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An electric molecular motor.

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 (CBPQT⁴⁺) 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_OF₁ ATP synthase⁹. The unidirectionality is powered by an oscillating¹⁰ voltage^11,12 or external modulation of the redox potential¹³. 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 CBPQT⁴⁺ 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-bound¹⁴ electric molecular motors.

SUBMITTER: Zhang L

PROVIDER: S-EPMC9834048 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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An electric molecular motor.

Zhang Long L Qiu Yunyan Y Liu Wei-Guang WG Chen Hongliang H Shen Dengke D Song Bo B Cai Kang K Wu Huang H Jiao Yang Y Feng Yuanning Y Seale James S W JSW Pezzato Cristian C Tian Jia J Tan Yu Y Chen Xiao-Yang XY Guo Qing-Hui QH Stern Charlotte L CL Philp Douglas D Astumian R Dean RD Goddard William A WA Stoddart J Fraser JF

Nature 20230111 7943

Macroscopic electric motors continue to have a large impact on almost every aspect of modern society. Consequently, the effort towards developing molecular motors1-3 that can be driven by electricity could not be more timely. Here we describe an electric molecular motor based on a [3]catenane4,5, in which two cyclobis(paraquat-p-phenylene)6 (CBPQT4+) rings are powered by electricity in solution to circumrotate unidirectionally around a 50-membered loop ...[more]

PMID: 36631649

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Project description:The membrane-bound component F(0), which is a major component of the F(0)F(1)-ATP synthase, works as a rotary motor and plays a central role in driving the F(1) component to transform chemiosmotic energy into ATP synthesis. We conducted molecular dynamics simulations of b(2)-free F(0) in a 1-palmitoyl-2-oleoyl-phosphatidylcholine lipid bilayer for tens of nanoseconds with two different protonation states of the cAsp-61 residue at the interface of the a-c complex in the absence of electric fields and under electric fields of +/-0.03 V/nm across the membrane. To our surprise, we observed that the upper half of the N-terminal helix of the c(1) subunit rotated about its axis clockwise by 30 degrees . An energetic analysis revealed that the electrostatic repulsion between this N-terminal helix and subunit c(12) was a major contributor to the observed rotation. A correlation map analysis indicated that the correlated motions of residues in the interface of the a-c complex were significantly reduced by external electric fields. The deuterium order parameter (S(CD)) profile calculated by averaging all the lipids in the F(0)-bound bilayer was not very different from that of the pure bilayer system, in agreement with recent (2)H solid-state NMR experiments. However, by delineating the lipid properties according to their vicinity to F(0), we found that the S(CD) profiles of different lipid shells were prominently different. Lipids close to F(0) formed a more ordered structure. Similarly, the lateral diffusion of lipids on the membrane surface also followed a shell-dependent behavior. The lipids in the proximity of F(0) exhibited very significantly reduced diffusional motion. The numerical value of S(CD) was anticorrelated with that of the diffusion coefficient, i.e., the more ordered lipid structures led to slower lipid diffusion. Our findings will help elucidate the dynamics of F(0) depending on the protonation state and electric field, and may also shed some light on the interactions between the motor F(0) and its surrounding lipids under physiological conditions, which could help to rationalize its extraordinary energy conversion efficiency.

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An electric molecular motor.

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An electric molecular motor.

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