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Synthetic investigations of the diisocyanide-bridged Cp*-cobalt rectangles

Journal of the Chinese Chemical Society 2024年第4期71卷 376-384页

作者： Huang, Cheng-Chang Chu, Yu-Ting Huang, Yen-Chung Chang, Yu-Lun Ding, Shangwu Hsu, Sodio C. N. Department of Medicinal and Applied Chemistry Kaohsiung Medical University Kaohsiung Taiwan Department of Chemistry National Sun Yat-Sen University Kaohsiung Taiwan International PhD Program for Science National Sun Yat-Sen University Kaohsiung Taiwan

This study explores the utilization of 1,4-diisocyanobenzene as a linear bridging ligand for the assembly of organometallic CpCo or Cp*Co complexes. Overcoming solubility challenges, the synthesis of organometallic Cp* cobalt complexes incorporating bridging 1,4-diisocyanobenzene ligands was successfully achieved, while similar CpCo complexes were not attainable. The presented approach encompasses investigations into both stepwise and self-assembly synthetic pathways, leading to the construction of a rectangular tetranuclear complex [(Cp*CoI)₄(μ-1,4-CNC₆H₄NC)₄](OTf)₄ (3). Through single-crystal x-ray diffraction and spectroscopic techniques such as infrared, nuclear magnetic resonance, and electrospray ionization-mass spectrometry, the cobalt-isocyanides complexes were characterized. © 2024 The Chemical Society Located in Taipei & Wiley-VCH GmbH.

关键词： 1,4-diisocyanobenzene cobalt Cp cyclic voltammetry self-assembly

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Teaching Green chemistry Through Student-Generated Open Educational Resources

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Journal of College Science Teaching 2023年第4期52卷 3-5页

作者： Grieger, Krystal Leontyev, Alexey Department of Chemistry and Biochemistry North Dakota State University in Fargo ND United States Department of Chemistry and Biochemistry and Discipline-Based Education Research PhD Program North Dakota State University Fargo ND United States

This article describes the implementation of a student-generated open educational resource project into a majors ’ organic chemistry laboratory. This scaffolded semester-long project was organized into six phases and designed to promote the goals of teaching students about both green chemistry and real-life applications of the reactions covered in the course while simultaneously creating open educational resources for future students. A project-based learning approach was utilized to promote student engagement, especially during remote instruction. To further promote engagement, multiple opportunities for peer feedback were provided using web-based software that supports anonymous feedback. The effect of the project on cognitive learning gains and student perceptions was assessed and is reported. Overall, positive learning gains on green chemistry knowledge and skills were observed, and most students viewed the project favorably. © 2023 National Science Teaching Association.

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Steric and electronic influence on Cu-Cu short contacts in β-thioketiminato tricopper(i) clusters

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Dalton Transactions 2024年第31期53卷 13160-13173页

作者： Penki, Venkata Sai Sashankh Chu, Yu-Ting Chen, Hsing-Yin Sudewi, Sri Li, Chien-Hung Huang, Genin Gary Hsu, Sodio C. N. Department of Medicinal and Applied Chemistry Kaohsiung Medical University Kaohsiung80708 Taiwan International PhD Program for Science National Sun Yat-sen University Kaohsiung80424 Taiwan Department of Pharmacy Faculty of Mathematic and Natural Science Universitas Sam Ratulangi Manado95115 Indonesia Department of Medical Research Kaohsiung Medical University Hospital Kaohsiung80708 Taiwan

A series of β-thioketiminate copper(i) complex trimers [LCuI]3 were synthesized by modifying the ligand framework with electron-withdrawing groups (F and Cl) or electron-donating groups (iPr and Me) at the N-aryl ring as well as with CF3 groups on the chelating backbone. This ligand modification significantly impacts the enhancement of Cu⋯Cu short contacts, which can be rationalized by using steric and electronic factors of the chelated ligand. We observed that this intramolecular cuprophilicity among [LCuI]3 complexes is primarily governed by the size of N-aryl ortho-substituents. These findings were well supported by X-ray crystallography, Raman spectroscopy, and Mayer bond order analysis. The electronic effects induced by the ligand modification on the LCuI fragment were investigated using CO and 2,4,6-CNC6H2Me3 as probe molecules. Corroborated by the FTIR and CV measurements, our results reveal that the β-thioketiminate SN chelators induce more pronounced changes in the electronic character of the LCuI fragment due to the presence of CF3 groups on the chelating backbone in comparison with the F or Cl substituents on the N-aryl ring. © 2024 The Royal Society of chemistry.

关键词： Ligands

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Rational Design of Ultrastable Conjugated Microporous Polymers Based on Pyrene and Perylene Units as High-Performance Organic Electrode Materials for Supercapacitor Applications

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ACS Applied Energy Materials 2023年第15期6卷 8277-8287页

作者： Singh, Poonam Nagendra Mohamed, Mohamed Gamal Chaganti, Swetha V. Sharma, Santosh U. Ejaz, Moshin Lee, Jyh-Tsung Kuo, Shiao-Wei Department of Materials and Optoelectronic Science Center for Functional Polymers and Supramolecular Materials National Sun Yat-Sen University Kaohsiung804 Taiwan Department of Chemistry Faculty of Science Assiut University Assiut71515 Egypt Department of Chemistry National Sun Yat-Sen University Kaohsiung80424 Taiwan International PhD Program for Science National Sun Yat-Sen University Kaohsiung80424 Taiwan Department of Medicinal and Applied Chemistry Kaohsiung Medical University Kaohsiung807 Taiwan

We successfully synthesized three perylene dianhydride (PDI)-based conjugated microporous polymers (CMPs), namely, Py-Ph-Pery, TPE-Ph-Pery, and TPA-Ph-Pery CMPs, through a Suzuki-Miyaura coupling reaction. The precursors used in the reaction contained brominated compounds of pyrene (Py), tetraphenylethylene (TPE), triphenylamine (TPA), and 1,4-benzeneboronic acid, which were coupled with redox-active PDI unit. To evaluate the thermal stability, molecular structure, and porosity properties of the synthesized CMPs, we conducted an examination of their Brunauer-Emmett-Teller isotherm, along with spectroscopic and microscopic analyses. These CMPs demonstrated moderate thermal stability based on thermogravimetric analysis. In terms of electrochemical performance, the Py-Ph-Pery CMP exhibited a high capacitance of 300 F g-1 (measured at 0.5 A g-1), indicating its excellent capacitive properties. Furthermore, the Py-Ph-Pery CMP displayed exceptional cycle stability at 10 A g-1, retaining more than 93% of its capacity over 5000 cycles. The findings illustrate the potential of these CMPs for reliable and durable energy storage applications. Additionally, we utilized synthesized CMPs to assess the electrochemical characteristics of a symmetric coin supercapacitor. The results further validate the suitability of these CMPs for practical electrical energy storage applications, highlighting their significant promise. © 2023 American Chemical Society.

关键词： Supercapacitor

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Recent advances in nanomaterials-based optical sensors for detection of various biomarkers (inorganic species, organic and biomolecules)

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Luminescence 2023年第7期38卷 954-998页

作者： Harshita Wu, Hui-Fen Kailasa, Suresh Kumar Department of Chemistry Sardar Vallabhbhai National Institute of Technology Gujarat Surat India Department of Chemistry National Sun Yat-Sen University Kaohsiung Taiwan School of Pharmacy College of Pharmacy Kaohsiung Medical University Kaohsiung Taiwan Institute of Medical Science and Technology National Sun Yat-Sen University Kaohsiung Taiwan International PhD Program for Science National Sun Yat-Sen University Kaohsiung Taiwan

This review briefly emphasizes the different detection approaches (electrochemical sensors, chemiluminescence, surface-enhanced Raman scattering), functional nanostructure materials (quantum dots, metal nanoparticles, metal nanoclusters, magnetic nanomaterials, metal oxide nanoparticles, polymer-based nanomaterials, and carbonaceous nanomaterials) and detection mechanisms. Furthermore, the emphasis of this review is on the integration of functional nanomaterials with optical spectroscopic techniques for the identification of various biomarkers (nucleic acids, glucose, uric acid, oxytocin, dopamine, ascorbic acid, bilirubin, spermine, serotonin, thiocyanate, Pb2+, Cu2+, Hg2+, F−, peptides), and cancer biomarkers (mucin 1, prostate specific antigen, carcinoembryonic antigen, CA15-3, human epidermal growth factor receptor 2, C-reactive protein, and interleukin-6). Analytical characteristics of nanomaterials-based optical sensors are summarized in the tables, providing the insights of nanomaterials-based optical sensors for biomarkers detection. Finally, the opportunities and challenges of nanomaterials-based optical analytical approaches for the detection of various biomarkers (inorganic, organic, biomolecules, peptides and proteins) are discussed. © 2022 John Wiley & Sons Ltd.

关键词： Biomarkers

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Taming Multiple Binding Poses in Alchemical Binding Free Energy Prediction: the β-cyclodextrin Host-Guest SAMPL9 Blinded Challenge

arXiv

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arXiv 2023年

作者： Khuttan, Sheenam Azimi, Solmaz Wu, Joe Z. Dick, Sebastian Wu, Chuanjie Xu, Huafeng Gallicchio, Emilio Department of Chemistry Brooklyn College The City University of New York United States PhD Program in Biochemistry Graduate Center of the City University of New York United States PhD Program in Chemistry Graduate Center of the City University of New York United States Roivant Sciences New YorkNY United States

We apply the Alchemical Transfer Method (ATM) and a bespoke fixed partial charge force field to the SAMPL9 bCD host-guest binding free energy prediction challenge that comprises a combination of complexes formed between five phenothiazine guests and two cyclodextrin hosts. Multiple chemical forms, competing binding poses, and computational modeling challenges pose significant obstacles to obtaining reliable computational predictions for these systems. The phenothiazine guests exist in solution as racemic mixtures of enantiomers related by nitrogen inversions that bind the hosts in various binding poses, each requiring an individual free energy analysis. Due to the large size of the guests and the conformational reorganization of the hosts, which prevent a direct absolute binding free energy route, binding free energies are obtained by a series of absolute and relative binding alchemical steps for each chemical species in each binding pose. Metadynamics-accelerated conformational sampling was found to be necessary to address the poor convergence of some numerical estimates affected by conformational trapping. Despite these challenges, our blinded predictions quantitatively reproduced the experimental affinities for the β-cyclodextrin host, less one case of the methylated derivative being an outlier. The work illustrates the challenges of obtaining reliable free energy data in in-silico drug design for even seemingly simple systems and introduces some of the technologies available to tackle them. © 2023, CC BY.

关键词： Cyclodextrins

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One-pot synthesis of near-infrared absorbing silver nanoprisms via a simple photochemical method using an ultraviolet-C light source

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Optical Materials 2024年 148卷

作者： Gunawardana, Niwan Ke, Chung-Yu Huang, Cheng-Liang Yang, Chung-Hsin Department of Chemistry National Sun Yat-sen University Kaohsiung804201 Taiwan Department of Applied Chemistry National Chiayi University 300 Syuefu Road Chiayi60004 Taiwan International PhD Program for Science National Sun Yat-sen University Kaohsiung804201 Taiwan

This study describes a simple one-pot photochemical method to synthesize triangular silver nanoprisms (T-AgNPs), for which a mixture of silver nitrate (AgNO3) and citrate was irradiated with an ultraviolet-C (UVC) lamp reactor. We successfully synthesized T-AgNPs with edge lengths ranging from 50 to 150 nm, showing a significant localized surface plasmon resonance (LSPR) band over a wavelength of 1200 nm. This photochemical reaction appears to be unrestricted by plasmon resonance conditions, allowing for the formation of colloidal T-AgNPs with an LSPR band in the near-IR region. In addition, this new method does not require any highly reactive reducing agents or initially prepared silver seed solution. The reduction of Ag+ ions by citrate is induced by UVC light, and the nascent Ag first undergoes nucleation to form spherical or quasi-spherical silver nanoparticles (S-AgNPs). Subsequently, continuous irradiation with UVC light facilitates the transformation of these S-AgNPs into T-AgNPs. The growth kinetics of the nanoparticles with different reaction conditions were examined using ultraviolet–visible–near-infrared spectroscopy and transmission electron microscopy. This new method offers a simple, efficient, and cost-effective means to synthesize T-AgNPs with near-IR LSPR, contributing to wider applications in the fields of optoelectronics, spectroscopics, photovoltaics, etc. © 2024 Elsevier B.V.

关键词： Silver compounds

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Variations in kinase and effector signaling logic in a bacterial two component signaling network

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Journal of Biological chemistry 2025年第6期301卷 108534页

作者： Swingle, Danielle Epstein, Leah Aymon, Ramisha Isiorho, Eta A. Abzalimov, Rinat R. Favaro, Denize C. Gardner, Kevin H. Structural Biology Initiative CUNY Advanced Science Research Center New YorkNY United States PhD. Program in Biochemistry The Graduate Center – City University of New York New YorkNY United States Department of Chemistry and Biochemistry City College of New York New YorkNY United States PhD. Programs in Biochemistry Biology and Chemistry The Graduate Center – City University of New York New YorkNY United States

The general stress response (GSR) protects bacteria from a wide range of stressors. In Alphaproteobacteria, GSR activation is coordinated by HWE/HisKA2 family histidine kinases (HKs), which can exhibit noncanonical structure and function. For example, while most light-oxygen-voltage sensor-containing HKs are light-activated dimers, the Rubellimicrobium thermophilum RT-HK has inverted "dark on, light off" signaling logic with a tunable monomer/dimer equilibrium. Here, we further investigate these atypical behaviors of RT-HK and characterize its downstream signaling network. Using hydrogen-deuterium exchange mass spectrometry, we find that RT-HK uses a signal transduction mechanism similar to light-activated systems, despite its inverted logic. Mutagenesis reveals that RT-HK autophosphorylates in trans, with changes to the Jα helix linking sensor and kinase domains affecting autophosphorylation levels. Exploring downstream effects of RT-HK, we identified two GSR genetic regions, each encoding a copy of the central regulator PhyR. In vitro measurements of phosphotransfer from RT-HK to the two putative PhyRs revealed that RT-HK signals only to one and does so at an increased intensity in the dark, consistent with its reversed logic. X-ray crystal structures of both PhyRs revealed a substantial shift within the receiver domain of one, suggesting a basis for RT-HK specificity. We probed further down the pathway using nuclear magnetic resonance to determine that the single NepR homolog interacts with both unphosphorylated PhyRs, and this interaction is decoupled from activation in one PhyR. This work expands our understanding of HWE/HisKA2 family signal transduction, revealing marked variations from signaling mechanisms previously identified in other GSR networks. © 2025 The Authors

关键词： Signaling

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Kinetics of primary mechanochemical covalent-bond-forming reactions

RSC Mechanochemistry

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RSC Mechanochemistry 2024年第1期1卷 11-32页

作者： Yerzhan S. Zholdassov Ryan W. Kwok Milan A. Shlain Monil Patel Mateusz Marianski Adam B. Braunschweig Advanced Science Research Center at the Graduate Center of the City University of New York 85 St Nicholas Terrace New York NY 10031 USA abraunschweig@gc.cuny.edu Department of Chemistry Hunter College 695 Park Ave New York NY 10065 USA PhD Program in Chemistry Graduate Center of the City University of New York 365 5th Ave New York NY 10016 USA PhD Program in Biochemistry Graduate Center of the City University of New York 365 5th Ave New York NY 10016 USA

Mechanical activation of reactions can reduce significantly the amounts of solvent and energy required to form covalent organic bonds. Despite growing interest in the field of mechanochemistry and increasing reports of mechanochemical synthesis of organic molecules, the fundamental question of how stresses activate covalent-bond-forming (CBF) reactions remains unresolved. This question remains unresolved because of the difficulties involved in measuring the applied forces and the reaction times in mechanochemical reactors, and the challenges related to deconvoluting microscopic (primary) and macroscopic (secondary) processes in the analysis of reaction kinetics. Here we discuss the use nanoscopic probe-microscope tips to explore the kinetics of CBF reactions. Because these experiments examine reactions on monolayers, surfaces, or nanoscopic particles, they circumvent secondary processes to isolate how stress affects the rates of the primary, CBF events. The major result of these studies is an emerging consensus that stress accelerates reactions by distorting organic molecules and in doing so, lowers reaction activation energies and alters reaction trajectories. This new understanding of how stresses activate reactions can be used to predict the outcomes of CBF mechanochemical reactions, which will lead to the wider adoption of sustainable mechanochemical processes by the synthetic community.

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Mechanistic insights of evaporation-induced actuation in supramolecular crystals (Sept, 10.1038/s41563-020-0799-0, 2020)

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NATURE MATERIALS 2021年第3期20卷 434-434页

作者： Piotrowska, Roxana Hesketh, Travis Wang, Haozhen Martin, Alan R. G. Bowering, Deborah Zhang, Chunqiu Hu, Chunhua T. McPhee, Scott A. Wang, Tong Park, Yaewon Singla, Pulkit McGlone, Thomas Florence, Alastair Tuttle, Tell Ulijn, Rein V. Chen, Xi Advanced Science Research Center (ASRC) at the Graduate Center of the City University of New York New York NY USA PhD Program in Chemistry The Graduate Center of the City University of New York New York NY USA Department of Pure and Applied Chemistry University of Strathclyde Glasgow UK PhD Program in Physics The Graduate Center of the City University of New York New York NY USA EPSRC Continuous Manufacturing and Crystallisation Future Research Hub c/o Strathclyde Institute of Pharmacy and Biomedical Sciences Technology Innovation Centre University of Strathclyde Glasgow UK Department of Chemistry New York University New York NY USA Department of Chemistry and Biochemistry Hunter College City University of New York New York NY USA Department of Chemical Engineering The City College of New York New York NY USA

A Correction to this paper has been published: https://***/10.1038/s41563-021-00950-3.

关键词： Condensed-matter physics Materials science Soft materials

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