Review
Chemistry, Multidisciplinary
Yinlin Chen, Wanpeng Lu, Martin Schroder, Sihai Yang
Summary: Metal-organic frameworks (MOFs) are hybrid porous materials with high crystallinity, extensive surface area, and adjustable pore sizes. They have various applications in gas adsorption, separation, and catalysis. The design flexibility of organic ligands and precise engineering of uniform pore environments in MOFs enable rich interactions between the material and adsorbed gas molecules, which greatly impact the overall performance.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Biochemistry & Molecular Biology
Zhaoxi Sun, Qiaole He, Zhihao Gong, Payam Kalhor, Zhe Huai, Zhirong Liu
Summary: Atomic-level understanding of host-guest interactions is crucial in supramolecular chemistry. The remarkable guest binding behavior of Cucurbiturils makes them promising drug carriers. Computational investigations and comparisons of charge models and force fields provide guidelines for theoretical modeling of host-guest binding.
Article
Chemistry, Multidisciplinary
Dilanka V. D. Walpita Kankanamalage, Jennifer H. T. Tran, Noah Beltrami, Kun Meng, Xiao Zhou, Pravin Pathak, Lyle Isaacs, Alexander L. Burin, Mehnaaz F. Ali, Janarthanan Jayawickramarajah
Summary: This study introduces a synthetic surrogate called host-guest-driven toehold-mediated strand displacement (HG-TMSD) that utilizes bioorthogonal interactions to control the process of DNA strand displacement. The HG-TMSD method can be finely modulated by changing the structure of the input sequence and can also be regulated by competing small-molecule guests. It can be integrated into functional devices for controlling enzyme activity and detecting specific microRNA.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Shinnosuke Horiuchi, Takumi Yamaguchi, Jacopo Tessarolo, Hirotaka Tanaka, Eri Sakuda, Yasuhiro Arikawa, Eric Meggers, Guido H. Clever, Keisuke Umakoshi
Summary: In this study, we achieved symmetry-breaking self-assembly of a defined C-1-symmetric supramolecular structure by the synergistic effects of weak binding forces. The flexible capsule framework undergoes a large structural change upon guest binding, forming a distorted resorcin[4]arene hexameric capsule with an asymmetric cavity. The location of the chiral guest in the anisotropic environment leads to modulation of its Electric Dipole (ED) and Magnetic Dipole (MD) transition moments, resulting in increased emission quantum yield and circularly polarized luminescence.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Hector Fernandez-Caro, Alejandro Mendez-Ardoy, Javier Montenegro
Summary: The intracellular reconfiguration of nanoparticles by a host/guest mechanism with biocompatible oligomeric competitors has been achieved, allowing for the direct exchange of pendants at the surface of nanoparticles and the intracellular dynamic chemical reconfiguration of biocompatible colloidal systems.
Article
Physics, Multidisciplinary
Yue Xin, Qiao Shi, Ke Xu, Zhi-Sen Zhang, Jian-Yang Wu
Summary: Mechanical properties of clathrate hydrates are influenced by the ability of host-guest molecules to form hydrogen bonds and the polarity of guest molecules, with structures containing guests with weak hydrogen bonding ability exhibiting brittle failure, while structures entrapping guests with strong hydrogen bonding ability showing ductile failure.
FRONTIERS OF PHYSICS
(2021)
Article
Chemistry, Physical
Peng Lei, Long Zhao, Luan He, Fengying Zhao, Xunwen Xiao, Bin Tu, Qingdao Zeng
Summary: The study investigated the impact of temperature on the self-assembled structures of TTF-C6 molecules and found that temperature-induced structural transitions can capture different guest molecules. The experimental results were verified through density functional theory (DFT) calculations.
APPLIED SURFACE SCIENCE
(2021)
Review
Agriculture, Multidisciplinary
Wenjie Li, Weiwei Xu, Siyun Zhang, Jia Li, Juan Zhou, Demei Tian, Jing Cheng, Haibing Li
Summary: Significant progress has been made in the research on drug encapsulation and release based on supramolecular macrocycles, laying a solid foundation for the development of novel nanopesticide preparations.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2022)
Article
Chemistry, Applied
Rui Liu, Xiaoli Qin, Xiong Liu, Yonghua Wang, Jinfeng Zhong
Summary: The physicochemical properties and interactions of the complex of oleic acid (OA) and beta-cyclodextrin (beta-CD) were studied using experimental and computational methods. The study confirmed the stability improvement of the OA/beta-CD complex and the formation of hydrogen bonds between the carboxyl group of OA and the beta-CD cavity. This research provides a theoretical basis for the development of nutritional supplements containing unsaturated fatty acids encapsulated by beta-CD.
Article
Engineering, Environmental
Ki Hun Park, Dong Hyun Kim, Minjun Cha
Summary: A new structure II (sII) hydrate former, cyclobutanemethanol (CBM), was discovered for potential gas storage applications. The binary (CBM + CH4) hydrate showed higher thermodynamic stability and superior CH4 storage capacity compared to other hydrates, indicating potential for gas storage applications.
CHEMICAL ENGINEERING JOURNAL
(2021)
Review
Chemistry, Inorganic & Nuclear
Xi Yang, Di Yuan, Jinhong Hou, Adam C. Sedgwick, Suying Xu, Tony D. James, Leyu Wang
Summary: The field of supramolecular chemistry has rapidly expanded and become highly influential in various areas like biomedicine, energy materials, catalysis, and sensing. The combination of host/guest chemistry with functional inorganic nanoparticles has led to many new applications in drug delivery, bioimaging, and sensing. Recent progress in the development of organic/inorganic supramolecular nano-systems incorporating host/guest chemistry has been summarized, highlighting their applications in drug delivery, biological imaging, and sensing.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Helena Butkiewicz, Sandra Kosiorek, Volodymyr Sashuk, Oksana Danylyuk
Summary: The study explores the use of carboxylated pillar[5]arene in solid-state supramolecular chemistry, revealing its inclusion and self-assembly behavior in forming crystalline host-guest complexes with viologen derivatives. The unique distribution of carboxylic and carboxylate substituents on pillar[5]arene allows for self-assembly via different supramolecular synthons.
Article
Polymer Science
Yu-Liang Lin, Sheng Zheng, Chia-Wei Chang, Min-Jie Lee, Yi-Fan Chen, Jiun-Tai Chen
Summary: In this study, versatile and on-demand photocontrollable ionic conductive nanocomposite hydrogels were successfully synthesized via host-guest chemistry. The hydrogels showed higher conductivity under visible light irradiation and lower conductivity under UV irradiation, which could be further manipulated by adjusting the surface-area-to-volume ratio of the nanopores and the alkyl chain length of the anions.
Article
Chemistry, Multidisciplinary
David E. Clarke, Guanglu Wu, Ce Wu, Oren A. Scherman
Summary: Control of spatial and temporal behavior of peptide segments is crucial in fabricating functional peptide-based materials and nanostructures. Complex sequence design and inclusion of unnatural amino acids or synthetic modifications are often required to achieve desired structures. In this study, the structural properties of 1:1 inclusion complexes between specific oligopeptides and CB[8] were investigated, showing induction of turns and tunable structural chirality by altering peptide sequences. Extension of peptide sequence binding with CB[8] was also explored as a simple method to construct a peptide hairpin.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Laurent Severy, Jacek Szczerbinski, Mert Taskin, Isik Tuncay, Fernanda Brandalise Nunes, Chiara Cignarella, Gabriele Tocci, Olivier Blacque, Jurg Osterwalder, Renato Zenobi, Marcella Iannuzzi, S. David Tilley
Summary: The study demonstrates a non-covalent 'click' chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces through host-guest complexation. This efficient method enables the replacement and reuse of molecular catalysts, enhancing the attractiveness of electrosynthetic systems.
Article
Biochemistry & Molecular Biology
Kaylin G. Fosnacht, Matthew M. Cerda, Emma J. Mullen, Hannah C. Pigg, Michael D. Pluth
Summary: Persulfides are important reactive sulfur species that are associated with the biological functions of H2S. Directly studying persulfides is difficult due to their nucleophilic and electrophilic character. Persulfide donors are needed to generate persulfides in situ for investigating their effects.
ACS CHEMICAL BIOLOGY
(2022)
Review
Chemistry, Multidisciplinary
Hazel A. Fargher, Tobias J. Sherbow, Michael M. Haley, Darren W. Johnson, Michael D. Pluth
Summary: The study demonstrates that C-H midline bonds are often overlooked but important stabilizing interactions, meeting the definition of hydrogen bonding. By comparing with traditional hydrogen bond donors and acceptors, as well as investigating the effect of metal bonding, the generality of C-H midline hydrogen bonding can be established and used for identification in diverse systems.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Tobias J. Sherbow, Wen Fu, Lizhi Tao, Lev N. Zakharov, R. David Britt, Michael D. Pluth
Summary: S/N crosstalk species derived from the interconnected reactivity of H2S and NO play important roles in signaling, transport, and regulatory processes. Simple Fe2+ ions react with thionitrite and perthionitrite to form a dinitrosyl iron complex, and can also produce a hydrosulfido mononitrosyl iron complex through specific reactions. Furthermore, the dinitrosyl iron complex serves as a precursor for nitrosylated Fe-S clusters.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Kaylin G. Fosnacht, Matthew D. Hammers, Mary S. Earp, Annie K. Gilbert, Michael D. Pluth
Summary: A new fluorescent probe CT-MeRhoAz has been developed for the detection of H2S. The probe shows high selectivity and cell-trapping ability for H2S, and exhibits a significantly enhanced fluorescent signal in the presence of H2S.
CHEMISTRY-AN ASIAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Arman C. Garcia, Lev N. Zakharov, Michael D. Pluth
Summary: In this study, using cucurbit[7]uril (CB[7]) as a hydrophobic host, it was demonstrated that S8 can be encapsulated to form a 1:1 host-guest complex, and the encapsulated S8 can be reduced to H2S by attacking thiols. The study also showed that CB[7]/S8 can increase sulfane sulfur levels in live cells. This work suggests a general activation mechanism of S8 by hydrophobic motifs, which may have implications for understanding the translocation and trafficking of reactive sulfur species (RSS).
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Organic
Haley M. Smith, Michael D. Pluth
Summary: Recent efforts have focused on the development of small molecule donors that can release hydrogen sulfide (H2S), an important biological signaling molecule. In particular, 1,2,4-thiadiazolidin-3,5-diones (TDZNs) have shown promising efficacy in H2S-mediated relaxation. It has been discovered that TDZNs release carbonyl sulfide (COS) efficiently, which can be converted to H2S by the enzyme carbonic anhydrase (CA), rather than directly releasing H2S as previously thought.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Annie K. Gilbert, Michael D. Pluth
Summary: This study presents a library of organelle targeted H2S donors that can deliver H2S to specific subcellular organelles, showing enhanced protection against organelle-specific stress.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Keyan Li, Lev N. Zakharov, Michael D. Pluth
Summary: This study reports the synthesis, isolation, spectroscopic and structural characterization, and reactivity of persulfide (RSS-), perselenide (RSeSe-), thioselenide (RSSe-), and selenosulfide (RSeS-) anions. The chemical structures of these anions were confirmed by X-ray crystallography and NMR spectroscopy. The reactions of these anions with other molecules were also investigated, revealing their reactivity and detoxifying effects.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Michael M. Wade Wolfe, Michael D. Pluth
Summary: We investigated the differential oxidative and nucleophilic chemistry of reactive sulfur and oxygen anions using a simple reducing electrophile. The reaction with SSNO- resulted in the formation of a complex mixture of phosphorus products in the P(V) oxidation state. The selectivity for oxidation to P=S/P=O products or transformation to P-2 species was determined by the phosphine stoichiometry.
INORGANIC CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Haley M. Smith, Michael D. Pluth
Summary: This Perspective paper discusses the important advances and opportunities in the detection and quantification of H2S, focusing on the field of chemical biology. It presents commonly used methods for H2S detection and quantification in biological samples, highlighting the strengths and limitations of each technique. The goal of the paper is to simplify the decision-making process and identify key unmet needs and opportunities in the field.
Article
Chemistry, Inorganic & Nuclear
Michael M. Wade Wolfe, Michael D. Pluth
Summary: In this study, we investigated the different oxidative and nucleophilic chemistry between reactive sulfur and oxygen anions (SSNO-, SNO-, NO2-, S4(2)-, and HS-) using the reducing electrophile PPh2Cl. When SSNO- reacts with PPh2Cl, a complex mixture of mono and diphosphorus products exclusively in the P(V) oxidation state is formed. We found that the phosphine stoichiometry determines the selectivity for oxidation to P=S/P=O products or transformation to P-2 species. Interestingly, only chalcogen atoms are incorporated into the phosphorus products, while nitrogen is released as NO gas.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Turner D. D. Newton, Keyan Li, Jyoti Sharma, Pier Alexandre Champagne, Michael D. D. Pluth
Summary: Hydrogen selenide (H2Se) is an important precursor in biological organoselenium compound synthesis and can also act as a potential gasotransmitter and bioregulator. Researchers have investigated the release of H2Se from selenocarbamates and found that unlike their thiocarbamate counterparts, selenocarbamates release H2Se directly along with the formation of isocyanates, instead of releasing carbonyl selenide (COSe) as an intermediate. Computational studies support this finding by showing a significant energy difference between the H2Se and COSe release pathways. This study provides new insights into H2Se delivery and the reactivity differences between sulfur and selenium species.
Article
Chemistry, Multidisciplinary
Arman C. Garcia, Michael D. Pluth
Summary: It is found that surfactants can solubilize sulfur and promote its reduction to hydrogen sulfide by thiols. Anionic and cationic surfactants interact differently with intermediate sulfur carriers, indicating the impact of specific hydrophobic microenvironments on reactive sulfur species.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Grace M. Kuhl, Douglas H. Banning, Hazel A. Fargher, Willow A. Davis, Madeline M. Howell, Lev N. Zakharov, Michael D. Pluth, Darren W. Johnson
Summary: This article introduces a new approach for the direct and reversible detection and measurement of HS- in water, using supramolecular host-guest interactions and ChemFET architectures. By using a ChemFET material containing bambus[6]uril macrocycles as the HS- receptor, the authors experimentally determined the placement of HS- in the Hofmeister series. These results demonstrate the potential of this new method in addressing the challenge of HS- detection and measurement.
Article
Chemistry, Inorganic & Nuclear
Tobias J. Sherbow, Keyan Li, Lev N. Zakharov, Michael D. Pluth
Summary: This paper investigates the coordination chemistry of the [B-Ph((t)BuIm)(3)](1-) ligand with redox-inert zinc and explores the behavior of the zinc metal center in a strong coordinating environment. Different zinc coordination complexes with various ligand substitutions were obtained through a series of reactions.
DALTON TRANSACTIONS
(2022)
