ORCID Profile
0000-0001-7472-187X
Current Organisation
The University of Maine
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Macromolecular and Materials Chemistry | Nanochemistry and Supramolecular Chemistry | Physical Organic Chemistry
Publisher: American Chemical Society (ACS)
Date: 17-10-2019
DOI: 10.1021/JACS.9B08927
Abstract: Artificial molecular machines (AMMs) built from mechanically interlocked molecules (MIMs) can use energy ratchets to control the unidirectional motion of their component parts. These energy ratchets are operated by the alteration of kinetic barriers and thermodynamic wells, which are, in turn, determined by the switching on and off of noncovalent interactions. Previously, we have developed artificial molecular pumps (AMPs) capable of pumping rings consecutively onto a collecting chain as part of a molecular dumbbell, leading to the formation of rotaxanes. Here, we report a molecular dual pump (MDP) consisting of two in idual AMPs linked in a head-to-tail fashion, wherein a single ring is pumped, in a linear manner, on and off a dumbbell involving a [2]rotaxane intermediate by exploiting the redox properties of the two pumps. This MDP, defined by the finely tuned noncovalent interactions and fueled by either chemicals or electricity, utilizes an energy ratchet mechanism to capture a ring and subsequently release it back into solution. The unidirectional motion and the resulting
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CS00194B
Abstract: The year 2022 marks the 30th anniversary of the first reports of polyrotaxanes in the scientific literature.
Publisher: Springer Science and Business Media LLC
Date: 11-01-2023
DOI: 10.1038/S41586-022-05421-6
Abstract: Macroscopic electric motors continue to have a large impact on almost every aspect of modern society. Consequently, the effort towards developing molecular motors 1–3 that can be driven by electricity could not be more timely. Here we describe an electric molecular motor based on a [3]catenane 4,5 , in which two cyclobis(paraquat- p -phenylene) 6 (CBPQT 4+ ) rings are powered by electricity in solution to circumrotate unidirectionally around a 50-membered loop. The constitution of the loop ensures that both rings undergo highly (85%) unidirectional movement under the guidance of a flashing energy ratchet 7,8 , whereas the interactions between the two rings give rise to a two-dimensional potential energy surface (PES) similar to that shown by F O F 1 ATP synthase 9 . The unidirectionality is powered by an oscillating 10 voltage 11,12 or external modulation of the redox potential 13 . Initially, we focused our attention on the homologous [2]catenane, only to find that the kinetic asymmetry was insufficient to support unidirectional movement of the sole ring. Accordingly, we incorporated a second CBPQT 4+ ring to provide further symmetry breaking by interactions between the two mobile rings. This demonstration of electrically driven continual circumrotatory motion of two rings around a loop in a [3]catenane is free from the production of waste products and represents an important step towards surface-bound 14 electric molecular motors.
Publisher: American Chemical Society (ACS)
Date: 14-06-2019
DOI: 10.26434/CHEMRXIV.8259317.V2
Abstract: Intriguing reports of enhanced diffusion in enzymes and molecular catalysts have spurred significant interest in experimental and theoretical investigations of this phenomenon, with mechanistic understanding the subject of ongoing and lively debate. Here we use time-resolved diffusion NMR methods to measure the diffusion coefficients of small molecule species involved in chemical reactions with high temporal resolution. We show the enhanced diffusion of small molecules cannot be explained by reaction velocity, and that apparent measurements of enhanced diffusion by small molecules appear to be caused by bulk fluid flow processes such as convection.
Publisher: American Chemical Society (ACS)
Date: 08-04-2021
DOI: 10.1021/JACS.0C13388
Publisher: Springer Science and Business Media LLC
Date: 18-06-2021
Publisher: Wiley
Date: 12-11-2019
Abstract: Intriguing reports of enhanced diffusion in enzymes and molecular catalysts have spurred significant interest in experimental and theoretical investigations, and the mechanism of this phenomenon is the topic of lively debate. Here we use time‐resolved diffusion NMR methods to measure the diffusion coefficients ( D ) of small molecule species involved in chemical reactions with high temporal resolution. We show the enhanced diffusion of small molecules cannot be explained by reaction velocity, and that apparent measurements of enhanced diffusion by small molecules appear to be caused by bulk fluid flow processes such as convection.
Publisher: Springer Science and Business Media LLC
Date: 09-03-2022
DOI: 10.1038/S41586-021-04377-3
Abstract: Molecular recognition
Publisher: American Chemical Society (ACS)
Date: 31-07-2020
DOI: 10.1021/JACS.0C06663
Publisher: Wiley
Date: 12-11-2019
Abstract: Intriguing reports of enhanced diffusion in enzymes and molecular catalysts have spurred significant interest in experimental and theoretical investigations, and the mechanism of this phenomenon is the topic of lively debate. Here we use time‐resolved diffusion NMR methods to measure the diffusion coefficients ( D ) of small molecule species involved in chemical reactions with high temporal resolution. We show the enhanced diffusion of small molecules cannot be explained by reaction velocity, and that apparent measurements of enhanced diffusion by small molecules appear to be caused by bulk fluid flow processes such as convection.
Publisher: American Chemical Society (ACS)
Date: 14-06-2019
DOI: 10.26434/CHEMRXIV.8259317
Abstract: Intriguing reports of enhanced diffusion in enzymes and molecular catalysts have spurred significant interest in experimental and theoretical investigations of this phenomenon, with mechanistic understanding the subject of ongoing and lively debate. Here we use time-resolved diffusion NMR methods to measure the diffusion coefficients of small molecule species involved in chemical reactions with high temporal resolution. We show the enhanced diffusion of small molecules cannot be explained by reaction velocity, and that apparent measurements of enhanced diffusion by small molecules appear to be caused by bulk fluid flow processes such as convection. br
Publisher: American Association for the Advancement of Science (AAAS)
Date: 03-12-2021
Abstract: Numerous chemical processes, ranging from water purification to catalysis, involve sorption of small molecules onto surfaces. Typically, spontaneous attractive interactions favor the binding event. Feng et al . report a mechanisorption process that requires redox manipulations to pump macrocycles from bulk solution onto axles immobilized on a metal-organic framework. The resulting rotaxanes store energy through nonequilibrium charge concentration in their mechanical bonds. Ultimately, the technique could also prove useful for actively partitioning compounds with particular functionality between surface and bulk environments. —JSY
Publisher: Springer Science and Business Media LLC
Date: 09-06-2021
Publisher: American Association for the Advancement of Science (AAAS)
Date: 12-06-2020
Abstract: Rotaxanes consist of molecular rings threaded on a central axle. Most approaches to their synthesis have focused on introducing a single ring per axle. Qiu et al. now report a systematic approach to threading up to 10 adjacent rings consecutively. The axle's end groups were constructed to attract free-floating rings when reduced and then to push those rings toward the center upon oxidation. Products of each successive reduction-oxidation cycle were characterized by nuclear magnetic resonance spectroscopy and mass spectrometry. Science , this issue p. 1247
Publisher: American Chemical Society (ACS)
Date: 13-06-2019
DOI: 10.26434/CHEMRXIV.8259317.V1
Abstract: Intriguing reports of enhanced diffusion in enzymes and molecular catalysts have spurred significant interest in experimental and theoretical investigations of this phenomenon, with mechanistic understanding the subject of ongoing and lively debate. Here we use time-resolved diffusion NMR methods to measure the diffusion coefficients of small molecule species involved in chemical reactions with high temporal resolution. We show the enhanced diffusion of small molecules cannot be explained by reaction velocity, and that apparent measurements of enhanced diffusion by small molecules appear to be caused by bulk fluid flow processes such as convection.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0QM00022A
Abstract: Hypothetical transmembrane rotaxane as a model for trajectory thermodynamic theory of synthetic molecular pumps.
Publisher: Springer Science and Business Media LLC
Date: 06-09-2022
Location: United States of America
Start Date: 2019
End Date: 06-2022
Amount: $340,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 08-2022
End Date: 07-2025
Amount: $465,000.00
Funder: Australian Research Council
View Funded Activity