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A Near-Infrared Organoplatinum(Ⅱ) Metallacycle Conjugated with Heptamethine Cyanine for Trimodal Cancer Therapy

CCS Chemistry 2022年第6期4卷 2090-2101页

作者： Baoxuan Huang Xi Liu Guoliang Yang Jia Tian Zhiyong Liu Yucheng Zhu Xiaopeng Li Guangqiang Yin Wei Zheng Lin Xu Weian Zhang Shanghai Key Laboratory of Functional Materials Chemistry East China University of Science and TechnologyShanghai 200237 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518055 Department of Chemistry University of South FloridaTampaFL 33620

Discrete Pt(Ⅱ)metallacycles have attracted particular attention for the chemotherapeutic treatment of ***,a single chemotherapy cannot simultaneously balance efficiency and safety because the continuous administration throughout the entire therapy period will lead to inefficient therapy and potentially long-term systemic ***,the development of a novel organoplatinum(Ⅱ)metallacycle with multimodal treatment capabilities is urgently needed to overcome these ***,a discrete Pt(II)metallacycle(SCY)bearing the near-infrared(NIR)photosensitizer heptamethine cyanine was fabricated and further encapsulated by amphiphilic 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-methoxy(polyethyleneglycol)(DSPEmPEG)to form P@SCY *** cyanine,which has excellent photoconversion efficiency,can generate reactive oxygen species(ROS)and heat simultaneously,and the cyanine moiety can target mitochondria in cancer cells due to their quaternary ammonium salt cations,which improve the effect of *** to its excellent phototherapy and chemotherapy properties,P@SCY exhibited remarkable trimodal therapeutic effects[chemo-/photodynamic therapy(PDT)/photothermal therapy(PTT)]against cancer cells(HepG2 cells,MCF-7 cells,and 4T1 cells)in ***,in vivo results also confirmed thatP@SCY had superior antitumor properties with minimal side effects in the 4T1 tumor *** presents a practicable approach to develop a multifunctional organoplatinum(Ⅱ)metallacycle for multimodal tumor therapy.

关键词： near-infrared metallacycle cyanine phototherapy chemotherapy

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Enhancement of effluent degradation by zinc oxide, carbon nitride, and carbon xerogel trifecta on brass monoliths

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Environmental science and Pollution Research 2024年第40期31卷 53472-53496页

作者： da Silva, Émerson Felipe Mendonça Garcia, Ramón Raudel Peña Rodrigues, Liana Alvares Napoleão, Daniella Carla Sanz, Oihane Almeida, Luciano Costa Department of Chemical Engineering Technology and Geoscience Center Federal University of Pernambuco PE Recife50740-521 Brazil Pós Graduate Program in Materials Science and Engineering Federal University of Piauí PI Teresina64049-550 Brazil Academic Unit of Cabo de Santo Agostinho Federal Rural University of Pernambuco PE Cabo de Santo Agostinho54518-430 Brazil Dept. of Applied Chemistry Chemistry Faculty University of the Basque Country UPV/EHU P. Lardizabala 3 San Sebastian20018 Spain Escola de Engenharia de Lorena EEL/USP Estrada Municipal Do Campinho S/N São Paulo LorenaCEP 12602-810 Brazil

In recent years, heterogeneous photocatalysis has emerged as a promising alternative for the treatment of organic pollutants. This technique offers several advantages, such as low cost and ease of operation. However, finding a semiconductor material that is both operationally viable and highly active under solar irradiation remains a challenge, often requiring materials of nanometric size. Furthermore, in many processes, photocatalysts are suspended in the solution, requiring additional steps to remove them. This can render the technique economically unviable, especially for nanosized catalysts. This work demonstrated the feasibility of using a structured photocatalyst (ZnO, g-C3N4, and carbon xerogel) optimized for this photodegradation process. The synthesized materials were characterized by nitrogen adsorption and desorption, X-ray diffraction (XRD), and diffuse reflectance spectroscopy (DRS). Adhesion testing demonstrated the efficiency of the deposition technique, with film adhesion exceeding 90%. The photocatalytic evaluation was performed using a mixture of three textile dyes in a recycle photoreactor, varying pH (4.7 and 10), recycle flow rate (2, 4, and 6 L h−1), immobilized mass (1, 2, and 3 mg cm−2), monolith height (1.5, 3.0, and 4.5 cm), and type of radiation (solar and visible artificials;and natural solar). The structured photocatalyst degraded over 99% of the dye mixture under artificial radiation. The solar energy results are highly promising, achieving a degradation efficiency of approximately 74%. Furthermore, it was possible to regenerate the structured photocatalyst up to seven consecutive times using exclusively natural solar light and maintain a degradation rate of around 70%. These results reinforce the feasibility and potential application of this system in photocatalytic reactions, highlighting its effectiveness and sustainability. © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2024.

关键词： Heterojunctions

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Green Energy for Autonomous Devices: Surfactant-Enhanced Membraneless Hydrogen Peroxide Fuel Cells∗ 6

Green Energy for Autonomous Devices: Surfactant-Enhanced Mem...

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6th International Conference on Manipulation, Automation, and Robotics at Small Scales, MARSS 2023

作者： Zhu, Fenyang Kuzin, Aleksei Chen, Guoxiang Gorin, Dmitry A. Mohan, Brij Huang, Gaoshan Zhao, Shuangliang Mei, Yongfeng Solovev, Alexander A. Skolkovo Institute of Science and Technology Center for Photonic Science and Engineering Moscow121205 Russia Institute of Molecular Sciences Instituto Superior Tecnico Universidade de Lisboa Centro de Quimica Estrutural Lisboa1049-001 Portugal Fudan University State Key Laboratory of Molecular Engineering of Polymers Department of Materials Science Shanghai200433 China International Institute of Intelligent Nanorobots and Nanosystems Fudan University Shanghai200433 China Yiwu Research Institute of Fudan University Zhejiang Yiwu322000 China Guangxi University Guangxi Key Laboratory of Petrochemical Resources Processing and Process Intensification Technology School of Chemistry and Chemical Engineering Nanning530004 China Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception Fudan University Shanghai200433 China

ISBN: (纸本)9798350330397

The amphipathic properties of surfactant macromolecules, characterized by their hydrophilic and hydrophobic terminal groups, are ubiquitously used to modulate the surface tension of interfaces and clean surfaces. Previously, the crucial role of surfactants was reported for the performance of catalytic nano/- and micromotors. In this study, we extrapolate this concept to the membraneless hydrogen peroxide (H2O2) Fuel Cells (FCs), which exhibit performance dependence on the addition of different types of surfactants: cationic - Sodium Dodecyl Sulfate (SDS), anionic - Benzalkonium Chloride (BACl), and nonionic - Tween20. Among them, charged SDS and BACl show promotion and inhibition towards fuel cell performance, respectively. Non-charged Tween20 shows a neutral effect on fuel cell performance. © 2023 IEEE.

关键词： Oxidation

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Local Changes in Protein Filament Properties Drive Large-Scale Membrane Transformations Involved in Endosome Tethering and Fusion

arXiv

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arXiv 2023年

作者： Ghosh, Ashesh Spkaowitz, Andrew J. Department of Chemical Engineering Stanford University StanfordCA94305 United States Biophysics Program Stanford University StanfordCA94305 United States Department of Materials Science & Engineering Stanford University StanfordCA94305 United States

Large-scale cellular transformations are triggered by subtle physical and structural changes in individual biomacromolecular and membrane components. A prototypical example of such an event is the orchestrated fusion of membranes within an endosome that enables transport of cargo and processing of biochemical moieties. In this work, we demonstrate how protein filaments on the endosomal membrane surface can leverage a rigid-to-flexible transformation to elicit a large-scale change in membrane flexibility to enable membrane fusion. We develop a polymer field-theoretic model that captures molecular alignment arising from nematic interactions with varying surface density and fraction of flexible filaments, which are biologically controlled within the endosomal membrane. We then predict the collective elasticity of the filament brush in response to changes in the filament alignment, predicting a greater than 20-fold increase of the effective membrane elasticity over the bare membrane elasticity that is triggered by filament alignment. These results show that the endosome can modulate the filament properties to orchestrate membrane fluidization that facilitates vesicle fusion, providing an example of how active processes that modulate local molecular properties can result in large-scale transformations that are essential to cellular survival. © 2023, CC BY.

关键词： Elasticity

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Atomic Ionization: sd energy imbalance and Perdew-Zunger self-interaction correction energy penalty in 3d atoms

arXiv

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arXiv 2024年

作者： Maniar, Rohan Shukla, Priyanka B. Johnson, J. Karl Jackson, Koblar A. Perdew, John P. Department of Physics and Engineering Physics Tulane University New OrleansLA70118 United States Department of Chemical & Petroleum Engineering University of Pittsburgh PittsburghPA15261 United States Physics Department Science of Advanced Materials Program Central Michigan University Mount PleasantMI48859 United States

To accurately describe the energetics of transition metal systems, density functional approximations (DFAs) must provide a balanced description of s- and d- electrons. One measure of this is the sd transfer error, which has previously been defined as E(3dn−14s1)−E(3dn−24s2). Theoretical concerns have been raised about this definition due to its evaluation of excited-state energies using ground-state DFAs. A more serious concern appears to be strong correlation in the 4s2 configuration. Here we define a ground-state measure of the sd energy imbalance, based on the errors of s- and d-electron second ionization energies of the 3d atoms, that effectively circumvents the aforementioned problems. We find an improved performance as we move from LSDA to PBE to r2SCAN for first-row transition metal atoms. However, we find large (∼ 2 eV) ground-state sd energy imbalances when applying a Perdew-Zunger 1981 self-interaction correction. This is attributed to an "energy penalty" associated with the noded 3d orbitals. A local scaling of the self-interaction correction to LSDA results in a balance of s- and d-errors. Copyright © 2024, The Authors. All rights reserved.

关键词： Atoms

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Importance of kink energy in calculating the formation energy of a graphene edge

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Physical Review B 2023年第24期107卷 245420-245420页

作者： Wookhee Lee Daniel Hedman Jichen Dong Leining Zhang Zonghoon Lee Sung Youb Kim Feng Ding Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Korea Center for Multidimensional Carbon Materials (CMCM) Institute for Basic Science (IBS) Ulsan 44919 Korea Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 China Department of Mechanical Engineering Ulsan National Institute of Science and Technology Ulsan 44919 South Korea Faculty of Materials Science and Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences 1068 Xueyuan Blvd Shenzhen 518055 China

The formation energy of an arbitrary graphene edge or that of other 2D materials has been estimated as a summation of the armchair (AC) and zigzag (ZZ) edge sites. Such an estimation assumes that each site is independent from its neighboring sites, which is unlikely due to the overlap of electron densities. Here, we show that to accurately calculate the formation energy of graphene edges with various functional groups the energy of the junction between AC and ZZ sites, the “kink energy,” is essential. It is significant that the kink energies of graphene edges with different functional groups are all negative, namely, kink formation stabilizes the chiral graphene edges.

关键词： Defects Graphene Density functional calculations materials modeling

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Mechanistic Insight into Supramolecular Polymerization in Water Tunable by molecular Geometry

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CCS Chemistry 2022年第7期4卷 2212-2220页

作者： Fan Xu Stefano Crespi Lukas Pfeifer Marc C.A.Stuart Ben L.Feringa Stratingh Institute for Chemistry University of GroningenGroningen 9747 AG Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237 Angstrom Laboratory Department of ChemistryUppsala UniversityUppsala 75120 Laboratory of Photonics and Interfaces Department of Chemistry and Chemical EngineeringÉcole Polytechnique Fédérale de LausanneLausanne CH-1015

Supramolecular self-assembly in water based on non-covalent bonding is attracting major attention due to the potential of hydrogels and aqueous polymers in biomedical *** supramolecular polymerization in organic solvents is well established,the key design features,the assembly mechanisms in water and achieving control over the aggregate structures remain ***,we present the assembly and disassembly of geometrical isomers of a stiff-stilbene bis-urea amphiphile(SA)in pure water.A remarkable feature of this system is that the(E)-isomer forms supramolecular polymers in both pure water and organic *** advantage of this unique property,the hydrophobic effect was studied by comparing the supramolecular assembly in both *** assembly process inwater follows an enthalpy-driven nucleation-elongation(cooperative)supramolecular polymerization mechanism with a standard Gibbs free energy(ΔG°=−53 kJ mol^(−1))double the value of the one found in *** attributed this distinctive feature to the hydrophobic effect in ***,we discovered an isomer-dependent assembly process,which can be used to control aggregation in aqueous *** to the substantial geometric difference between(E)-SA and(Z)-SA,we compared their assembly in water to study the influence of different driving forces involved in the *** supramolecular polymerization of(E)-SA was cooperatively influenced by hydrogen bonding,π-stacking,and hydrophobic effects,whereas the assembly of(Z)-SAwasmainly driven by hydrophobic *** a result,the fiber length of(E)-SA in water is much longer than that of(Z)-SA,presenting opportunities for geometrical control of aggregation in aqueousmedia.

关键词： supramolecular polymerization stiff-stil-bene bis-urea hydrogen bonding π-stacking hydro-phobic effects

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Elastic Dipole Alignment is the Origin of Anelasticity and Electrostriction in Aliovalent-Doped Ceria

SSRN

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SSRN 2024年

作者： Lavie, Anna Xu, Boyuan Khodorov, Sergey Singh, Harishchandra Liu, Jinghe Hajbi, Tal-El Wachtel, Ellen Feldman, Yishay Ehre, David Donetsky, Dmitri Frenkel, Anatoly I. Qi, Yue Lubomirsky, Igor Dept. Molecular Chemistry and Materials Science Weizmann Institute of Science Rehovot Israel Department of Physics Brown University ProvidenceRI02912 United States Department of Materials Science and Chemical Engineering Stony Brook University Stony Brook NY11794 United States Department of Electrical and Computer Engineering Stony Brook University Stony Brook NY11794 United States Department of Chemical Research Support Weizmann Institute of Science Rehovot Israel Chemistry Division Brookhaven National Laboratory Upton NY11973 United States School of Engineering Brown University ProvidenceRI02912 United States

We investigated the nature of recently discovered anelasticity and electrostriction in aliovalent ceria. DC bias ≤10 kV/cm was applied to trivalent-doped ceria ceramics. ~20nm thick TaOx was used as a blocking layer at the Ta electrode/ceramic interface. Strain was monitored in-situ with X-ray diffraction and X-ray absorption spectroscopy. The electric field produces out-of-plane tensile strain ≤ 1200ppm near the positive electrode. Upon field removal, strain persists for ≥ 24h at 300K but is fully reversible following 5h at 413 K. The positive strain is not due to compositional change;rather, it is anelastic residual strain, confirming the existence of elastic dipoles. From the dopant concentration dependence of the saturation strain, the elastic dipole extent is estimated to be ~1.9 unit cells. DFT predicts formation of extended elastic dipoles due to interacting oxygen vacancies and trivalent dopants. Combining DFT and molecular dynamics calculations, we offer a model that explains key experimental observations: absence of zero-field elastic dipole;contraction in the direction of electric field on a time scale ≤ 4 sec;and large expansion in the DC electric field after 14h. The proposed model may describe anelasticity and electrostriction in other ionic conductors where they originate from vacancy-induced elastic dipoles. © 2024, The Authors. All rights reserved.

关键词： X ray absorption spectroscopy

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Preparation of nanoparticles of shellac and shellac-oligomer conjugates

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Journal of Macromolecular science, Part A 2022年第3期59卷 228-240页

作者： Mongkhol Prawatborisut Jindaporn Janprasit Farzad Seidi Thanyaporn Wongnate Adrian Flood Doungporn Yiamsawas Daniel Crespy a Department of Materials Science and Engineering School of Molecular Science and Engineering Vidyasirimedhi Institute of Science and Technology (VISTEC) Rayong Thailand b Department of Biomolecular Science and Engineering School of Biomolecular Science and Engineering Vidyasirimedhi Institute of Science and Technology (VISTEC) Rayong Thailand c Department of Chemical and Biomolecular Engineering School of Energy Science and Engineering Vidyasirimedhi Institute of Science and Technology (VISTEC) Rayong Thailand d National Nanotechnology Center (NANOTEC) National Science and Technology Development Agency (NSTDA) Pathumthani Thailand

Shellac is a natural biodegradable oligoester produced by lac insects, containing reactive functional groups such as hydroxyl, carboxylic acid, ester, aldehyde, and alkene groups, which can be used for chemical functionalization. Herein, shellac is functionalized with poly(ethylene glycol) (PEG) or poly(N-isopropylacrylamide) (PNIPAM) via grafting-to and grafting-from methods. The functional polymer conjugates are then processed as nanoparticles by the miniemulsion-solvent evaporation process. Shellac-PEG nanoparticles are enriched with apolipoprotein AI after incubation in fetal bovine serum at 37 °C. Moreover, shellac-PNIPAM nanoparticles adsorb specifically prothrombin at 37 °C (T> volume phase transition temperature, VPTT).Graphical Abstract

关键词： Nanoparticle PEGylation PNIPAM shellac temperature-responsive

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Large-Scale Distributed Multidisciplinary Design Optimization of the NASA Lift-Plus-Cruise Air Taxi Concept

Large-Scale Distributed Multidisciplinary Design Optimizatio...

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AIAA science and Technology Forum and Exposition, AIAA SciTech Forum 2025

作者： van Schie, Sebastiaan P. C. Ruh, Marius L. Fletcher, Andrew Warner, Michael Sperry, Mark Scotzniovsky, Luca Orndorff, Nicholas C. Xiang, Ru Yan, Jiayao Zhao, Han Krokowski, Joshua J. Chen, J.S. Sarojini, Darshan Gill, Hyunjune Lee, Seongkyu Tagg, Andrew Anderson, Ryan Green, Eric Joseph, Cibin Ning, Andrew Cheng, Zeyu Cao, Zhi Mi, Chunting Guibert, Alexandre T. R. Cronk, Ashley Kim, H. Alicia Meng, Y. Shirley Silva, Christopher Hwang, John T. University of California San Diego 9500 Gilman Dr La Jolla CA92093 United States Department of Mechanical and Aerospace Engineering University of California San Diego 9500 Gilman Dr La Jolla CA92093 United States Department of Structural Engineering University of California San Diego 9500 Gilman Dr La Jolla CA92093 United States Aerospace and Ocean Engineering Department Virginia Tech 1600 Innovation Dr BlacksburgVA24060 United States Department of Mechanical and Aerospace Engineering University of California Davis 1 Shields Avenue DavisCA95616 United States Mechanical Engineering Brigham Young University ProvoUT84602 United States Department of Electrical & Computer Engineering San Diego State University 5500 Campanile Dr San Diego92182 United States Structural Engineering Department University of California San Diego 9500 Gilman Dr La Jolla CA92093 United States Materials Science & Engineering Program University of California San Diego 9500 Gilman Dr La Jolla CA92093 United States Pritzker School of Molecular Engineering The University of Chicago ChicagoIL60607 United States NASA Ames Research Center Moffett FieldCA94035 United States

ISBN: (数字)9781624107238

ISBN: (纸本)9781624107238

Large-scale gradient-based Multidisciplinary Design Optimization (MDO) can aid in the exploration of high-dimensional design spaces for novel air vehicle concepts, thereby leading to more efficient and economic designs. This paper builds on past works where we demonstrated large-scale physics-based MDO capabilities and applied these to NASA’s lift-plus-cruise electric air taxi concept. We extend this comprehensive mid-fidelity system-level optimization problem with high(er)-fidelity subsystem-level optimizations of various aircraft systems and mission phases, with the aim of further enhancing the accuracy and scope of the aforementioned system-level optimization problem: 1) Power minimization during the transition mission phase;2) Electrical powertrain topology optimization;3) Cell chemistry modeling and thermomechanical battery pack topology optimization;4) Shell-based coupled aero-elastic wing structure optimization. An Analytical Target Cascading-like distributed MDO architecture allows us to couple the system- and subsystem-level optimizations in order to arrive at a consistent and feasible design. We find that the system-level design is most heavily impacted by the reduced battery pack-level energy densities that stem from power peaks in the mission profile. These power peaks seem to result from the inefficient lift rotor blade designs that are needed to satisfy noise constraints. We draw conclusions based on trends in our results and give recommendations for future MDO studies of electrical air taxi vehicle concepts. © 2025, American Institute of Aeronautics and Astronautics Inc, AIAA. All rights reserved.

关键词： Shape optimization

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