Article
Chemistry, Multidisciplinary
Rebecca L. Spicer, Helen M. O'Connor, Yael Ben-Tal, Hang Zhou, Patrick J. Boaler, Fraser C. Milne, Euan K. Brechin, Guy. C. Lloyd-Jones, Paul J. Lusby
Summary: Coordination cage catalysis is a strategy that utilizes a cage as an exogenous catalyst, rather than relying on the endogenous binding of substrates. The cage alters the properties of a cofactor guest, which then transfers reactivity to the bulk-phase to catalyze reactions.
Article
Chemistry, Organic
Courtney Ngai, Bryce da Camara, Connor Z. Woods, Richard J. Hooley
Summary: A self-assembled Fe4L6 cage with internally oriented carboxylic acid functions can catalyze a variety of dissociative nucleophilic substitution reactions, showing strong selectivity for specific substrate shapes. The reactivity of the cage is highly influenced by even small structural differences in reactants, indicating a complex control of catalytic behavior.
JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Kuntrapakam Hema, Angela B. Grommet, Michal J. Bialek, Jinhua Wang, Laura Schneider, Christoph Drechsler, Oksana Yanshyna, Yael Diskin-Posner, Guido H. Clever, Rafal Klajn
Summary: The architecture of self-assembled host molecules can significantly impact the properties of the encapsulated guests. A Pd6L4 coordination host has been found to exhibit a Janus nature, transforming from a tube-shaped isomer to a cage-shaped host upon encapsulating tetrahedrally shaped guests. The reversible toggling between these vastly different isomers allows for control over the functional properties of coordination hosts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
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
Meng-Qi Wang, Qian Wang, Meng Chen, Da-Hui Qu
Summary: The study successfully fabricated a supramolecular luminescence system with tunable fluorescence emissions ranging from yellow to green by assembling a simple fluorescent molecule, 4-(pyren-1-yl)-1-(4-vinylbenzyl)pyridin-1-ium chloride (PPD), and cucurbit[n]uril (CB[n], n = 7, 8) via host-guest interactions. This system exhibited enhanced emission efficiency and longer fluorescence lifetime, making it suitable for applications in fluorescent ink and potential for information encryption materials.
Article
Chemistry, Multidisciplinary
Shihui Li, Rong Ma, Xin-Yue Hu, Hua-Bin Li, Wen-Chao Geng, Xianglei Kong, Chao Zhang, Dong-Sheng Guo
Summary: Macrocyclic delivery and therapeutics are important topics in supramolecular biomedicine. This study proposes a drug-in-drug strategy, using a functionalized macrocyclic host to encapsulate an active drug, forming a multifunctional supramolecular active pharmaceutical ingredient. This strategy enables synergistic anti-inflammatory effect in the treatment of rheumatoid arthritis.
ADVANCED MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Takehiro Hirao, Takeharu Haino
Summary: This review introduces the research directions for the synthesis of supramolecular fullerene polymers, including the linear, networked, helical arrays directed by the use of calix[5]arene-fullerene interactions, and the investigation of the calix[5]arene-fullerene interaction for control over the chain structures of covalent polymers.
CHEMISTRY-AN ASIAN JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Cristina Mozaceanu, Atena B. Solea, Christopher G. P. Taylor, Burin Sudittapong, Michael D. Ward
Summary: The binding of three isomeric guests inside an octanuclear cubic coordination cage host has been studied in different solvents. The binding free energy was found to be correlated with the polarity of the guests, with increased binding observed for more polar guests. The binding in water was further enhanced by a hydrophobic contribution, while the improvement in guest binding was found to be entropy-driven. These findings suggest that solvent effects play a crucial role in guest binding.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Miguel A. Soto, Veronica Carta, Ingrid Suzana, Brian O. Patrick, Francesco Lelj, Mark J. MacLachlan
Summary: Macrocycle engineering is a key topic in supramolecular chemistry. This study combines different approaches and post-synthetic modifications to transform a single tether into multiple rings. The macrocycles undergo redox reactions, allowing for control of conformational changes and host activity, enabling the capture and release of guests, ring transformations, and control of pseudorotaxane-to-pseudorotaxane conversions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yuan-He Li, Su-Lei Zhang, Yong Lu, Bo Xiao, Tian-Yu Sun, Qian-Qian Xu, Jia-Hua Chen, Zhen Yang
Summary: A highly enantioselective catalytic system for exo-Diels-Alder reactions was developed using bispyrrolidine diboronates(BPDB). Activated by various Lewis or Bronsted acids, BPDB can catalyze highly stereoselective asymmetric exo-Diels-Alder reactions. The catalyst can also distinguish between different binding sites to achieve highly regioselective reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Dan-Ni Yan, Li-Xuan Cai, Shao-Jun Hu, Yan-Fang Zhou, Li-Peng Zhou, Qing-Fu Sun
Summary: The adaptive self-assembly and host-guest catalysis of a new water-soluble organo-palladium host are reported. The host undergoes conformational changes upon guest binding, allowing for efficient and selective catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Organic
Nan-Fang Mo, Ying Zhang, Zheng-Hui Guan
Summary: An asymmetric organocatalyzed three-component Povarov reaction has been developed to construct azaspirocycles. A chiral phosphoric acid catalyst with a unique structure was highly efficient in the reaction, leading to a wide range of azaspirocycles in high yields and excellent enantioselectivities. This reaction has expanded the scope of the traditional Povarov reaction.
Article
Chemistry, Multidisciplinary
Wenbing Cao, Haoyu Wang, Mao Quan, Yuxuan Li, Yeyu Su, Yuhang Li, Wei Jiang, Tao Liu
Summary: We identified a high-affinity host-guest pair and developed a molecular-recognition strategy to control tetrazine reactions. This strategy efficiently and reversibly regulates the reactivity of tetrazine, enabling site-specific protein labeling and dual conjugate formation in living organisms.
Review
Chemistry, Applied
Maxim G. Vinogradov, Olga V. Turova, Sergei G. Zlotin
Summary: This review retrospectively considers the pivotal achievements and recent advances in catalytic asymmetric aza-DAR reported up to 2020, showcasing their potency for enantioselective synthesis of useful chiral piperidine, quinoline, pyridazine, oxazine, and oxadiazine derivatives. The data are systematized based on key electron transfer modes and attainable heterocyclic products, with significant attention to activation strategies and plausible reaction pathways over stereoselective cyclization processes. The review contains 310 references and 122 synthetic schemes.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Review
Chemistry, Multidisciplinary
Kaiya Wang, Jacobs H. Jordan, Krishnasamy Velmurugan, Xueqi Tian, Minzan Zuo, Xiao-Yu Hu, Leyong Wang
Summary: Pillarenes, with their useful features such as rigidity, capaciousness, hydrophobic cavities, and exposed functional groups, have become increasingly popular since their discovery in 2008. This Minireview focuses on the use of functionalized Pillarenes and their assembled supramolecular materials in catalysis, providing insights into their mechanisms and potential applications. Subdivided topics include catalysis promoted by the Pillarene rim/cavity, Pillarene-based nanomaterials, and Pillarene-based polymeric materials, making it the first comprehensive overview on Pillarene-based catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Jilin Fan, Mingjun Xuan, Pengkun Zhao, Mark Loznik, Junlin Chen, Fabian Kiessling, Lifei Zheng, Andreas Herrmann
Summary: The development of ultrasound-responsive microcapsule structures has enabled the controlled delivery of macromolecular cargoes for biomedical applications. However, delivering small molecular cargoes using microcapsules has been a challenge due to drug leakage. In this study, we proposed a new strategy by using nanodrugs encapsulated in microcapsules, which prevented drug leakage and provided responsiveness to ultrasound. Furthermore, we demonstrated the activation of antibacterial activity by ultrasound using the nanodrug@Microcapsules.
Article
Chemistry, Multidisciplinary
Rundong Ding, Qing Liu, Lifei Zheng
Summary: Metal-organic frameworks UiO-66 and UiO-66-NH2 were synthesized and their piezoelectric properties were characterized. It was found that under mechanical agitation, UiO-66 and UiO-66-NH2 acted as electron donors to reduce aryl diazonium salts, generating aryl radical species, which further reacted with bis(pinacolato)diborane or heteroarenes to produce desired products. The reactions mediated by UiO-66-NH2, which had better piezoelectric property, showed higher efficiency than those promoted by UiO-66. The convenient regeneration of spent catalysts without loss of activity was achieved due to the repairability of metal-organic frameworks. Mechanistic studies revealed the involvement of a radical pathway in these transformations.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Yu Zhou, Silvia P. Centeno, Kuan Zhang, Lifei Zheng, Robert Goestl, Andreas Herrmann
Summary: This study reports the development of a series of ratiometric optical force probes (OFPs) based on fluorescent-protein-dye and protein-protein conjugates, and their incorporation into genetically engineered bio-glues. The OFPs efficiently modulate Forster resonance energy transfer upon force application, reporting on force-induced molecular alterations independent of concentration and fluorescence intensity. By fluorescence spectroscopy in solution and in the solid state, as well as fluorescence lifetime imaging microscopy, stress concentrations are visualized and adhesive and cohesive failure in the fracture zone is differentiated.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kai-Oliver Brenske, Meike Emondts, Sven T. Hoernig, Sinan Panitz, Maria I. Pieper, Aron Ligori, Alexander Schacht, Johanna Henkel, Juergen Klankermayer, Andreas Herrmann
Summary: Enhancing the NMR signals of biomacromolecules by hyperpolarization is challenging due to the requirement of specific catalytic interactions and the large size and insolubility of the biomolecules. In this study, we achieved unprecedented hyperpolarization of the cancer-targeting DNA aptamer AS1411 by screening different molecular motifs and adjusting the polarity of AS1411. The results have the potential to advance hyperpolarized molecular imaging technology for disease detection.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Michele Partipilo, Jacob J. Whittaker, Nicola Pontillo, Jelmer Coenradij, Andreas Herrmann, Albert Guskov, Dirk Jan Slotboom
Summary: In this study, a chemically resistant formate dehydrogenase (Fdh(SNO)) was discovered, which is specific for NAD(+). Through rational engineering, the protein was modified to have better catalytic efficiency for reducing NADP(+). The findings of this study provide a method and theoretical basis for utilizing Fdh(SNO) in the (bio)manufacture of value-added chemicals.
Article
Chemistry, Multidisciplinary
Aman Ishaqat, Xiaofeng Zhang, Qing Liu, Lifei Zheng, Andreas Herrmann
Summary: In this study, we developed a DNA circuit that delivers CpG oligodeoxynucleotides (CpG ODNs) with immunostimulation function. The circuit utilizes a complementary DNA (cDNA) strand to deactivate the biological function of CpG ODNs, and T7 exonuclease to activate and release the CpG ODN as an active molecule. We investigated various factors that influenced the circuit's behavior and demonstrated its potential in controlling pharmacological activity and drug delivery.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaoyi Wang, Tina-Marie Thomas, Ren Ren, Yu Zhou, Peng Zhang, Jingjing Li, Shenglin Cai, Kai Liu, Aleksandar P. Ivanov, Andreas Herrmann, Joshua B. Edel
Summary: The analysis of proteins and their interactions at the single-molecule level has important implications for understanding biological processes and diseases, especially for proteins found in low copy numbers in biological samples. Nanopore sensing is a label-free detection technique that is well-suited for applications such as studying protein-protein interactions, biomarker screening, drug discovery, and protein sequencing. However, current limitations in protein nanopore sensing pose challenges in controlling protein translocation and relating protein structures and functions to nanopore readouts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Mingjun Xuan, Jilin Fan, Vu Ngoc Khiem, Miancheng Zou, Kai-Oliver Brenske, Ahmed Mourran, Rostislav Vinokur, Lifei Zheng, Mikhail Itskov, Robert Goestl, Andreas Herrmann
Summary: Polymer mechanochemistry is a promising technology to convert mechanical energy into chemical functionality by breaking bonds. In this study, a microbubble system was used to accelerate the mechanochemical activation of disulfides, and optimization conditions were identified.
ADVANCED MATERIALS
(2023)
Article
Virology
Markus Kastner, Andreas Karner, Rong Zhu, Qiang Huang, Andreas Geissner, Anne Sadewasser, Markus Lesch, Xenia Woermann, Alexander Karlas, Peter H. Seeberger, Thorsten Wolff, Peter Hinterdorfer, Andreas Herrmann, Christian Sieben
Summary: The study compared influenza virus receptor specificity with virus binding to live cells using glycan arrays and single-virus force spectroscopy. The findings revealed that the receptor binding preference of the virus does not necessarily reflect its specificity to cells. Single-virus force spectroscopy was proposed as a tool to understand the cell binding preference of influenza A viruses.
Article
Materials Science, Biomaterials
Jianfei Tu, Qing Liu, Shengye You, Zhuojun Meng, Shiji Fang, Binhong Yu, Xumin Chen, Yu Zhou, Lulu Zeng, Andreas Herrmann, Gang Chen, Jianliang Shen, Lifei Zheng, Jiansong Ji
Summary: Heparin is a widely used anticoagulant, but its effect needs to be reversed to prevent side effects. Protamine sulfate (PS) is the only licensed antidote, but it has severe adverse effects. This study shows that supercharged polypeptides could be a promising alternative to PS. The polypeptide with 72 charges (K72) exhibited excellent heparin-neutralizing behavior comparable to PS, with negligible toxic effects.
BIOMATERIALS SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Roman A. Barmin, Mirjavad Moosavifar, Anshuman Dasgupta, Andreas Herrmann, Fabian Kiessling, Roger M. Pallares, Twan Lammers
Summary: Ultrasound (US) is widely used for diagnostic imaging and treatment, and polymeric materials with cavitation nuclei properties can enhance US imaging and promote local drug delivery. This review discusses engineered polymeric materials, such as microbubbles and gas-releasing nanoparticles, that respond to US and their formulation aspects. It focuses on microbubbles and explores the chemical toolbox to enhance their performance in US imaging and drug delivery. The review also summarizes the emerging applications of polymeric microbubbles in molecular imaging, sonopermeation, and gas and drug delivery, highlighting their potential in US imaging and therapy.
Article
Chemistry, Physical
Jilin Fan, Mingjun Xuan, Pengkun Zhao, Mark Loznik, Junlin Chen, Fabian Kiessling, Lifei Zheng, Andreas Herrmann
Summary: The development of ultrasound-responsive microcapsule structures has provided new insights into the development of ultrasound triggered small molecule drug delivery assisted by metallic nanoparticles. By employing nanodrugs encapsulated in microcapsules, drug leakage can be prevented and the delivery system can respond to high-intensity focused ultrasound.
