transition Cyclic performance High voltage performance

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Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

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Science China Chemistry 2024年第6期67卷 2102-2110页

作者： Xiaoyu Ji Shuo Zhang Furong Yu Huidong Zhang Liqing Zhan Yue Hu Wei-Hong Zhu Yongzhen Wu key laboratory for Advanced Materials and Joint International Research laboratory of Precision Chemistry and Molecular Engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China School of Chemistry University of EdinburghKing’s BuildingsEdinburghEH93FJUK

Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low ***,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 ***,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and *** assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase *** energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 *** V_(OC)-deficit(<0.40 V)is the lowest value reported for *** work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.

关键词： cyanovinyl phosphonic acid energy level alignment hole-selective material open-circuit voltage wide-bandgap perovskite

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Recent Advances in Pd-Catalyzed Reactions Involving the “On-Water” Mechanism

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Chinese Journal of Chemistry 2024年第5期42卷 533-542页

作者： Dong Wei Guo-Qiang Lin State key laboratory of Systems Medicine for Cancer Shanghai Cancer InstituteShanghai Key Laboratory of Systems Regulation and Clinical Translation for CancerRen Ji HospitalShanghai Jiao Tong University School of MedicineShanghai200127 China State key laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032 China

As the chemical industry grapples with the need for more eco-friendly practices,the use of water as a reaction medium is gaining attraction in organic *** mini-review delves into Pd-catalyzed reactions that utilize the "on-water" mechanism,spanning from 2019 to late *** reactions are neatly categorized into several types: (A) Catalytic C—H activations,(B) Mizoroki- Heck-type reactions,(C) Suzuki-Miyaura reactions,and (D) Cyclization *** showcasing the potential of water as a sustainable reaction medium for organic transformations,these reactions leave no doubt about the importance of embracing eco-friendly practices in the chemical *** Scientists In 1980,a seminal work by Breslow et *** an acceleration of reaction rate in the Diels-Alder *** and co-workers noted a significant increase in the rate of the [2σ+2σ+2π] cycloaddition of quadricyclane and dimethyl azodicarboxylate (DMAD) when the reaction was conducted in water,as opposed to when it was carried out in organic *** term "on-water" was then coined to describe this *** strategy was further expanded to transition-metal catalyzed transformations by Ackermann in ***,Varma and Leazer disclosed a Pd-catalyzed Mizoroki-Heck type arylation of alkenes with diaryliodonium salts “on-water”.The enantioselective version of "on-water" process was not realized until 2014 by the Zhou *** on,the Schaub group described a Pd-catalyzed Suzuki–Miyaura coupling reaction of electron-poor aryl chlorides with water,using only 50 ppm of catalyst *** recently,Liu and Lin extended the "on-water" strategy to Pd-catalyzed double Mizoroki-Heck *** mini-review has focused on Pd-catalyzed reactions involving the “on-water” mechanism.

关键词： Pd-catalyzed “On-water” Green chemistry Aqueous reactions Mechanism Methodology and reactions Mizoroki-Heck reaction Cross-coupling

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Fluorogenic sensing of amorphous aggregates,amyloid fibers,and chaperone activity via a near-infrared aggregation-induced emission-active probe

Aggregate

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Aggregate 2024年第1期5卷 309-320页

作者： Wei He Yuanyuan Yang Yuhui Qian Zhuoyi Chen Yongxin Zheng Wenping Zhao Chenxu Yan Zhiqian Guo Shu Quan State key laboratory of Bioreactor Engineering Shanghai Collaborative Innovation Center for Biomanufacturing(SCICB)East China University of Science and TechnologyShanghaiChina key laboratory for Advanced Materials and Joint International Research laboratory of Precision Chemistry and Molecular Engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghaiChina shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism East China University of Science and TechnologyShanghaiChina

The presence of protein aggregates in numerous human diseases underscores the significance of detecting these aggregates to comprehend disease mechanisms and develop novel therapeutic approaches for combating these *** the development of various biosensors and fluorescent probes that selectively target amyloid fibers or amorphous aggregates,there is still a lack of tools capable of simultaneously detecting both types of ***,we demonstrate the quantitative discernment of amorphous aggregates by QM-FN-SO3,an aggregationinduced emission(AIE)probe initially designed for detecting amyloid *** probe easily penetrates the membranes of the widely-used prokaryotic model organism Escherichia coli,enabling the visualization of both amorphous aggregates and amyloid fibers through near-infrared ***,the probe exhibits sensitivity in distinguishing the varying aggregation propensities of proteins,regardless of whether they form amorphous aggregates or amyloid fibers in *** properties contribute to the successful application of the QM-FN-SO3 probe in the subsequent investigation of the antiaggregation activities of two outer membrane protein(OMP)chaperones,both in vitro and in their physiological ***,our work introduces a near-infrared fluorescent chemical probe that can quantitatively detect amyloid fibers and amorphous aggregates with high sensitivity in vitro and in ***,it demonstrates the applicability of the probe in chaperone biology and its potential as a high-throughput screening tool for protein aggregation inhibitors and folding factors.

关键词： aggregation-induced emission fluorescence molecular chaperone protein aggregation

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A novel domain decomposition-based model for efficient dynamic predictions of large composite machine tools

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Science China(Technological Sciences) 2024年第6期67卷 1765-1782页

作者： YU YangBo JI Yu Lei CHEN YanRen XU Kun BI QingZhen State key laboratory of Mechanical System and Vibration School of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai200240China

We propose a large combined moving component composed of carbon fiber reinforced polymer(CFRP)laminates for making lightweight machine tools with high dynamic *** accurate dynamic prediction of composite machine tools is essential for the new generation machine *** paper aims to address two challenges in numerical dynamic modeling and the design of composite machine tools to enhance development efficiency.(1)Anisotropic composite laminates,which form the composite machine tool,exhibit coupling in various *** propose the generalized continuity condition of the boundary to tackle this dynamic modeling challenge.(2)Composite machine tools feature numerous composite-metal coupled *** mechanical model correction of isotropic metals is performed to address their *** take the example of a five-axis gantry machine tool with composite moving parts,establish a dynamic model for efficient prediction,and verify it through simulation and *** proposed method yields remarkable results,with an average relative error of only 3.85%in modal frequency prediction and a staggering 99.7%reduction in solution time compared to finite element *** further discuss the dynamic performance of the machine tool under varied stacking angles and layer numbers of the composite machine *** propose general design criteria for composite machine tools to consider the modal frequency and manufacturing cost of machine tools.

关键词： machine tool dynamics carbon fiber reinforced polymer composite laminates

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Application of total keratometry in ten intraocular lens power calculation formulas in highly myopic eyes

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Eye and Vision 2024年第2期10卷 22-30页

作者： Ling Wei Kaiwen Cheng Wenwen He Xiangjia Zhu Yi Lu Department of Ophthalmology and Eye Institute Eye and ENT Hospital of Fudan UniversityShanghai 200031China key laboratory of Myopia(Fudan University)key laboratory of Myopiashanghai key laboratory of Visual Impairment and Restoration National Health CommissionChinese Academy of Medical ScienceShanghai 200031China State key laboratory of Medical Neurobiology Fudan UniversityShanghai 200031China

Background:The accuracy of using total keratometry(TK)value in recent IOL power calculation formulas in highly myopic eyes remained ***:Highly myopic patients who underwent uneventful cataract surgery were prospectively enrolled in this prospective comparative *** one month postoperatively,standard deviation(SD)of the prediction errors(PEs),mean and median absolute error(MedAE)of 103 highly myopic eyes were back-calculated and compared among ten formulas,including XGboost,RBF 3.0,Kane,Barrett Universal II,Emmetropia Verifying Optical 2.0,Cooke K6,Haigis,SRK/T,and Wang-Koch modifications of Haigis and SRK/T formulas,using either TK or standard keratometry(K)***:In highly myopic eyes,despite good agreement between TK and K(P>0.05),larger differences between the two were associated with smaller central corneal thickness(P0.05),which both presented smaller MedAEs than others(all P0.05),and statistically larger percentages than the other eight formulas(P<0.05).Conclusions:Highly myopic eyes with thinner corneas tend to have larger differences between TK and *** XGboost enhancement calculator and RBF 3.0 formula using TK showed the most promising outcomes in highly myopic eyes.

关键词： High myopia Total keratometry Cataract surgery IOL power calculation

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