Transforming<i>Escherichia coli</i>Proteomembranes into Artificial Chloroplasts Using Molecular Photocatalysis

Mengele, Alexander K.; Weixler, Dominik; Amthor, Sebastian; Eikmanns, Bernhard J.; Seibold, Gerd M.; Rau, Sven

doi:10.1002/anie.202114842

Cited by 17 publications

(17 citation statements)

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“…While both BNA + and 1,4-BNAH show an absorption band below 300 nm (though with maxima at different wavelengths, inset of Figure 2), the reduced form (1,4-BNAH) displays a characteristic absorption ranging from 320 to 420 nm. 26,[30][31][32]68 S1), a BNAH yield of 48% after an irradiation time of 150 min is estimated (red trace in Figure 2B). Aside from the 1,4-BNAH reduction product, the singleelectron transfer reaction promoted by the photosensitizer can in principle lead to regioisomers or the well-known BNA dimer, 69 which absorbs around 356 nm.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

et al. 2023

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Nicotinamide adenine nucleotide (NADH) is involved in many biologically relevant redox reactions, and the photochemical regeneration of its oxidized form (NAD+) under physiological conditions is of interest for combined photo- and biocatalysis. Here, we demonstrate that tri-anionic, water-soluble variants of typically very lipophilic iridium(III) complexes can photo-catalyze the reduction of an NAD+ mimic in a comparatively efficient manner. In combination with a well-known rhodium co-catalyst to facilitate regioselective reactions, these iridium(III) photo-reductants outcompete the commonly used [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) photosensitizer in water by up to 1 order of magnitude in turnover frequency. This improved reactivity is attributable to the strong excited-state electron donor properties and the good chemical robustness of the tri-anionic iridium(III) sensitizers, combined with their favorable Coulombic interaction with the di-cationic rhodium co-catalyst. Our findings seem relevant in the greater context of photobiocatalysis, for which access to strong, efficient, and robust photoreductants with good water solubility can be essential.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

et al. 2023

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“…The ruthenium complex can reduce the NAD + cofactor to NADH to be used by the NADH dehydrogenase present in the E. coli vesicle, thereby generating a proton motive force, followed by ATP generation (Figure 6d). [ 152 ]…”

Section: Types Of Cell Membrane Vesicles As Nano‐ and Microreactorsmentioning

confidence: 99%

Bridging the Gap between Nonliving Matter and Cellular Life

Kumar

Karmacharya

Cho

2022

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with simple primitive life. However, whether life emerges from scratch from nonliving matter remains a mystery. Accordingly, understanding the fundamental principles of life processes is still a major scientific challenge. [1] Engineers can create a biological environment absent in nature by employing synthetic biology tools, thus allowing the discovery and elucidation of fundamentally complex biological cells in ways that remain currently impossible. [2] As a result, its essential goal is to regulate the required components to enhance their complexity as the need for comprehension grows. [3] To address fundamental questions regarding the transition from chemistry to biology, the chemical techniques applied to non-living matter to produce life are divided into top-down or bottom-up synthesis. [2] The majority of the top-down approaches have focused on genetic engineering and molecular biology techniques applied to prokaryotes such as Escherichia coli (E. coli), Klebsiella pneumonia (K. pneumonia), and others to isolate and generate enzymes, drug precursors, and biofuels for their application in health, bioremediation, environmental, and other therapeutic strategies. [4,5] A bottom-up approach is typically used to create new life-like features, known as artificial cells, from cellular components or non-living matter, to better understand specific cellular characteristics and the origin of life.The generation of an artificial cell factory provides a foundation for critical cell biology research. However, the concept of an artificial cell can be controversial, as factors such as cell size, genetic composition, and morphological similarity need to be considered. [6] Vesicles such as giant unilamellar vesicles (GUVs), polysaccharidosomes, membrane-less coacervate microdroplets, and hydrogel particles are being explored to mimic the cell organelles and provide a functional unit to address their issues. [7][8][9][10] Though synthetic micro or nanoreactors have been used to mimic life-like functions and to learn about the fundamental biology of natural cells, constructing a life-like structure out of non-living building blocks remains a considerable challenge. In this review, we focus on hybrid approaches that use both natural and synthetic materials to mimic and interface with biological systems (Figure 1). Using hybrid vesicle micro or nanoreactors, bioinspired life-like functions such as chemical compartments, cascade signaling, energy generation, growth, replication, and environmental A cell, the fundamental unit of life, contains the requisite blueprint information necessary to survive and to build tissues, organs, and systems, eventually forming a fully functional living creature. A slight structural alteration can result in data misprinting, throwing the entire life process off balance. Advances in synthetic biology and cell engineering enable the predictable redesign of biological systems to perform novel functions. Individual functions and fundamental processes at the core of the biology of cells can be investig...

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“…Photocatalytic water splitting was shown to be influenced by these aromatic interplays as well (38)(39)(40)(41)(42)(43)(44)(45). Over the last two decades, our group has developed a library of photocatalysts for visible-light-driven hydrogen evolution based on the polyheteroaromatic tetrapyridophenazine bridging ligand and derivatives thereof which have recently also been integrated into a functional biochemical apparatus for light-driven ATP synthesis (46)(47)(48)(49). Regarding the effect of π-π stacking on catalytic turnover, it was demonstrated that manipulation of the bridging ligand by polyaromatic additives such as pyrene and anthracene has a beneficial effect on the H 2 evolution of a respective molecular Ru-Pd photocatalyst (50).…”

Section: Introductionmentioning

confidence: 99%

Evaluation of 1H‐NMR Spectroscopy‐Based Quantification Methods of the Supramolecular Aggregation of a Molecular Photosensitizer^†

Pehlken

Pfeffer

Reich

et al. 2022

Photochem & Photobiology

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The supramolecular dimerization of a ruthenium polypyridyl precursor of a well‐developed family of hydrogen‐evolving photocatalysts via π–π interactions of the polyheteroaromatic bridging ligand was quantified with concentration‐dependent 1H‐NMR spectroscopy. The data sets were analyzed with different calculation and fit methods. A comparison between the results of direct calculation and linear and nonlinear approaches showed that the application of a global nonlinear fit procedure yields the best results. The presented methods are also applicable for dimerization processes in the solution of other molecular moieties.

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TransformingEscherichia coliProteomembranes into Artificial Chloroplasts Using Molecular Photocatalysis

Cited by 17 publications

References 83 publications

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

Bridging the Gap between Nonliving Matter and Cellular Life

Evaluation of 1H‐NMR Spectroscopy‐Based Quantification Methods of the Supramolecular Aggregation of a Molecular Photosensitizer^†

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TransformingEscherichia coliProteomembranes into Artificial Chloroplasts Using Molecular Photocatalysis

Cited by 17 publications

References 83 publications

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

Photocatalytic Regeneration of a Nicotinamide Adenine Nucleotide Mimic with Water-Soluble Iridium(III) Complexes

Bridging the Gap between Nonliving Matter and Cellular Life

Evaluation of 1H‐NMR Spectroscopy‐Based Quantification Methods of the Supramolecular Aggregation of a Molecular Photosensitizer†

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Evaluation of 1H‐NMR Spectroscopy‐Based Quantification Methods of the Supramolecular Aggregation of a Molecular Photosensitizer^†