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In Vivo Voltammetric Imaging of Metal Nanoparticle-Catalyzed Single-Cell Electron Transfer by Fermi Level-Responsive graphene

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research 2024年第1期2023卷 271-280页

作者： Qing Xia Rui Liu Xueqin Chen Zixuan Chen Jun-Jie Zhu State Key Laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023P.R.China Shenzhen research Institute of Nanjing University Shenzhen 518000P.R.China

Metal nanomaterials can facilitate microbial extracellular electron transfer(EET)in the electrochemically active ***,the role of nanomaterials/bacteria interaction in this process is still ***,we reported the single-cell voltammetric imaging of Shewanella oneidensis MR-1 at the single-cell level to elucidate the metal-enhanced EET mechanism in vivo by the Fermi level-responsive graphene *** oxidation currents of~20 fA were observed from single native cells and gold nanoparticle(AuNp)-coated cells in linear sweep voltammetry *** the contrary,the oxidation potential was reduced by up to 100 mV after AuNp *** revealed the mechanism of AuNp-catalyzed direct EET decreasing the oxidation barrier between the outer membrane cytochromes and the *** method offered a promising strategy to understand the nanomaterials/bacteria interaction and guide the rational construction of EET-related microbial fuel cells.

关键词： Fermi voltammetry Electron

Supramolecular Biomaterials for Cancer Immunotherapy

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research 2024年第2期2023卷 491-509页

作者： Huan Liang Qingqing Lu Jie Yang guocan Yu College of Science Nanjing Forestry UniversityNanjing 210037P.R.China Key Laboratory of Bioorganic phosphorus chemistry&Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084P.R.China

Cancer immunotherapy has achieved tremendous successful clinical results and obtained historic victories in tumor ***,great limitations associated with feeble immune responses and serious adverse effects still cannot be neglected due to the complicated multifactorial etiology and pathologic microenvironment in *** rapid development of nanomedical science and material science has facilitated the advanced progress of engineering biomaterials to tackle critical *** supramolecular biomaterials with flexible and modular structures have exhibited unparalleled advantages of high cargo-loading efficiency,excellent biocompatibility,and diversiform immunomodulatory activity,thereby providing a powerful weapon for cancer *** past decades,supramolecular biomaterials were extensively explored as versatile delivery platforms for immunotherapeutic agents or designed to interact with the key moleculars in immune system in a precise and controllable *** this review,we focused on the crucial role of supramolecular biomaterials in the modulation of pivotal steps during tumor immunotherapy,including antigen delivery and presentation,T lymphocyte activation,tumor-associated macrophage elimination and repolarization,and myeloid-derived suppressor cell *** on extensive research,we explored the current limitations and development prospects of supramolecular biomaterials in cancer immunotherapy.

关键词： biomaterials limitations thereby

Nanozyme catalysis in a crowded environment:The impact of diffusion and surface shielding

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Nano research 2024年第7期17卷 5795-5800页

作者： Vasily g.panferov Juewen Liu department of chemistry Waterloo Institute for NanotechnologyWaterlooOntario N2L 3G1Canada

Nanozymes are widely used in various applications as nanosized catalysts for replacing *** accurate estimation of the catalytic activity of nanozymes in real conditions is *** this article,for the first time,we systematically studied the effect of macromolecular molecules co-existing in the real system on the oxidoreductase(peroxidase,oxidase,and catalase)-mimicking nanozymes made of a gold nanoparticle core and a platinum shell,prussian Blue,Mn2O3 and CoO *** were made with horseradish *** distinguished two main mechanisms of the negative impact of macromolecules on nanozyme catalysis—slowed diffusion and surface shielding of *** the first mechanism is typical for enzymes,the second one is specific only for *** the mechanisms is essential for developing approaches to reduce the unavoidable impact of macromolecules for various analytical and biomedical applications.

关键词： molecular crowding biosensors nanoparticles

Recent Advances in 0D Ni/Co-based Hollow Electrocatalysts for Electrochemical Water Splitting

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Chemical research in Chinese Universities 2024年第3期40卷 437-450页

作者： gE Wenjing CHEN Xiaocui MA Ruizhao ZHENg Siyuan SHANg Ningzhao ZHAO Xiaoxian department of chemistry College of ScienceHebei Agricultural UniversityBaoding 071001P.R.China

Electrochemical water splitting using renewable energy sources has been recognized as a sustainable way to produce hydrogen energy due to the characteristics of low-carbon and no ***,the slow hydrogen/oxygen evolution reactions(HER/OER)seriously hinder the practical application of large-scale water *** this paper,the 0D Ni/Co-based hollow material is discussed in detail because of adjustable morphology,low mass density and abundant active sites,which provides an effective solution for improving the HER/OER reaction *** synthesis methods of hollow materials,such as hard template,soft template and self-template are ***,catalysts with different structural designs of hollow structures are reviewed,including hollow single-shelled structure,hollow core-shelled structure,hollow double-shelled structure and hollow multi-shelled structure(HoMS)***,the research progress of the 0D Ni/Co-based HoMS electrocatalysts in recent years and their prominent performances in water splitting are ***,the challenges and development prospects of designing Ni/Co-based HoMS catalysts in water splitting in the future are discussed.

关键词： Electrochemical watersplitting Morphological regulation Hollow structure Hollow multi-shelled structure(HoMS)

Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

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Carbon Energy 2024年第3期6卷 64-117页

作者： Karl Adrian gandionco Juwon Kim Lieven Bekaert Annick Hubin Jongwoo Lim department of chemistry Seoul National UniversitySeoulRepublic of Korea research group Electrochemical and Surface Engineering(SURF) Department of Materials and ChemistryVrije Universiteit BrusselBrusselsBelgium

The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel *** this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral *** the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic ***-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon ***,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon *** this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom *** is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.

关键词： electrocatalysis electrochemical CO_(2)reduction hydrocarbons oxygenates single-atom catalysts

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

Engineering of efficient visible light photocatalysts:Ti_(1-x+y)Cu_(x)La_(y)O_(2)(x=0.03;y=0,0.005,0.01) compositions

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Journal of Rare Earths 2024年第3期42卷 497-505,I0003页

作者： S.M.Yakout A.M.Youssef Inorganic chemistry department National Research Centre(NRC)El Buhouth StDokkiCairo12622Egypt

In dye-photocatalysis, widening the wavelengths absorption range of catalysts as well as aborting the recombination of the photoexcited charge carriers(electrons-holes pairs) are of paramount *** the current study, we report the photocatalytic characteristics of four compositions composed of TiO_(2),Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders for two harmful dyes(Congo red and methylene blue). The X-ray diffraction technique verified the configuration of mixed anatase and rutile phases in pure TiO_(2)and Ti_(0.97)Cu_(0.03)O_(2)powders while Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders possess anatase phase only. The changes of the band gap structure and dimensions of the unit cell volume of TiO_(2)confirm the substitution of Ti^(4+)sites by Cu^(2+)and La^(3+)ions. Remarkable widening of wavelengths absorption with formation of long absorption tails were found in TiO_(2)(3.13 e V) through insertion of La^(3+)plus Cu^(2+)ions. Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)samples exhibit a visible light band gap of 2.3 and 2.7 e V, respectively. Based on SEM images, incorporation of Cu^(2+)and La^(3+)ions influences the surface morphology of TiO_(2). The resulting Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders present enhanced photocatalytic activity towards Congo red dye degradation compared to pure one under natural solar spectrum. The best Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst exhibits superior photocatalytic activity of 96% for 10 ppm CR dye in 20 min as well as above average photocatalytic efficiency of 63% for 30 ppm CR dye in 120 min. As well, it showed acceptable photodegradation activity of 52% for 30 ppm MB solution in 140 min of sunlight irradiation. The heightened photodegradation efficiency of Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst can be clarified in terms of higher ch

关键词： Semiconductor TiO_(2) Rare earths Congo red Methylene blue Solar spectrum photodegradation

Single-atom pt on carbon nanotubes for selective electrocatalysis

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Carbon Energy 2024年第1期6卷 63-71页

作者： Samuel S.Hardisty Xiaoqian Lin Anthony R.J.Kucernak David Zitoun department of chemistry Bar Ilan Institute of Nanotechnology and Advanced Materials(BINA)Bar Ilan UniversityRamat GanIsrael department of chemistry Molecular Science Research HubImperial College LondonLondonUK

Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox *** via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the *** electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the *** single-atom samples showed higher HOR activity than state-of-the-art 30%pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating *** selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.

关键词： confinement electrocatalysis hydrogen platinum single atom catalysts

Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANg Shuang gUO Yong LIU Xiaohui WANg Yanqin Key Laboratory for Advanced Materials and Joint International research Laboratory of precision chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)