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Journal of Materials Science & Technology 2024年第1期168卷 103-113页

作者： Ghufran Aulia Bin Azizar Jong Wook Hong department of chemistry University of UlsanUlsan 44610Korea

The visible-light-driven hydrogen evolution is extremely important,but the poor charge transfer capa-bility,a sluggish evolution rate of hydrogen,and severe photo-corrosion make photocatalytic hydrogen evolution *** this study,we present 1D/2D ReS_(2)-CdS hybrid nanorods for photocatalytic hy-drogen evolution,comprised of a ReS_(2)nanosheet layer grown on CdS *** found that precise control of the contents of the ReS_(2)nanosheet layer allows for manipulating the electronic structure of Re in the ReS_(2)-CdS hybrid *** ReS_(2)-CdS hybrid nanorods with optimal ReS_(2)nanosheet layer content dramatically improve photocatalytic hydrogen evolution ***,photocatalytic hydro-gen evolution activity(64.93 mmol g^(−1)h^(−1))of ReS_(2)-CdS hybrid nanorods with ReS_(2)nanosheet layers(Re/Cd atomic ratio of 0.051)is approximately 136 times higher than that of pure CdS nanorods under visible light ***,intimated coupling of the ReS_(2)nanosheet layer with CdS nanorods reduced the surface trap-site of the CdS nanorods,resulting in enhanced photocatalytic *** de-tailed optical and electrical investigations demonstrate that the optimal ReS_(2)nanosheet layer contents in the ReS_(2)-CdS hybrid nanorods can provide improved charge transfer capability,catalytic activity,and light absorption *** study sheds light on the development of photocatalysts for highly efficient photocatalytic hydrogen evolution.

关键词： Photocatalyst Hydrogen evolution reaction ReS_(2)-CdS heterostructure Control of ReS_(2)nanosheet layer growth Optimization of cocatalyst activity and light absorption

The reformation of catalyst:From a trial-and-error synthesis to rational design

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Nano Research 2024年第4期17卷 3261-3301页

作者： Ligang Wang Jiabin Wu Shunwu Wang Huan Liu Yao Wang Dingsheng Wang department of chemistry Tsinghua UniversityBeijing 100084China

The appropriate catalysts can accelerate the reaction rate and effectively boost the efficient conversion of various molecules,which is of great importance in the study of chemistry,chemical industry,energy,materials and environmental ***,efficient,environmentally friendly,and easy to operate synthesis methods have been used to prepare various types of *** previous studies have reported the synthesis and characterization of the aforementioned catalysts,more still remain in trial and error methods,without in-depth consideration and improvement of traditional synthesis ***,we comprehensively summarize and compare the preparation methods of the trial-and-error synthesis strategy,structure–activity relationships and density functional theory(DFT)guided catalysts rational design for nanomaterials and atomically dispersed *** also discuss in detail the utilization of the nanomaterials and single atom catalysts for converting small molecules(H_(2)O,O_(2),CO_(2),N_(2),etc.)into value-added products driven by electrocatalysis,photocatalysis,and ***,the challenges and outlooks of mass preparation and production of efficient and green catalysts through conventional trial and error synthesis and DFT theory are featured in accordance with its current development.

关键词： trial-and-error synthesis structure–activity relationships density functional theory(DFT)guidance nanomaterials atomically dispersed catalysts

Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao Jie P.Li Zijian Guo State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two PtIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a Pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology

Development of an active-site titrant for SARS-CoV-2 main protease as an indispensable tool for evaluating enzyme kinetics

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2349-2357页

作者： Rabea Voget Julian Breidenbach Tobias Claff Alexandra Hingst Katharina Sylvester Christian Steinebach Lan Phuong Vu Renato H.Weiße Ulrike Bartz Norbert Sträter Christa E.Müller Michael Gütschow Pharmaceutical Institute Pharmaceutical&Medicinal ChemistryUniversity of BonnBonn 53121Germany Institute of Bioanalytical chemistry Center for Biotechnology and BiomedicineLeipzig UniversityLeipzig 04103Germany department of Natural Sciences University of Applied Sciences Bonn-Rhein-SiegRheinbach 53359Germany

A titrant for the SARS-CoV-2 main protease(M^(pro))was developed that enables,for the first time,the exact determination of the concentration of the enzymatically active M^(pro) by active-site *** covalent binding mode of the tetrapeptidic titrant was elucidated by the determination of the crystal structure of the enzyme–titrant *** fluorogenic substrates of M^(pro),including a prototypical,internally quenched Dabcyl-EDANS peptide,were compared in terms of solubility under typical assay *** exploiting the new titrant,key kinetic parameters for the M^(pro)-catalyzed cleavage of these substrates were determined.

关键词： COVID-19 SARS-CoV-2 Main protease Peptide nitriles Fluorogenic substrates Active-site titration X-ray crystallography Inner filter effect

Small-sized Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C for efficient alkaline and acidic hydrogen evolution reaction by an anchoring calcination strategy

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Frontiers of Chemical Science and Engineering 2024年第5期18卷 95-103页

作者： Jianxia Gu Ying Zhu Haiyan Zheng Chunyi Sun Zhongmin Su department of chemistry Xinzhou Normal UniversityXinzhou 034000China School of chemistry Northeast Normal UniversityChangchun 130024China

A novel,cheap and highly efficient Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C nanocomposite has been successfully constructed through simple one-step carbonization method in a nitrogen *** in the precursor can effectively anchor molybdenum-based Keggin-type polyoxometallate and NiCo-layered double hydroxide through electrostatic and coordination interactions,which avoids the aggregation of catalyst particles during the pyrolysis *** optimization,the obtained Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C possesses small size(3-8 nm),large specific surface area and hierarchical pore *** importantly,Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C presents remarkable hydrogen evolution reaction activity with low overpotentials in 0.5 mol·L^(-1)H_(2)SO_(4)(102.3 mV)and 1 mol·L^(-1)KOH(95 mV)to afford the current density of 10 mA·cm^(-2),as well as small Tafel slopes of 82.49 and 99.92 mV·dec^(-1),***,this catalyst also shows outstanding stability for 12 h without a significant change in current *** excellent catalytic performance of Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C can put down to the synergistic effect between multiple components and the small size of the *** work provides unique insights into the preparation of efficient transition metal-based catalysts for HER.

关键词： polyoxometallates layered double hydroxide transition metal-based electrocatalysts hydrogen evolution reaction

A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

A New Approach for the Determination of Metronidazole Using Switchable Solvent Coupled with Au-MWCNTs-Modified Electrochemical Sensor

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Journal of Analysis and Testing 2024年第2期8卷 191-200页

作者： Siamak Kiani Shahvandi Mehrorang Ghaedi Hamid Ahmar chemistry department Yasouj UniversityYasouj75918-74831Iran chemistry department University of ZabolZabol98615-538Iran

In this work,a new liquid-phase microextraction method coupled with an electrochemical technique using a switchable solvent was proposed for the determination of *** extraction solvent used was dipropylamine(DPA),which exhibited switchable *** means that it can become miscible or immiscible when in contact with carboxylic acids in the aqueous *** metronidazole was then measured using a glassy carbon electrode that was modified with Au-multiwalled carbon nanotubes(MWCNTs).The eff ect of diff erent parameters such as the type and amount of trigger,the addition of salt,and the volume of extraction solvent on the e fficiency of switchable hydrophilic solvent-based liquid-phase microextraction(SHS-LPME)was investigated using the one-factor-at-a-time *** optimizing the conditions,the linear calibration curve was obtained in the concentration range of 0.005–250μmol/***,the limit of quantification(LOQ)of 0.005μmol/L and the limit of detection(LOD)of 0.0015μmol/L were obtained,respectively.

关键词： Switchable solvent Metronidazole Liquid-phase microextraction Electrochemical techniques

Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

Decoding the genetic program of micronucleus formation: linking chromosomal instability to human disease

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Signal Transduction and Targeted Therapy 2024年第7期9卷 2840-2842页

作者： Jörg Fahrer Division of Food chemistry and Toxicology Department of ChemistryRPTU Kaiserslautern-Landau67663 KaiserslauternGermany

A recent study by Adams and colleagues published in Nature unveiled more than one hundred genes that are involved in micronucleus formation,1 which is a biomarker for genomic instability and associated with aging,cancer,and other disorders.2 As an outstanding achievement,the authors identified DSCC1(DNA Replication And Sister Chromatid Cohesion 1)as a critical gene protecting against early developmental defects,genomic instability,reduced proliferative capacity,cohesinopathy-related phenotypes,and tumor development in vivo.

关键词： chromosomal linking Replication

Liquid-metals-induced formation of MXene/polyacrylamide composite organohydrogels for wearable flexible electronics

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Nano Research 2024年第3期17卷 1913-1922页

作者： Minying Wu Bin Chen Xueliang Fan Tong Ye Yuanyuan Fang Qian Zhang Fangzhou Zhou Yajun Wang Yi Tang department of chemistry Fudan UniversityShanghai 200433China College of chemistry&Materials Engineering Wenzhou UniversityWenzhou 325027China

Organohydrogels have demonstrated superior environmental adaptability and frost resistance compared to conventional hydrogels,thereby prompting considerable interests in the development and design of innovative ***,we report an effective one-pot method for fabricating MXene/polyacrylamide(MXene/PAM)composite organohydrogel(MAOH)by employing Ga liquid metals(Ga LMs)as a highly reactive component in the induced free radical polymerization reaction,without the need for additional heating or cross-linking *** synthetic protocol addresses the time-consuming and organic solvent waste concerns associated with traditional solvent displacement methods for organohydrogel *** incorporation of MXene not only highly enhances the conductivity but also confers improved mechanical properties of *** MAOH exhibits excellent environmental adaptability(>7 d),sustained moisture retention,remarkable self-healing capabilities,and outstanding mechanical properties under low temperatures(-20℃).It demonstrates exceptional performance in micro-motion monitoring,rapid response time(125 ms),superior stretchability,and a broad range of strains(0.3%–600%).Therefore,the designed MAOH has great potential for applications in diverse fields such as prosthetics,electronic skin,human–machine interaction,and smart terminals.

关键词： organohydrogels MXene conductivity mechanical properties environmental adaptability