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13. Tunneling Mechanisms of Quinones in Photosynthetic Reaction Center–Light Harvesting 1 Supercomplexes.

Author

Mao, Ruichao, Guo, Jianping, Bie, Lihua, Liu, Lu‐Ning, and Gao, Jun

Subjects
GIBBS' energy diagram, HYDROQUINONE, RHODOPSEUDOMONAS palustris, ELECTRON transport, MOLECULAR dynamics
Abstract

In photosynthesis, light energy is absorbed and transferred to the reaction center, ultimately leading to the reduction of quinone molecules through the electron transfer chain. The oxidation and reduction of quinones generate an electrochemical potential difference used for adenosine triphosphate synthesis. The trafficking of quinone/quinol molecules between electron transport components has been a long‐standing question. Here, an atomic‐level investigation into the molecular mechanism of quinol dissociation in the photosynthetic reaction center–light‐harvesting complex 1 (RC–LH1) supercomplexes from Rhodopseudomonas palustris, using classical molecular dynamics (MD) simulations combined with self‐random acceleration MD‐MD simulations and umbrella sampling methods, is conducted. Results reveal a significant increase in the mobility of quinone molecules upon reduction within RC–LH1, which is accompanied by conformational modifications in the local protein environment. Quinol molecules have a tendency to escape from RC–LH1 in a tail‐first mode, exhibiting channel selectivity, with distinct preferred dissociation pathways in the closed and open LH1 rings. Furthermore, comparative analysis of free energy profiles indicates that alternations in the protein environment accelerate the dissociation of quinol molecules through the open LH1 ring. In particular, aromatic amino acids form π‐stacking interactions with the quinol headgroup, resembling the key components in a conveyor belt system. This study provides insights into the molecular mechanisms that govern quinone/quinol exchange in bacterial photosynthesis and lays the framework for tuning electron flow and energy conversion to improve metabolic performance. [ABSTRACT FROM AUTHOR]

Published
2024
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24. Visualization of Bacterial Microcompartment Facet Assembly Using High-Speed Atomic Force Microscopy

Author

Sutter, Markus, Faulkner, Matthew, Aussignargues, Clément, Paasch, Bradley C, Barrett, Steve, Kerfeld, Cheryl A, and Liu, Lu-Ning

Subjects
Biochemistry and Cell Biology, Macromolecular and Materials Chemistry, Chemical Sciences, Biological Sciences, Bacterial Proteins, Crystallography, X-Ray, Microscopy, Atomic Force, Myxococcales, Point Mutation, Protein Conformation, Bacterial microcompartment, high-speed atomic force microscopy, protein dynamics, protein interaction, self-assembly, Nanoscience & Nanotechnology
Abstract

Bacterial microcompartments (BMCs) are proteinaceous organelles widespread among bacterial phyla. They compartmentalize enzymes within a selectively permeable shell and play important roles in CO2 fixation, pathogenesis, and microbial ecology. Here, we combine X-ray crystallography and high-speed atomic force microscopy to characterize, at molecular resolution, the structure and dynamics of BMC shell facet assembly. Our results show that preformed hexamers assemble into uniformly oriented shell layers, a single hexamer thick. We also observe the dynamic process of shell facet assembly. Shell hexamers can dissociate from and incorporate into assembled sheets, indicating a flexible intermolecular interaction. Furthermore, we demonstrate that the self-assembly and dynamics of shell proteins are governed by specific contacts at the interfaces of shell proteins. Our study provides novel insights into the formation, interactions, and dynamics of BMC shell facets, which are essential for the design and engineering of self-assembled biological nanoreactors and scaffolds based on BMC architectures.

Published
2016

35. Conjugated Polymer/Recombinant Escherichia coliBiohybrid Systems for Photobiocatalytic Hydrogen Production

Author

Yang, Ying, Zwijnenburg, Martijn A., Gardner, Adrian M., Adamczyk, Sylwia, Yang, Jing, Sun, Yaqi, Jiang, Qiuyao, Cowan, Alexander J., Sprick, Reiner Sebastian, Liu, Lu-Ning, and Cooper, Andrew I.

Abstract

Biohybrid photocatalysts are composite materials that combine the efficient light-absorbing properties of synthetic materials with the highly evolved metabolic pathways and self-repair mechanisms of biological systems. Here, we show the potential of conjugated polymers as photosensitizers in biohybrid systems by combining a series of polymer nanoparticles with engineered Escherichia colicells. Under simulated solar light irradiation, the biohybrid system consisting of fluorene/dibenzo [b,d]thiophene sulfone copolymer (LP41) and recombinant E. coli(i.e., a LP41/HydA BL21 biohybrid) shows a sacrificial hydrogen evolution rate of 3.442 mmol g–1h–1(normalized to polymer amount). It is over 30 times higher than the polymer photocatalyst alone (0.105 mmol g–1h–1), while no detectable hydrogen was generated from the E. colicells alone, demonstrating the strong synergy between the polymer nanoparticles and bacterial cells. The differences in the physical interactions between synthetic materials and microorganisms, as well as redox energy level alignment, elucidate the trends in photochemical activity. Our results suggest that organic semiconductors may offer advantages, such as solution processability, low toxicity, and more tunable surface interactions with the biological components over inorganic materials.

Published
2024
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45. Making the connections : physical and electric interactions in biohybrid photosynthetic systems

Author

Yang, Ying, Liu, Lu-Ning, Tian, Haining, Cooper, Andrew I., Sprick, Reiner Sebastian, Yang, Ying, Liu, Lu-Ning, Tian, Haining, Cooper, Andrew I., and Sprick, Reiner Sebastian

Abstract

Biohybrid photosynthesis systems, which combine biological and non-biological materials, have attracted recent interest in solar-to-chemical energy conversion. However, the solar efficiencies of such systems remain low, despite advances in both artificial photosynthesis and synthetic biology. Here we discuss the potential of conjugated organic materials as photosensitisers for biological hybrid systems compared to traditional inorganic semiconductors. Organic materials offer the ability to tune both photophysical properties and the specific physicochemical interactions between the photosensitiser and biological cells, thus improving stability and charge transfer. We highlight the state-of-the-art and opportunities for new approaches in designing new biohybrid systems. This perspective also summarises the current understanding of the underlying electron transport process and highlights the research areas that need to be pursued to underpin the development of hybrid photosynthesis systems. Biohybrid systems of synthetic materials and microorganisms can be obtained using a range of assembly strategies based on their interactions. This influences charge transfer between the components and their efficiency for solar fuels generation.

Published
2023
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48. In situ visualization of Braun’s lipoprotein on E. coli sacculi

Author

Sheng, Qi, primary, Zhang, Meng-Yao, additional, Liu, Si-Min, additional, Chen, Zhuo-Wei, additional, Yang, Pei-Ling, additional, Zhang, Hong-Su, additional, Liu, Meng-Yun, additional, Li, Kang, additional, Zhao, Long-Sheng, additional, Liu, Ning-Hua, additional, Liu, Lu-Ning, additional, Chen, Xiu-Lan, additional, Hobbs, Jamie K., additional, Foster, Simon J., additional, Zhang, Yu-Zhong, additional, and Su, Hai-Nan, additional

Published
2023
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