Review
Chemistry, Physical
Jorn D. Steen, Daniel R. Duijnstee, Wesley R. Browne
Summary: Molecular switching has become a key functionality in addressable materials and surfaces. However, the wide variation in interfaces studied, from single-molecule devices to two-dimensional self-assembled monolayers and thin films, poses challenges in their use and characterization. The low number density of molecules on modified interfaces and the complexity of characterizing molecular function further complicate the analysis. This review discusses the techniques and approaches used for characterizing molecular switches applied to interfaces and emphasizes the importance of understanding the limitations and quirks of specific techniques through the use of model compounds.
SURFACE SCIENCE REPORTS
(2023)
Review
Chemistry, Multidisciplinary
Anirban Mondal, Ryojun Toyoda, Romain Costil, Ben L. Feringa
Summary: This article summarizes the design, synthesis, and dynamic properties of molecular machines, and presents methods for controlled switching or rotation of different classes of atropisomers under chemical stimulus, categorizing them as molecular switches, rotors, motors, and autonomous motors. Future perspectives and challenges for building sophisticated molecular machines are also provided.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Fan Xu, Ben L. Feringa
Summary: Photoresponsive supramolecular polymers are highly organized assemblies with photosensitive molecules as monomers, showing reversible changes in geometry, dipole moment, and chirality upon light stimuli. They have broad applications in smart materials, including light-driven soft actuators, fluorescent anticounterfeiting, and light-triggered electronic devices. This review focuses on the light-activated molecules used in photoresponsive supramolecular polymers and the different changes induced by light. It also highlights the disassembly, reassembly, actuation, emission, and chirality transfer of these polymers. Future opportunities and challenges, such as using visible/near IR light and enabling biomedical applications, are also discussed.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jian Sun, Wei Hu, Lanying Zhang, Ruochen Lan, Huai Yang, Deng-Ke Yang
Summary: This study introduces a novel overcrowded alkene motor that can achieve photoisomerization under UV exposure, and modulate the photodynamic storage modulus through dynamic stable-unstable isomerization. This leads to light-driven self-oscillating behavior from chaotic to regular movement in polymer networks.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Polymer Science
Peiqiong Zhao, Meigui Deng, Yongfang Yang, Jimin Zhang, Yue Zhang
Summary: Amphiphilic graft copolymers display interesting self-assembly behaviors, with their molecular architectures playing a significant role in shaping the morphology and functionality of the self-assemblies. The Passerini reaction and molecular recognition are introduced for the synthesis of functional thermoresponsive graft copolymers, aiming to enable the fabrication of well-defined graft copolymers with desired functional groups for potential applications in nanocarrier design. The resulting biohybrid graft copolymer can self-assemble into peptide-modified polymersomes at temperatures above its lower critical solution temperature.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Review
Chemistry, Multidisciplinary
Alexis Perrot, Emilie Moulin, Nicolas Giuseppone
Summary: The implementation of molecular switches and motors in soft materials to generate macroscopic actuation under external stimulation requires consideration of important structural and dynamic aspects at all length scales. Different ratcheting strategies are highlighted for these actuators to enable unidirectional cyclic motion and continuous increase in work output.
TRENDS IN CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Valeriy P. Shendrikov, Anna S. Alekseeva, Erik F. Kot, Konstantin S. Mineev, Daria S. Tretiakova, Abdulilah Ece, Ivan A. Boldyrev
Summary: This study describes azophenylindane based molecular motors, which have different rotamers in trans and cis configurations. The behaviors of these motors were investigated experimentally and computationally, revealing that the conversion of the motor results in a mixture of isomers. Some cis-rotamers can directly convert to each other, while others require conversion via trans-configuration. The motion of these motors is similar to a mixing machine, with the indane group acting as a base and the phenol group as a beater. These aphin-switches may have promising applications in advanced biological systems or in cases where molecular packing disordering is desired, such as lipid bilayers.
Article
Nanoscience & Nanotechnology
Richard Korytar, Ferdinand Evers
Summary: In this paper, an alternative driving agent for molecular rotors is presented, which works even when angular momentum is conserved. Through quantitative analysis using a classical model, it is shown that in the presence of chirality, the rotor undergoes directed motion as long as the incident current exceeds a threshold value.
BEILSTEIN JOURNAL OF NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Ao Juan, Siyang Lin, Yanrong He, Qingyan Fan, Jinbao Guo
Summary: Reflective color switching and fluorescence tuning of cholesteric liquid crystal cells induced by upconversion luminescence were investigated. It was found that under 980 nm NIR light exposure, both the color and fluorescence intensity of the cells could be controlled effectively.
Article
Nanoscience & Nanotechnology
Shuntaro Amano, Stefan Borsley, David A. Leigh, Zhanhu Sun
Summary: This article discusses the complex functions exhibited by biological and chemical systems under non-equilibrium conditions, as well as the mechanisms of energy extraction and utilization through chemical engines. By linking different examples using a common conceptual framework, it explores future challenges and potential applications. The focus of the research is on how to utilize these mechanisms to operate chemical engines.
NATURE NANOTECHNOLOGY
(2021)
Article
Physics, Multidisciplinary
Rick Bebon, Ulrich S. Schwarz
Summary: The article explores the computation of complex energy landscapes in biological systems, particularly their effects on first-passage times (FPTs). The authors propose a method to identify the most relevant features of energy landscapes by coarse-graining the Fokker-Planck equation to a master equation and decomposing its FPTs iteratively. They apply this method to the electrostatic interaction between two nonmuscle myosin II (NM2) rods and identify the most relevant energy barriers for their self-assembly into NM2 minifilaments and how they change under force.
NEW JOURNAL OF PHYSICS
(2022)
Article
Robotics
Hongyue Zhang, Zesheng Li, Changyong Gao, Xinjian Fan, Yuxin Pang, Tianlong Li, Zhiguang Wu, Hui Xie, Qiang He
Summary: Neutrophil-based microrobots, constructed by phagocytosis of drug-loaded magnetic nanogels enveloped in Escherichia coli membrane, exhibit controllable intravascular movement and can autonomously aggregate in the brain by positive chemotactic motion along the gradient of inflammatory factors. These dual-responsive neutrobots show promise for targeted drug delivery to inhibit tumor cell proliferation compared to traditional drug injection, leveraging the biological characteristics of natural neutrophils that artificial microrobots cannot replicate.
Review
Chemistry, Multidisciplinary
Liang Qiu, Xinyue Han, Chengfen Xing, Ulrich Glebe
Summary: The combination of biomolecules and synthetic polymers offers great potential for developing innovative materials and promoting the application of biomolecules in various fields. Polymerization-induced self-assembly (PISA), as an efficient technique, allows for the fabrication of advanced polymer-based biohybrid nanostructures (PBBNs). This review presents current strategies for preparing PBBNs using the PISA technique, including grafting-from and grafting-through methods, as well as biomolecule encapsulation.
Article
Chemistry, Multidisciplinary
Indrajit Maity, Dharm Dev, Kingshuk Basu, Nathaniel Wagner, Gonen Ashkenasy
Summary: This study presents a new cascade pathway utilizing a switchable peptide-based replicating network to regulate various features of Au nanoparticle shape and assembly, bridging the fields of systems chemistry and nanotechnology for dynamically controlled design of functional materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Kody D. Wolfe, Avi Gargye, Faustin Mwambutsa, Long Than, David E. Cliffel, G. Kane Jennings
Summary: Efficient electron transfer between biomolecules and electrode interfaces is crucial for many bioelectrochemical processes. By leveraging electrostatic interactions, PSI protein complexes can be deposited as monolayers within a short time, and high loadings of PSI between PEDOT:PSS layers can be achieved through layer-by-layer deposition, improving electron collection rates.
Review
Chemistry, Multidisciplinary
David Villaron, Sander J. Wezenberg
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Review
Chemistry, Multidisciplinary
Sander J. Wezenberg
Article
Chemistry, Multidisciplinary
Filippo Tosi, Jose Augusto Berrocal, Marc C. A. Stuart, Sander J. Wezenberg, Ben L. Feringa
Summary: This study demonstrates the synthesis and self-assembly of a chiral bis(urea) amphiphile, revealing that chirality plays a crucial role in controlling morphology. The molecular-scale chiral information is translated into mesoscopic twisted ribbons in water. The system exhibits thermo-responsive aggregation behavior, with a transition from ribbons to vesicles upon heating, and morphology can be easily controlled by varying the enantiomeric excess of the amphiphile.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Fabio Castiglioni, Wojciech Danowski, Jacopo Perego, Franco King-Chi Leung, Piero Sozzani, Silvia Bracco, Sander J. Wezenberg, Angiolina Comotti, Ben L. Feringa
Article
Chemistry, Multidisciplinary
Fan Xu, Lukas Pfeifer, Stefano Crespi, Franco King-Chi Leung, Marc C. A. Stuart, Sander J. Wezenberg, Ben L. Feringa
Summary: The study focused on controlling supramolecular polymerization using photoresponsive stiff-stilbene-based bis-urea monomers in organic solvents, achieving fast light-triggered depolymerization-polymerization and reversible gel formation. Precise control over supramolecular polymerization and gelation was achieved by manipulating the high photostationary states of cis-trans isomerization. The research also revealed a kinetically controlled nucleation-elongation mechanism for temperature-dependent and photoinduced supramolecular polymerization in organic solvents.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
David Villaron, Nol Duindam, Sander J. Wezenberg
Summary: The donor-acceptor substituted stiff-stilbene molecule undergoes isomerization induced by visible light and the process is inhibited by protonation, which restricts the photochromic properties. Furthermore, the addition of a mild acid triggers fast thermal back-isomerization, providing a new avenue for the stiff-stilbene photoswitches.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Sander J. Wezenberg, Li-Jun Chen, Jasper E. Bos, Ben L. Feringa, Ethan N. W. Howe, Xin Wu, Maxime A. Siegler, Philip A. Gale
Summary: Membrane transport proteins have important regulatory functions in biology and can respond to environmental stimuli. Using bis(thio)ureas derived from stiff-stilbene, photocontrol of transmembrane transport and electric potential has been demonstrated through UV-vis and H-1 NMR spectroscopy. The (Z)-isomers show stronger binding properties and are more active in transmembrane transport compared to the (E)-isomers.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Nanoscience & Nanotechnology
Stefan Mommer, Sander J. Wezenberg
Summary: Supramolecular anion binding to squaramide crosslinkers in poly(N,N-dimethylacrylamide) gel networks enhances swelling and allows reversible chemically driven actuation. The volume swelling ratio of the gels is shown to depend on both the type of anion and its concentration. H-1 NMR and UV-vis titrations with the squaramide crosslinkers reveal a relationship between anion binding affinity and the concentration-dependent swelling behavior. Gel swelling is shown to be reversible, and by embedding a solid support into rod shaped gels, soft actuators are fabricated that undergo forward and backward bending motion in response to changing anion concentration. The swelling and bending process, which is accompanied by intense green coloration of the gel, is achieved by using only low amounts of crosslinker. This macroscopic actuation achieved by anion binding to specific molecular entities in the polymer network will open new opportunities in the field of chemically responsive materials.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Review
Chemistry, Multidisciplinary
Sander J. Wezenberg
Summary: This feature article summarizes the development and design principles of molecular tweezers containing a molecular photoswitch as the core unit. It introduces the strategy of using a molecular photoswitch to control binding affinity and discusses the effect of substrate binding on the behavior of the molecular switch.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Thomas Freese, Balint Fridrich, Stefano Crespi, Anouk S. Lubbe, Katalin Barta, Ben L. Feringa
Summary: Lignin, as the largest natural source of functionalized aromatics, holds great potential for synthesis of aromatic products. However, the diversification of these structures and their applications have not been well-studied. In this study, a novel light-driven unidirectional molecular motor was synthesized from a specific aromatic platform chemical derived from lignocellulose. The synthetic path followed the principles of green chemistry and aimed to maintain the intrinsic functionality of the lignin-derived platform molecule.
Article
Chemistry, Multidisciplinary
Daisy R. S. Pooler, Anouk S. Lubbe, Stefano Crespi, Ben L. Feringa
Summary: This article focuses on the key aspects of motor design, discussing how to manipulate these properties without impeding motor integrity, and provides a comprehensive evaluation of all artificial light-driven rotary motor scaffolds currently present in the literature.
Article
Chemistry, Multidisciplinary
Jos C. M. Kistemaker, Anouk S. Lubbe, Ben L. Feringa
Summary: This perspective focuses on the exploration of rotary molecular motors and their applications in functional materials, as well as the major challenges in bringing dynamic properties to complex molecular systems.
MATERIALS CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
David Villaron, Maxime A. Siegler, Sander J. Wezenberg
Summary: This study presents a Calix[4]pyrrole receptor that can be reversibly switched by light between a strong chloride-binding Z-isomer and a weakly binding E-isomer. The significant difference in binding affinity between the Z- and E-isomer is quantified using H-1 NMR and ITC titrations in MeCN. Structural insights into the photogenerated E-isomer and the chloride-bound receptors are provided through DFT calculations and X-ray crystallographic analysis, offering new prospects for on-demand binding and release in extractions and membrane transport processes.
Article
Chemistry, Multidisciplinary
Thomas S. C. MacDonald, Ben L. Feringa, William S. Price, Sander J. Wezenberg, Jonathon E. Beves
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Organic
Jinyu Sheng, Stefano Crespi, Ben L. Feringa, Sander J. Wezenberg
ORGANIC CHEMISTRY FRONTIERS
(2020)
Article
Chemistry, Organic
Fuying Zhu, Yamei Lin
Summary: In this study, a low-metal iron-supported catalyst (Fe20/NC-Mg) was reported for the efficient synthesis of quinoxaline compounds, using water as a solvent and without additional bases. The synergistic effect of FeNx site and Mg (OH)2 nanorods in the catalyst played a key role in achieving high yields (82-91%) in 16 examples. The gram-level synthesis and reusability of the catalysts after four cycles demonstrated its industrial application potential.
Article
Chemistry, Organic
Mikhail Kozlov, Alexey Tyurin, Andrey Dmitrenok, Vyacheslav Rusak, Aleksander Fedorov, Igor Zavarzin, Yulia Volkova
Summary: This study presents a novel and practical synthesis method for phosphorus-substituted 1,3,4-thiadiazolines using phosphorylthioformic acid hydrazides and ketones. The protocol demonstrates operational simplicity, availability of reagents, and tolerance towards different functional groups.
Article
Chemistry, Organic
Jisna Jose, Thomas Mathew
Summary: 2-Cyclopentenone and its derivatives are highly esteemed synthetic intermediates with exceptional utility in organic synthesis. They are favored structural motifs in numerous pharmaceutical drugs and natural products, highlighting their significance. The review discusses the various methods used to synthesize cyclopentenones from 2016 to 2023.
