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Lighting up aggregate emission of perylene diimide by leveraging polymerization-mediated through-space charge transfer and π-π stacking

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Science China chemistry 2024年

作者： Suiying Ye Désirée Füglistaller Tian Tian Anjay Manian Sudhir Kumar Celine Nardo Andrew J.Christofferson Salvy P.Russo Chih-Jen Shih Jean-Christophe Leroux Yinyin Bao Institute of Pharmaceutical Sciences Department of Chemistry and Applied Biosciences ETH Zurich Vladimir-Prelog-Weg 3 Institute for Chemical and Bioengineering Department of Chemistry and Applied Biosciences ETH Zurich Vladimir-Prelog-Weg 1-5 ARC Centre of Excellence in Exciton Science School of Science RMIT University School of Science STEM College RMIT University

The molecular engineering of fluorescent organic/polymeric materials, specifically those emitting in the deep red to near-infrared spectrum, is vital for advancements in optoelectronics and biomedicine. Perylene diimide(PDI), a well-known fluorescent scaffold, offers high thermal and photophysical stability but suffers from fluorescence quenching in solid or aggregate states due to intense π-π interactions. To mitigate this, simple and versatile methods for strong PDI aggregate emission without extensive synthetic demands are highly desirable but still lacking. Here, we report a straightforward strategy to enhance the solid-state emission of PDI by introducing certain degree of through-space charge transfer(TSCT) via controlled radical polymerization,which can efficiently distort the typical face-to-face PDI stacking, enabling greatly enhanced deep red emission. This is achieved by growing electron-donating star-shape styrenic(co)polymers from a multidirectional electron-accepting PDI initiator. The incorporation of polycyclic aromatic monomers further shifted the emission into the near-infrared region, albeit with a reduced intensity. Overall, the emission of the PDI-based TSCT polymers can be systematically manipulated by leveraging the balance between PDI stacking and the TSCT degree, as confirmed by both experimental study and theoretical calculations. Our approach circumvents complex synthetic procedures, offering highly emissive materials with large Stokes shifts and showing broad potential for optoelectronic technology.

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Recent Advances in Single-Cell Metabolomics Based on Mass Spectrometry

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CCS chemistry 2023年第2期5卷 310-324页

作者： Qinlei Liu Sandra Martínez-Jarquín Renato Zenobi department of chemistry and applied biosciences ETH ZurichCH-8093 Zurich

Cellular heterogeneity is essential for the physiological functions of organisms,and precise interpretation of the relevant biological mechanisms involved requires accurate measurement of biomolecules,including DNA,RNA,proteins,and metabolites at the single-cell *** metabolites react most rapidly to environmental and biochemical changes such that their detection is a critical step in determining the physiological state of ***,their limited amounts,structural diversity,and significant content variation render single-cell metabolomics analysis technically *** spectrometry,with its high sensitivity,good selectivity,and wide dynamic range,has been widely used in the single-cell analysis in recent *** terms of ionization techniques,there are four main types of single-cell mass spectrometry methods:nano-electrospray ionization mass spectrometry,matrix-assisted laser desorption/ionization mass spectrometry,secondary ion mass spectrometry,and dielectric barrier discharge ionization mass *** this mini review,the progress of single-cellmass spectrometrymethodologies and data processing strategies are summarized,and the future trends in single-cell mass spectrometry are outlined.

关键词： single-cell analysis metabolomics mass spectrometry ionization techniques analytical methods

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Probing On-Surface chemistry at the Nanoscale Using Tip-Enhanced Raman Spectroscopy

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CCS chemistry 2023年第1期5卷 55-71页

作者： Zhen-Feng Cai Naresh Kumar Renato Zenobi department of chemistry and applied biosciences ETH ZurichZurich CH-8093

chemistry on solid surfaces is central to many research areas of practical interest,such as synthesis,catalysis,electrochemistry,photochemistry,and materials science.A comprehensive understanding of the nanoscale on-surface chemistry involved in these areas is important for establishing composition-structure-performance *** the rapid development of tip-enhanced Raman spectroscopy(TERS),it has become possible to investigate physical and chemical processes on suitable surfaces at the nanoscale level and in real *** this review,after a brief introduction of the background of onsurface chemistry and TERS,we systematically discuss the progress in the application of TERS in this *** focus is the applications of TERS to nanoscale coordination processes,decomposition reactions,polymerization processes,electrochemical reactions,catalytic chemistry,and functionalization chemistry on solid *** conclude by discussing the future challenges and development of TERS techniques and related applications in on-surface chemistry.

关键词： on-surface chemistry tip-enhanced Raman spectroscopy scanning probe microscopy chemical imaging nanoscale chemical analysis spatial resolution

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Tough PEG-only hydrogels with complex 3D structure enabled by digital light processing of“all-PEG”resins

Aggregate

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Aggregate 2023年第6期4卷 57-70页

作者： Safira Noor Anindita Riccardo Conti Doris Zauchner Nevena Paunovi´c Wanwan Qiu Marina Green Buzhor Adva Krivitsky Zhi Luo Ralph Müller Hansjörg Grützmacher Xiao-Hua Qin Jean-Christophe Leroux Yinyin Bao department of chemistry and applied biosciences Institute of Pharmaceutical SciencesETH ZurichZunichSwitzerland Laboratory of Inorganic Chemitry Department of Chemistry and Applied BiosciencesETH ZurichZurichSwitzerland department of Health Sciences and Technology Institute for BiomechanicsETH ZurichZurichSwitzerland

Digital light processing(DLP)of structurally complex poly(ethylene glycol)(PEG)hydrogels with high mechanical toughness represents a long-standing challenge in theﬁeld of 3D ***,we report a 3D printing approach for the high-resolution manufacturing of structurally complex and mechanically strong PEG hydrogels via heat-assisted *** of using aqueous solutions of photo-crosslinkable monomers,PEG macromonomer melts wereﬁrst printed in the absence of water,resulting in bulk PEG ***,post-printing swelling of the printed networks was achieved in water,producing high-ﬁdelity 3D hydrogels with complex *** employing a dual-macromonomer resin containing a PEG-based four-arm macrophotoinitiator,“all-PEG”hydrogel constructs were pro-duced with compressive toughness up to 1.3 MJ m^(-3).By this approach,porous 3D hydrogel scaffolds with trabecular-like architecture were fabricated,and the scaf-fold surface supported cell attachment and the formation of a monolayer mimicking bone-lining *** study highlights the promises of heat-assisted DLP of PEG photopolymers for hydrogel fabrication,which may accelerate the development of 3D tissue-like constructs for regenerative medicine.

关键词： 3D printing digital light processing PEG hydrogels

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Gelation of polymeric nanoparticles

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Particuology 2014年第3期12卷 1-11页

作者： Hua Wu Massimo Morbidelli Institute for Chemical and Bioengineering.department of chemistry and applied biosciences ETH Zurich8093 ZurichSwitzerland

We review how, starting from polymeric nanoparticles, to generate clusters of fractal morphology and to expand the entire space and interconnect to form gels, through either Brownian motion or intense shear-induced aggregation. In the case of Brownian motion-induced gelation, specific techniques developed to obtain uniform structure of gels under both reaction-limited and diffusion-limited cluster aggregation conditions have been described. In the case of intense shear-induced gelation as a newly developed technique, our focus is on its principle, theoretical development and advantages with respect to Brownian motion-induced gelation in practical applications. We consider gelation of both rigid and soft particles. As a physical process, the bonding between the particles within gels is owed to van der Waals attractions, thus being easily broken. However, in the case of soft particles that can coalesce upon contact, the coalescence can allow the particles to stick together forming permanent gels. In this case, the gel structure can be controlled by controlling the degree of coalescence. Techniques used to control the degree of coalescence have also been described.

关键词： Structured material Fractal Gelation Gel Polymer

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Ceria in halogen chemistry

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Chinese Journal of Catalysis 2020年第6期41卷 915-927页

作者： Matthias Scharfe Guido Zichittella Vladimir Paunovic Javier Pérez-Ramírez Institute for Chemical and Bioengineering Department of Chemistry and Applied BiosciencesETH ZurichVladimir-Prelog-Weg 18093 ZurichSwitzerland

Halogen chemistry constitutes an essential part in the industrial production of polymers and gains increasing attention as an attractive strategy to activate light alkanes that constitute natural gas. CeO2-based catalysts offer an exciting potential for advances in hydrogen halide recovery that enables a high efficiency of halogen-based processes for activation of small molecules. This review provides an overview of recently developed ceria-based catalysts in the context of polymer industry(polyvinyl chloride, polyurethanes, and polycarbonates) and activation of light hydrocarbons for natural gas upgrading. In addition, mechanistic insight and the challenges of ceria catalysts are provided, aiding the design of future catalytic materials and applications.

关键词： CeO2 Hydrogen halides ethylene Alkanes Selective natural gas upgrading Oxidation Oxyhalogenation Vinyl chloride

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Hydrogel-based composites beyond the porous architectures for electromagnetic interference shielding

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Nano Research 2022年第10期15卷 9614-9630页

作者： Yunfei Yang Mingrui Han Wei Liu Na Wu Jiurong Liu Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials School of Materials Science and EngineeringShandong UniversityJinan 250061China State Key Laboratory of Crystal Materials Shandong UniversityJinan 250100China Shenzhen research institute of Shandong University Shenzhen 518052China department of chemistry and applied biosciences ETH ZurichZurich CH-8093Switzerland

With the rapid development of the electronic industry and wireless communication technology,electromagnetic interference(EMI)or pollution has been increasingly *** not only severely endangers the normal operation of electronic equipment but also threatens human ***,it is urgent to develop high-performance EMI shielding *** advent of hydrogel-based materials has given EMI shields a novel *** combined with conductive functional materials have good mechanical flexibility,fatigue durability,and even high stretchability,which are beneficial for a wide range of applications,especially in EMI shielding and some flexible functional ***,the current progress of hydrogel-based EMI shields was reviewed,in the meanwhile,some novel studies about pore structure design that we believe will help advance the development of hydrogel-based EMI shielding materials were also *** the outlook,we suggested some promising development directions for the hydrogel-based EMI shields,by which we hope to provide a reference for designing hydrogels with excellent EMI shielding performance and multifunctionalities.

关键词： electromagnetic interference(EMI)shielding porous hydrogels structural design composites

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PET radiopharmaceuticals for neuroreceptor imaging

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Nuclear Science and Techniques 2006年第3期17卷 143-147页

作者： S. M. AMETAMEY P. A. SCHUBIGER Center for Radiopharmaceutical Science of eth PSI and USZ Department of Chemistry and Applied Biosciences of ETH Zurich Switzerland

Routine clinical PET radiopharmaceuticals for the noninvasive imaging of brain receptors, transporters, and enzymes are commonly labeled with positron emitting nuclides such as carbon-11 or fluorine-18. Certain minimal conditions need to be fulfilled for these PET ligands to be used as imaging agents in vivo. Some of these prerequisites are discussed and examples of the most useful clinical PET radiopharmaceuticals that have found application in the central nervous system are reviewed.

关键词： PET 放射性药品大脑受体碳-11 氟-18

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Biopolymer-Based Aerogels for Electromagnetic Wave Shielding and Absorbing

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Chinese Journal of chemistry 2023年第3期41卷 322-334页

作者： Mingrui Han Runa Zhang Qilei Wu Na Wu Jiurong Liu Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials Ministry of Education and School of Materials Science and EngineeringShandong UniversityJinanShandong250061 China Science and Technology on Electromagnetic Compatibility Laboratory China Ship Development and Design CentreWuhanHubei430064 China department of chemistry and applied biosciences ETH ZurichCH-8093 ZurichSwitzerland

The rapid development of communication technology and electronic industry has brought unprecedented serious electromagnetic interference(EMI)and electromagnetic wave(EMW)*** EMI shields and EMW absorbers based on metal or magnetic materials were used to solve these problems,they have long been criticized for their high price,high density and easy *** order to achieve low density and efficient dissipation of electromagnetic energy,aerogels stand out among manifold ***,constructing aerogels with good EMI shielding or EMW absorption performance and acceptable mechanical properties is not an easy *** biopolymers,such as cellulose,lignin,chitin/chitosan and alginate,breathe new life into aerogels for high-efficiency EMW shielding and ***,we reviewed the contributions of biopolymers in the fields of aerogels for EMW shielding and *** the same time,some challenges and outlook were also pointed out,aiming to promote the advance of aerogel-based EMI shields and EMW absorbers as well as the rational utilization of biopolymers.

关键词： Polymers Sustainable chemistry Electromagnetic interference(EMI)shielding Electromagnetic wave(EMW)absorbing Biomass Aerogels Biopolymers

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Pneumatic programmable superrepellent surfaces

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Droplet 2022年第1期1卷 48-55页

作者： Songtao Hu Xiaobao Cao Tom Reddyhoff Xijia Ding Xi Shi Daniele Dini Andrew J.deMello Zhike Peng Zuankai Wang School of Mechanical Engineering State Key Laboratory of Mechanical System and VibrationShanghai Jiao Tong UniversityShanghaiChina Guangzhou Laboratory GuangzhouChina department of Mechanical Engineering Imperial College LondonLondonUK department of chemistry and applied biosciences ETH ZurichZurichSwitzerland department of Mechanical Engineering City University of Hong KongHong KongChina

Morphological transformation of surface structures is widely manifested in nature and highly preferred for many applications such as wetting interaction;however,in situ tuning of artificial morphologies independent of smart responsive materials remains ***,with the aid of microfluidics,we develop a pneumatic programmable superrepellent surface by tailoring conventional wetting materials(e.g.,polydimethylsiloxane)with embedded flexible chambers connecting a microfluidic system,thus realizing a morphological transformation for enhanced liquid repellency based on a nature‐inspired rigid‐flexible hybrid principle(i.e.,triggering symmetry breaking and oscillator coupling mechanisms).The enhancement degree can be in situ tuned within around 300 ms owing to pneumatically controllable chamber *** also demonstrate that the surface can be freely programmed to achieve elaborated morphological pathways and gradients for preferred droplet manipulation such as directional rolling and *** study highlights the potential of an in situ morphological transformation to realize tunable wettability and provides a programmable level of droplet control by intellectualizing conventional wetting materials.

关键词： transformation connecting breaking

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