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Light/pH dual-responsive magnetic metal-organic frameworks composites for phosphorylated peptide enrichment

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Chinese Chemical Letters 2024年第7期35卷 222-226页

作者： Rui Wang He Qi Haijiao Zheng Qiong Jia College of Chemistry Jilin UniversityChangchun 130012China key laboratory for molecular enzymology and engineering of ministry of education School of Life SciencesJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological *** this study,we introduced a pyridinyl zwitterionic ligand with light/pH dual response into magnetic MOF composite(Fe_(3)O_(4)@ZW-MOF)for enrichment of phosphorylated peptides for the first *** introduction of the developed ligand gives MOF material dual response *** stimulation affects the generation/disappearance of free radicals of the pyridine derivative,resulting in a change in the charge gradient of the zwitterion,and zwitterion can also regulate the p H of the solution by adding acid or ***,the reversible capture and release of phosphorylated peptides can be easily achieved by adjusting light and *** established phosphorylated peptide enrichment platform exhibits high sensitivity(detection limit of 1 fmol),high selectivity(β-casein:BSA,1:1000),and good reusability(7 cycles).In addition,the method was applied to the enrichment of phosphorylated peptides in complex systems(non-fat milk and human serum),demonstrating the feasibility of this method for phosphoproteom *** conclusion,the synthesized Fe_(3)O_(4)@ZW-MOF is a promising MOF material,which provides the possibility to advance the application of responsive MOFs materials in proteomics.

关键词： Light pH Dual-response Metal-organic frameworks Phosphorylated peptide

Synthesis of uniform two-dimensional MoS_(2) films via thermal evaporation

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Nano Research 2024年第4期17卷 3217-3223页

作者： Xue-Wei Lu Zhewei Li Chen-Kai Yang Weijia Mou Liying Jiao key laboratory of Organic Optoelectronics and molecular engineering of the ministry of education Department of ChemistryTsinghua UniversityBeijing 100084China

Two-dimensional(2D)molybdenum disulfide(MoS_(2))holds great potential for various applications such as electronic devices,catalysis,lubrication,anti-corrosion and so *** evaporation is a versatile thin film deposition technique,however,the conventional thermal evaporation techniques face challenges in producing uniform thin films of MoS_(2) due to its high melting temperature of 1375℃.As a result,only thick and rough MoS_(2) films can be obtained using these *** address this issue,we have designed a vacuum thermal evaporation system specifically for large-scale preparation of MoS_(2) thin *** using K2MoS4 as the precursor,we achieved reliable deposition of uniform polycrystalline MoS_(2) thin films with a size of 50 mm×50 mm and controllable thickness ranging from 0.8 to 2.4 *** approach also allows for patterned deposition of MoS_(2) using shadow masks and sequential deposition of MoS_(2) and tungsten disulfide(WS_(2)),similar to conventional thermal evaporation ***,we have demonstrated the potential applications of the obtained MoS_(2) thin films in field effect transistors(FETs),memristors and electrocatalysts for hydrogen evolution reaction(HER).

关键词： thermal evaporation molybdenum disulfide two-dimensional memristors hydrogen evolution reaction

Thiazoloisoindigo-based Polymer Semiconductors: Synthesis,Structure-Property Relationship, Charge Carrier Polarity, and Field-Effect Transistor Performance

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Chinese Journal of Polymer Science 2024年第1期42卷 24-31,I0006页

作者： Bo-Wen Li Miao Xiong Mei-Hua Liu Zhi-Gao Li Long Sang Zi-Han Xiong Biao Xiao Jian Pei Xiao-Bo Wan key laboratory of Optoelectronic Chemical Materials and Devices Ministry of EducationSchoolofOptoelectronic Materials&TechnologyJianghan UniversityWuhan430056China Bejing National laboratoryfor molecular Sciences the Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Developing new polymeric semiconductors with excellent device performance is essential for organic electronics. Herein, we synthesized two new thiazoloisoindigo(Tz II)-based polymers, namely, P(Tz II-d Th-d Th) and P(Tz II-d Th-d Tz), by copolymerizing thiophene-flanked Tz II with bithiophene and bithiazole, respectively. Owing to the more electron-deficient nature of bithiazole than bithiophene, P(Tz II-d Th-d Tz)possesses deeper LUMO/HOMO levels of-3.45/-5.47 e V than P(Tz II-d Th-d Th)(-3.34/-5.32 e V). The organic field-effect transistor(OFET) devices based on P(Tz II-d Th-d Th) exhibited p-type behaviors with an average hole mobility value as high as 1.43 cm^(2)·V^(-1)·s^(-1), while P(Tz II-d Th-d Tz)showed typical ambipolar characteristics with average hole and electron mobilities of 0.38 and 0.56 cm^(2)·V^(-1)·s^(-1). In addition, we compared the performances of both polymers with other Tz II-based polymers reported in our previous work, and showed that the charge carrier polarity can be manipulated by adjusting the number of the thiophene units between the acceptor unit. As the increase of the number of thiophene rings,charge carrier polarity shifts from electron-dominated ambipolar transport to hole-dominated ambipolar transport and then to unipolar hole transport in OFETs, which provides an effective molecular design strategy for further optimization of polymer OFET performance.

关键词： Field-effect transistor Charge carrier polarity Thiazoloisoindigo

Polyelectrolyte Complexes and Coacervates Formed by De novo-Designed Peptides and Oligonucleotide

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Chinese Journal of Polymer Science 2024年第9期42卷 1333-1340,I0007页

作者： Tian-Hao Ren De-Hai Liang Beijing National laboratory for molecular Sciences Department of Polymer Science and Engineering and the Key Laboratory of Polymer Chemistry and Physics of the Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic *** the regulation mechanism is still a *** this work,we designed a series of peptides(XXLY)_(6)SSSGSS and studied their complexation and coacervation behavior with single-stranded ***“X”and“Y”are varied to combine known amounts of charged and non-charged amino acids,together with the introduction of secondary structures and pH *** show that the electrostatic interaction,which is described as charge density,controls both the strength of complexation and the degree of chain relaxation,and thus determines the growth and size of the *** hydrophobic interaction is prominent when the charges are ***,the secondary structures of peptides exhibit profound effect on the morphology of the phases,such as solid phase to liquid phase *** study gains insight into the phase separation under physiological *** is also helpful to create coacervates with desirable structures and functions.

关键词： Polyelectrolyte complex Coacervate Peptides Secondary structure Electrostatic interaction

Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu key laboratory of Organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China key laboratory of Organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for *** this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction ***3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 *** a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film ***3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer ***,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 *** work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor

“Three-in-one” strategy of trifluoromethyl regulated blood-brain barrier permeable fluorescent probe for peroxynitrite and antiepileptic evaluation of edaravone

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Chinese Chemical Letters 2024年第10期35卷 360-363页

作者： Lei Shen Hongmei Liu Ming Jin Jinchao Zhang Caixia Yin Shuxiang Wang Yutao Yang key laboratory of Medicinal Chemistry and molecular Diagnosis of the ministry of education Chemical Biology Key Laboratory of Hebei ProvinceState Key Laboratory of New Pharmaceutical Preparations and ExcipientsCollege of Chemistry and Materials ScienceHebei UniversityBaoding 071002China key laboratory of Chemical Biology and molecular engineering of ministry of education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China

Epilepsy,as a chronic neurological disease of the brain,is closely related to oxidative stress,and the peroxynitrite(ONOO-)significantly rise up in this ***,ONOO-is considered as a potential biomarker for early prediction of ***,some potential diagnostic reagents for epilepsy are hindered by the blood-brain barrier(BBB).Meanwhile,“drug repurposing”is attracting a growing ***(EDA),as a first-line drug in the clinical treatment of cerebral ischemia,plays antioxidant roles in scavenging free radicals,promising potential antiepileptic ***,it is imperative to develop fluorescent probes for monitoring ONOO-fluctuations in the epileptic ***,we proposed a novel fluorescent probe with the thiocarbonate as the promising recognition unit for ONOO-and dicyanoisophorone derivative as the ***,by the“three-in-one”strategy,the introduction of trifluoromethyl into DCI-ONOO-3 can extend the emission wavelength of the fluorophore,shorten the response and increase ***,DCI-ONOO-3 was used for monitoring ONOO-fluxes in brain of epileptic mice and evaluating the antiepileptic efficacy of *** opens up a new way for the design of BBB permeable fluorescent probes,and provides a convincing new method for the diagnosis and treatment of epilepsy.

关键词： Fluorescent probe Blood-brain barrier Peroxynitrite Epilepsy Drug repurposing

Comparison of Measurements for Enhanced Diffusion Problem in Chemical Reaction Systems

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Chinese Journal of Chemistry 2024年第14期42卷 1659-1664页

作者： Ah-Young Jee Ziyang Wen Huan Wang Beijing National laboratory for molecular Sciences College of Chemistry and Molecular EngineeringBeijing Key Laboratory of Polymer Chemistry&Physics of Ministry of EducationPeking UniversityBeijing100871 China

The problem of molecular diffusion in the soup of chemical reactions attracts mounting interest across fields ranging from chemistry to biophysics to material *** reactions involve bond breakup and formation,whose time scale is typically on the orders of fs to ps,while molecular diffusion occurs at time scales ofμs to *** two processes are often considered orthogonal,given the vastly different *** serial results show that the enzyme's diffusion is enhanced in a substrate-dependent manner,which was further extended to small molecule reaction systems,challenging this classical ***,the results from different groups using different techniques do not quantitatively agree,and a general mechanism is yet to be *** summarize experimental studies on diffusion problems and seek to reconcile the interpretation with understanding the limits of measurement tools and the chemical nature of reaction *** molecular diffusion in chemical reactions will provide fresh thoughts in designing chemical systems such as molecular machines that harvest work at the nanoscale in a controllable manner.

关键词： molecular diffusion Chemical reactions Enzyme reactions Active matter Diffusion measurements Single-molecule studies Fluorescence Time-resolved spectroscopy

Self-assembly Induced by Complexation of Diblock Copolyelectrolytes and Oppositely Charged Homopolymers

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Chinese Journal of Polymer Science 2024年第9期42卷 1321-1332,I0006页

作者： Ling Zhao Zhi-Yuan Yin Jia-Di Jiang Er-Qiang Chen Shuang Yang Beijing National laboratory for molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Mater Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Beijing National laboratory for molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

We investigate the solution self-assembly of a mixture of positively charged homopolymers and AB diblock copolymers,in which the A blocks are negatively charged,and the B blocks are *** electrostatic complexation between oppositely charged polymers drives the formation of many ordered *** microstructures and phase diagrams are calculated using self-consistent field theory(SCFT)based on an ion-pair model with an equilibrium constant K to characterize the strength of binding between positively and negatively charged *** effects of the charge ratio,representing the ratio of charges from the homopolymer over all charges from polymers in the system,on the ordered structure are systematically studied,both for hydrophobic and hydrophilic A *** charge ratio plays an important role in determining the phase boundaries in the phase diagram of salt concentration versus polymer *** also provide information about the varying tendency of the domain spacing and core size of the spherical phase when the charge ratio is changed,and the results are in good agreement with *** studies provide a deep understanding of the self-assembled microstructures of oppositely charged diblock copolymer-homopolymer systems.

关键词： Self-assembly Polyelectrolyte complexation Self-consistent field theory Ion-pair

Soil conditioning of clay based on interface adhesion mechanism:Microscopic simulation and laboratory experiment

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Underground Space 2024年第5期18卷 239-255页

作者： Yong Fang Bin Zhuo Ruyue Zhang Yubo Wang Liupan Dou Yuxiang Yao key laboratory of Transportation Tunnel engineering Ministry of EducationSouthwest Jiaotong UniversityChengdu 610031China

Clogging frequently occurs in the cutter head,excavation chamber or screw conveyor when an earth pressure balance(EPB)shield machine is tunneling in soft or silty clay ground with high clay mineral *** this paper,montmorillonite,kaolinite,and illite were selected as research objects,and molecular dynamics simulation and laboratory experiment were *** the microscopic scale,dynamic contact behavior and interfacial mechanical behavior of the interface between clay minerals and water/surfactant solution was simulated and the interfacial adhesion and conditioning mechanism between clay minerals and water/surfactant solution was ***,sodium dodecyl benzene sulfonate surfactant was selected as the main composition of the soil ***,the adhesion stress before and after soil conditioning and the contact angles between clay minerals and water/surfactant solution were tested and analyzed at the macroscopic *** result shows that the contact angle between droplet and clay mineral surface is an important parameter to characterize soil *** simulation rules of the microscopic contact angle are consistent with the experiment ***,the adsorption energy between microscopic substances is dominated by electrostatic force,which can reflect the adhesion stress between macroscopic *** adhesion stress can be effectively decreased by adding the surfactant to the soil conditioner.

关键词： EPB clogging Clay minerals Microscopic simulation Mechanism analysis laboratory experiment Adhesion stress