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living/controlled polymerization of vinylpyridines into sequence-regulated copolymers by Lewis pair

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Science China Chemistry 2024年第8期67卷 2737-2746页

作者： Qiankun Ding Wuchao Zhao Fukuan li Jianghua he Yuetao zhang Department of State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China

The poly(vinylpyridine)(PVP) based(co)polymers are of particular interest in materials science, due to their multifunctionality and diverse applications. So far, there is no report on the sequence-regulated copolymerization of vinylpyridines(VPs) and methacrylate monomer in one-step manner yet. here we designed and synthesized a series of guanidine phosphines as Lewis base(LB), which is combined with bulky organoaluminium to construct Lewis pairs(LPs) for polymerization of VPs. The living/controlled polymerization of 4-vinylpyridine(4-VP) or 2-vinylpyridine(2-VP) can be accomplished with remarkable efficiency by such Lewis pair polymerization(LPP), furnishing polymers with high molecular weight(up to 288 kg/mol) and narrow molecular weight distribution(as low as 1.17). Mechanistic studies reveal the interaction of LPs and formation of zwitterionic intermediates, providing solid evidences to support the proposed polymerization mechanism. More importantly, by simply adjusting the LA dosage, this LPP strategy realizes the unprecedented control over the sequence regulation of 2-VP-based copolymers from gradient to block in one-step manner, regardless of the monomer ratio, which greatly expands the versatility of the LPP.

关键词： guanidine phosphine Lewis pair polymerization living/controlled polymerization vinyl pyridine sequence regulation

A novel method for the synthesis of sulfur substituted-cyclopyrophosphate of cADPR analogs

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Chinese Chemical Letters 2014年第12期25卷 1583-1585页

作者： Ren-Min Wu Na Qi Yu-Wen Jia Zhu Guan liang-Ren zhang li-he zhang Zhen-Jun Yang State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking University

A facile and efficient protocol for the synthesis of sulfur substituted-cyclopyrophosphate of cIDPRE（P_S^1-cIDPRE） was *** key step was the cyclization process which was completed by the sulfur substituted cyclizati... 详细信息

关键词： cADPR cIDPRE Phosphoramidite strategy Cyclopyrophosphate

Unlock the full potential of carbon cloth-based scaffolds towards magnesium metal storage via regulation on magnesiophilicity and surface geometric structure

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Journal of Energy Chemistry 2024年第3期90卷 423-434,I0010页

作者： Jing liu Min Wang Zhonghua zhang Jinlei zhang Yitao he Zhenfang Zhou Guicun li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Department of Pharmacy Jining Medical UniversityRizhao 276826ShandongChina Department of Energy and Power Engineering School of Energy and EnvironmentAnhui University of TechnologyMa’anshan 243000AnhuiChina

The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal ***,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of *** this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon *** revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of *** fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also *** a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best ***,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous *** work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.

关键词： Magnesium metal anodes Electrodeposition heterogeneous nucleation

Hydrogen evolution reaction activity enhancement from active site turnover mechanism

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Journal of Energy Chemistry 2024年第5期92卷 629-638页

作者： Jiacheng Wang Tongqing Yang Xiyue li Haiqin zhang Yixue zhang Yan he Hongyao Xue College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061ShandongChina

Although heteroatom doping is an effective way to improve the catalytic activity of transition metal phosphides(TMPs),the mechanism of activity enhancement needs to be further *** this end,we synthesized a Co-doped Ni_(2)P catalyst as a research model and found that the introduction of heterogeneous Co reconstructed the charge distribution around the P site,which effectively enhanced the hydrogen evolution reaction(heR)activity of the pure Ni_(2)*** on in-situ Raman real-time monitoring technology,we monitored for the first time that Co doping triggered a switch of the active site(from the original Co-active site to the P-active site),which promoted the adsorption of H_(2)O to enhance the heR *** density functional theory(DFT)calculations indicated that the P site of Co-Ni_(2)P expressed the highest activity and the Ni site of pure Ni_(2)P expressed the highest activity,which further confirms the in-situ Raman monitoring *** active site turnover mechanism discovered in this study will undoubtedly provide more rational and targeted ideas for future catalyst design.

关键词： In-situ Raman observation heteroatom doping Activesites turnover Hydrogen production

Real-time identification of multiple nanoclusters with a protein nanopore in single-cluster level

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Nano Research 2024年第1期17卷 262-269页

作者： ling zhang Peilei he Huang Chen Qingda liu libo li Xun Wang Jinghong li Department of Chemistry Center for BioAnalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry&Chemical BiologyTsinghua UniversityBeijing 100084China School of Chemistry and Chemical Engineering Guangdong Prov Key Lab Green Chem Prod TechnolSouth China University of TechnologyGuangzhou 510640China New Cornerstone Science Laboratory Shenzhen 518054China Beijing Institute of life Science and Technology Beijing 102206China Center for BioAnalytical Chemistry Hefei National Laboratory of Physical Science at MicroscaleUniversity of Science and Technology of ChinaHefei 230026China

It is important and challenging to analyze nanocluster structure with atomic ***,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their *** such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be *** nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and ***,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with *** nanopore platform provides a novel powerful tool for nanocluster characterization.

关键词： nanopore single-molecule nanocluster polyoxometalates real-time detection

Ordered mesoporous materials for water pollution treatment: Adsorption and catalysis

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Green Energy & Environment 2024年第8期9卷 1239-1256页

作者： Peng zhang Mingming he Wei Teng Fukuan li Xinyuan Qiu Kexun li Hao Wang College of Environmental Science and Engineering MOE Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution TreatmentTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai University Department of Chemistry and State Key Laboratory Marine Pollution Hong Kong Institute for Advanced Study City University of Hong Kong State Key Laboratory for Pollution Treatment College of Environmental Science and EngineeringShanghai Institute of Pollution Treatment and Ecological SecurityTongji University State Key Laboratory of Simulation and Regulation of Water Cycles in River Basins China Institute of Water Resources and Hydropower Research

To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is *** mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore *** properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and *** this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals (Hg2+,Pb2+,Cd2+,Cr6+,etc.),toxic anions （nitrate,phosphate,fluoride,etc.）,and organic contaminants （organic dyes,antibiotics,etc.）.These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active ***,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are *** work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.

关键词： Water pollution treatment Ordered mesoporous materials Toxic contaminants Adsorption Catalysis

In-situ construction of abundant active centers on hierarchically porous carbon electrode toward high-performance phosphate electrosorption: Synergistic effect of electric field and capture sites

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Green Energy & Environment 2024年第1期9卷 126-137页

作者： Peng zhang Fukuan li Mingming he Silu Huo Xueli zhang Benqiang Cen Dezhi Fang Kexun li Hao Wang College of Environmental Science and Engineering Nankai UniversityTianjin300350China MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai UniversityTianjin300350China State Key Laboratory of Simulation and Regulation of Water Cycles in River Basins China Institute of Water Resources and Hydropower ResearchBeijing100038China

Phosphate removal is crucial for eutrophication control and water quality ***-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater ***,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and ***,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally *** resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron *** LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing *** superior phosphate removal performance originates from abundant active centers formed by the coupling of electricﬁeld and capture ***,the stability and selectivity toward phosphate capture were maintained well even under comprehensive ***,a series of kinetics and isotherms models were employed to validate the electrosorption *** work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.

关键词： Electro-assisted adsorption Electrosorption Phosphate removal Active centers MOF-derived carbon

Food-derived protein hydrolysates and peptides:anxiolytic and antidepressant activities,characteristics,and mechanisms

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Food Science and Human Wellness 2024年第3期13卷 1168-1185页

作者： Wenhui li Yu Xi Junru Wang Yinxiao zhang he li Xinqi liu Beijing Advanced Innovation Center for Food Nutrition and Human health Beijing Engineering and Technology Research Center of Food AdditivesNational Soybean Processing Industry Technology Innovation CenterBeijing Technology and Business UniversityBeijing 100048China

Globally,the prevalence of anxiety and depression has reached epidemic ***-derived protein hydrolysates and peptides delivered through dietary supplementation can avoid the negative risks associated with traditional pharmaceuticals while delivering superior anxiolytic and antidepressant *** review summarizes current research on food-derived anxiolytic and antidepressant protein hydrolysates and peptides,and subsequently analyses their physicochemical characteristics and elaborates on their *** aim of this work is to contribute to the in-depth study and provide a theoretical foundation for the development of related products to better serve patients with anxiety and depression.

关键词： Anxiolytic Antidepressant Peptides Protein hydrolysates Neurotransmitter

Coupling Reaction of 4-Chloro-7-H-Pyrrolo[2,3-d]Pyrimidine with 2,3,5-Tri-O-Acetyl-b-D-Ribofuranosyl Chloride

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Chinese Chemical Letters 2001年第5期12卷 391-394页

作者： Yun Long zhang liang Ren zhang Zhen Jun YANG Ji Mei MIN li he zhang Yang LU Ning Bo GONG Qi Tai ZheNG National Research Laboratory of Natural and Biomimetic Drugs Peking UniversityBeijing 100083 Institue of Materia Medica Chinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100050

Coupling reaction of 4-chloro-7-H-pyrrolo[2,3-d]pyrimidine with 2,3,5-tri-O-acetyl -β-D-ribofuranosyl chloride under the basic condition was investigated. An abnormal coupling reaction, in which the heterocyclic base attacked at the carbon of 1,2-O-methylidene moiety instead of anomeric carbon of ribose was observed and the structure of products 5a, 5b were identified by NMR and X-Ray diffraction.

关键词： Chloropyrrolo[2 3-d]pyrimidine 1-chloro-2 3 5-tri-O-acetyl-D-ribofuranose neigh-boring participation effect X-ray diffraction.