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Amplifiable protein identification via residue-resolved barcoding and composition code counting

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National Science Review 2024年第7期11卷 205-217页

作者： Weiming Guo Yuan Liu Yu Han Huan Tang Xinyuan Fan Chu Wang Peng R.Chen Synthetic and Functional Biomolecules Center Beijing National Laboratory for Molecular SciencesKey Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University Peking-Tsinghua Center for Life Sciences Academy for Advanced Interdisciplinary Studies Peking University

Ultrasensitive protein identification is of paramount importance in basic research and clinical diagnostics but remains extremely challenging. A key bottleneck in preventing single-molecule protein sequencing is that, unlike the revolutionary nucleic acid sequencing methods that rely on the polymerase chain reaction(PCR) to amplify DNA and RNA molecules, protein molecules cannot be directly amplified. Decoding the proteins via amplification of certain fingerprints rather than the intact protein sequence thus represents an appealing alternative choice to address this formidable challenge. Herein, we report a proof-of-concept method that relies on residue-resolved DNA barcoding and composition code counting for amplifiable protein fingerprinting(AmproCode). In AmproCode, selective types of residues on peptides or proteins are chemically labeled with a DNA barcode, which can be amplified and quantified via quantitative PCR. The operation generates a relative ratio as the residue-resolved ‘composition code’ for each target protein that can be utilized as the fingerprint to determine its identity from the proteome database. We developed a database searching algorithm and applied it to assess the coverage of the whole proteome and secretome via computational simulations, proving the theoretical feasibility of AmproCode. We then designed the residue-specific DNA barcoding and amplification workflow, and identified different synthetic model peptides found in the secretome at as low as the fmol/L level for demonstration. These results build the foundation for an unprecedented amplifiable protein fingerprinting method. We believe that, in the future,AmproCode could ultimately realize single-molecule amplifiable identification of trace complex samples without further purification, and it may open a new avenue in the development of next-generation protein sequencing techniques.

关键词： protein identification amplifiable fingerprinting residue-specific chemistry DNA barcoding composition code counting

Nanomaterial Assisted Exosome Analysis Using Mass Spectrometry

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Chemical Research in Chinese Universities 2024年第2期40卷 237-254页

作者： ZHANG Yi ZHOU Bokai LI Qiuning JIN Mingshi BAI Yu Beijing National laboratory for molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871P.R.China Department of Chemistry Yanbian UniversityYanji133002P.R.China

Exosomes,extracellular vesicles(EVs)that play crucial roles in biological processes,have emerged as attractive targets for noninvasive disease diagnosis and *** spectrometry(MS)offers high sensitivity,high throughput,and excellent qualification and quantification capacity,which is the ideal approach for exosome ***’unique physiochemical properties,controllable morphology,and large surface area make them promising in biological sample pretreatment and *** contributed diverse functions to the exosome MS analysis,encompassing substrates for exosome isolation and cargos enrichment,matrices for laser desorption/ionization(LDI),read-out signals and supporters for signal amplification strategies,*** this review,recent progress in the applications of nanomaterial in the exosome MS analysis was summarized and a comprehensive discussion on the challenges and perspectives was proposed for the development of an advancing analysis approach of exosomes for the accurate diagnosis and monitoring of diseases.

关键词： Exosome Nanomaterial Enrichment Matrix Mass spectrometry

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

Synthesis and reactivity of cobalt dinitrogen complex supported by nonsymmetrical pincer ligand

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Chinese Chemical Letters 2024年第7期35卷 259-263页

作者： Yuanjin Chen Xianghui Shi Dajiang Huang Junnian Wei Zhenfeng Xi Beijing National laboratory for molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China State Key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryShanghai 200032China

A nonsymmetrical PNN pincer ligand[6-(^(t)Bu_(2)PNH)C_(5)H_(4)N-2-(3-Mes)C_(3)H_(2)N_(2)]and its corresponding cobalt-N_(2)complex were synthesized and *** the stoichiometric reaction of the PNN ligand lithium salt with CoCl_(2),the complex 3,(PNN)CoCl,was ***,reduction of 3 with NaBHEt3under a dinitrogen atmosphere yielded complex 5,(PNN)Co(Ⅰ)(η^(1)-N_(2)).Single-crystal X-ray analysis,IR spectrum,and DFT calculations revealed that the dinitrogen in 5 was only weakly reduced by the cobalt *** reactions of 5 with carbon monoxide and 2,6-dimethylphenyl isocyanide gave carbonyl and isocyanide complexes 6 and 7 with the release of N_(2),***,these cobalt complexes,especially complex 5,demonstrated the capacity to convert dinitrogen to N(TMS)_(3)with moderate efficiency.

关键词： Dinitrogen fixation Dinitrogen transformation Nonsymmetrical pincer ligand Cobalt complex Catalytic silylamine formation

Natural products inspired[3+2]cycloaddition enables efficient construction of hydroxylated tetrahydrofuran acetals and concise syntheses of lignans

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Science China Chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State Key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of Sciences Beijing 100049China Beijing National laboratory for molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom *** studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol *** the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and *** the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National Science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National laboratory for molecular Science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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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

Chiral electron transporting material for circularly polarized organic light-emitting diode

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Science China Chemistry 2024年第11期67卷 3777-3784页

作者： Peihao Huo Tianyu Yang Peiyu Fang Yujia Li Nanlong Zheng Min Gong Zuqiang Bian Zhiwei Liu Beijing National laboratory for molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular Engineering Peking University

Circularly polarized organic light-emitting diode(CP-OLED) has attracted increasing interest for its efficient ability to generate circularly polarized light directly. So far, many CP-OLEDs were successfully fabricated with chiral emitters or chiral hosts. In this study, a new strategy based on chiral electron transporting layer is proposed to construct CP-OLEDs. A pair of chiral electron transporting materials, 1,3,5-tris((R/S)-4-isopropyl-4,5-dihydrooxazol-2-yl)benzene((R/S)-TOxiPr), are firstly designed and synthesized. The crystalline films of(R/S)-TOxiPr show circularly polarized photoluminescence with photoluminescence dissymmetry factors of-0.067 and +0.041, respectively. The CP-OLEDs based on(R/S)-TOxiPr and three types of achiral emitters all exhibit circularly polarized electroluminescence, showing feasibility and strong versatility of this new strategy. The mechanism is attributed to in-situ electrical excitation instead of simply light filtering of non-circularly polarized light. This work demonstrates a new approach for realizing circularly polarized electroluminescence which may provide a valuable strategy to develop CP-OLEDs.

关键词： circularly polarized organic light-emitting diodes chiral electron transporting layer trisoxazolinylbenzene circularly polarized electroluminescence

Capturing metal clusters at the strong-interaction region to reverse Ostwald ripening

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Science China Materials 2024年第4期67卷 1363-1364页

作者： Shuheng Tian Ding Ma Beijing National laboratory for molecular Sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

High-temperature interactions induce sintering of metal nanoparticles(NPs) on heterogeneous catalyst surfaces, leading to reduced surface area and active site loss through Ostwald ripening [1]. This irreversible deactivation necessitates costly catalyst replacement, notably impacting metals like copper in hydrogenation and reforming reactions [2].

关键词： catalyst reforming irreversible