scholarly journals Enzyme-free synthesis of natural phospholipids in water

2019 ◽  
Author(s):  
Luping Liu ◽  
Yike Zou ◽  
Ahanjit Bhattacharya ◽  
Dongyang Zhang ◽  
Susan Q. Lang ◽  
...  

AbstractAll living organisms synthesize phospholipids as the primary constituent of their cell membranes. While phospholipids can spontaneously self-assemble in water to form membrane-bound vesicles, their aqueous synthesis requires pre-existing membrane-embedded enzymes. This limitation has led to models in which the first cells used simpler types of membrane building blocks and has hampered integration of phospholipid synthesis into artificial cells. Here we demonstrate that a combination of ion pairing and self-assembly of reactants allows high-yielding synthesis of cellular phospholipids in water. Acylation of 2-lysophospholipids using cationic thioesters occurs in mildly alkaline solutions resulting in the formation of cell-like membranes. A variety of membrane-forming natural phospholipids can be synthesized. Membrane formation takes place in water from natural alkaline sources, such as soda lakes and hydrothermal oceanic vents. When formed vesicles are transferred to more acidic solutions, electrochemical proton gradients are spontaneously established and maintained.


2015 ◽  
Vol 112 (27) ◽  
pp. 8187-8192 ◽  
Author(s):  
Michael D. Hardy ◽  
Jun Yang ◽  
Jangir Selimkhanov ◽  
Christian M. Cole ◽  
Lev S. Tsimring ◽  
...  

Cell membranes are dynamic structures found in all living organisms. There have been numerous constructs that model phospholipid membranes. However, unlike natural membranes, these biomimetic systems cannot sustain growth owing to an inability to replenish phospholipid-synthesizing catalysts. Here we report on the design and synthesis of artificial membranes embedded with synthetic, self-reproducing catalysts capable of perpetuating phospholipid bilayer formation. Replacing the complex biochemical pathways used in nature with an autocatalyst that also drives lipid synthesis leads to the continual formation of triazole phospholipids and membrane-bound oligotriazole catalysts from simpler starting materials. In addition to continual phospholipid synthesis and vesicle growth, the synthetic membranes are capable of remodeling their physical composition in response to changes in the environment by preferentially incorporating specific precursors. These results demonstrate that complex membranes capable of indefinite self-synthesis can emerge when supplied with simpler chemical building blocks.



2016 ◽  
Vol 44 (3) ◽  
pp. 723-730 ◽  
Author(s):  
Yuval Elani

The quest to construct artificial cells from the bottom-up using simple building blocks has received much attention over recent decades and is one of the grand challenges in synthetic biology. Cell mimics that are encapsulated by lipid membranes are a particularly powerful class of artificial cells due to their biocompatibility and the ability to reconstitute biological machinery within them. One of the key obstacles in the field centres on the following: how can membrane-based artificial cells be generated in a controlled way and in high-throughput? In particular, how can they be constructed to have precisely defined parameters including size, biomolecular composition and spatial organization? Microfluidic generation strategies have proved instrumental in addressing these questions. This article will outline some of the major principles underpinning membrane-based artificial cells and their construction using microfluidics, and will detail some recent landmarks that have been achieved.



Author(s):  
Ahyoung Kim ◽  
Lehan Yao ◽  
Falon Kalutantirige ◽  
Shan Zhou ◽  
Qian Chen

Biological building blocks (i.e., proteins) are encoded with the information of target structure into the chemical and morphological patches, guiding their assembly into the levels of functional structures that are crucial for living organisms. Learning from nature, researchers have been attracted to the artificial analogues, “patchy particles,” which have controlled geometries of patches that serve as directional bonding sites. However, unlike the abundant studies of micron-scale patchy particles, which demonstrated complex assembly structures and unique behaviors attributed to the patches, research on patchy nanoparticles (NPs) has remained challenging. In the present chapter, we discuss the recent understandings on patchy NP design and synthesis strategies, and physical principles of their assembly behaviors, which are the main factors to program patchy NP self-assembly into target structures that cannot be achieved by conventional non-patched NPs. We further summarize the self-assembly of patchy NPs under external fields, in simulation, and in kinetically controlled assembly pathways, to show the structural richness patchy NPs bring. The patchy NP assembly is novel by their structures as well as the multicomponent features, and thus exhibits unique optical, chemical, and mechanical properties, potentially aiding applications in catalysts, photonic crystals, and metamaterials as well as fundamental nanoscience.



Crystals ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 467 ◽  
Author(s):  
Melese Getenet ◽  
Juan Manuel García-Ruiz ◽  
Cristóbal Verdugo-Escamilla ◽  
Isabel Guerra-Tschuschke

Mineral vesicles and chemical gardens are self-organized biomimetic structures that form via abiotic mineral precipitation. These membranous structures are known to catalyze prebiotic reactions but the extreme conditions required for their synthesis has cast doubts on their formation in nature. Apart from model solutions, these structures have been shown to form in serpentinization-driven natural silica-rich water and by fluid-rock interaction of model alkaline solutions with granites. Here, for the first time, we demonstrate that self-assembled hollow mineral vesicles and gardens can be synthesized in natural carbonate-rich soda lake water. We have synthesized these structures by a) pouring saturated metal salt solutions, and b) by immersing metal salt pellets in brines collected from Lake Magadi (Kenya). The resulting structures are analyzed by using SEM coupled with EDX analysis, Raman spectroscopy, and powder X-ray diffraction. Our results suggest that mineral self-assembly could have been a common phenomenon in soda oceans of early Earth and Earth-like planets and moons. The composition of the obtained vesicles and gardens confirms the recent observation that carbonate minerals in soda lakes sequestrate Ca, thus leaving phosphate behind in solution available for biochemical reactions. Our results strengthens the proposal that alkaline brines could be ideal sites for “one-pot” synthesis of prebiotic organic compounds and the origin of life.



2012 ◽  
Vol 9 (1) ◽  
pp. 43 ◽  
Author(s):  
Hueyling Tan

Molecular self-assembly is ubiquitous in nature and has emerged as a new approach to produce new materials in chemistry, engineering, nanotechnology, polymer science and materials. Molecular self-assembly has been attracting increasing interest from the scientific community in recent years due to its importance in understanding biology and a variety of diseases at the molecular level. In the last few years, considerable advances have been made in the use ofpeptides as building blocks to produce biological materials for wide range of applications, including fabricating novel supra-molecular structures and scaffolding for tissue repair. The study ofbiological self-assembly systems represents a significant advancement in molecular engineering and is a rapidly growing scientific and engineering field that crosses the boundaries ofexisting disciplines. Many self-assembling systems are rangefrom bi- andtri-block copolymers to DNA structures as well as simple and complex proteins andpeptides. The ultimate goal is to harness molecular self-assembly such that design andcontrol ofbottom-up processes is achieved thereby enabling exploitation of structures developed at the meso- and macro-scopic scale for the purposes oflife and non-life science applications. Such aspirations can be achievedthrough understanding thefundamental principles behind the selforganisation and self-synthesis processes exhibited by biological systems.



2018 ◽  
Author(s):  
Erik Leonhardt ◽  
Jeff M. Van Raden ◽  
David Miller ◽  
Lev N. Zakharov ◽  
Benjamin Aleman ◽  
...  

Extended carbon nanostructures, such as carbon nanotubes (CNTs), exhibit remarkable properties but are difficult to synthesize uniformly. Herein, we present a new class of carbon nanomaterials constructed via the bottom-up self-assembly of cylindrical, atomically-precise small molecules. Guided by supramolecular design principles and circle packing theory, we have designed and synthesized a fluorinated nanohoop that, in the solid-state, self-assembles into nanotube-like arrays with channel diameters of precisely 1.63 nm. A mild solution-casting technique is then used to construct vertical “forests” of these arrays on a highly-ordered pyrolytic graphite (HOPG) surface through epitaxial growth. Furthermore, we show that a basic property of nanohoops, fluorescence, is readily transferred to the bulk phase, implying that the properties of these materials can be directly altered via precise functionalization of their nanohoop building blocks. The strategy presented is expected to have broader applications in the development of new graphitic nanomaterials with π-rich cavities reminiscent of CNTs.



2017 ◽  
Author(s):  
Niamh Mac Fhionnlaoich ◽  
Stephen Schrettl ◽  
Nicholas B. Tito ◽  
Ye Yang ◽  
Malavika Nair ◽  
...  

The arrangement of nanoscale building blocks into patterns with microscale periodicity is challenging to achieve via self-assembly processes. Here, we report on the phase transition-driven collective assembly of gold nanoparticles in a thermotropic liquid crystal. A temperature-induced transition from the isotropic to the nematic phase leads to the assembly of individual nanometre-sized particles into arrays of micrometre-sized aggregates, whose size and characteristic spacing can be tuned by varying the cooling rate. This fully reversible process offers hierarchical control over structural order on the molecular, nanoscopic, and microscopic level and is an interesting model system for the programmable patterning of nanocomposites with access to micrometre-sized periodicities.



2021 ◽  
Author(s):  
Alexander Banger ◽  
Julian Sindram ◽  
Marius Otten ◽  
Jessica Kania ◽  
Alexander Strzelczyk ◽  
...  

We present the synthesis of so called amphiphilic glycomacromolecules (APGs) by using solid-phase polymer synthesis. Based on tailor made building blocks, monosdisperse APGs with varying compositions are synthesized, introducing carbohydrate...



2006 ◽  
pp. 4847-4849 ◽  
Author(s):  
Bulusu Jagannadh ◽  
Marepally Srinivasa Reddy ◽  
Chennamaneni Lohitha Rao ◽  
Anabathula Prabhakar ◽  
Bharatam Jagadeesh ◽  
...  


2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Daniel Valente

AbstractImitating the transition from inanimate to living matter is a longstanding challenge. Artificial life has achieved computer programs that self-replicate, mutate, compete and evolve, but lacks self-organized hardwares akin to the self-assembly of the first living cells. Nonequilibrium thermodynamics has achieved lifelike self-organization in diverse physical systems, but has not yet met the open-ended evolution of living organisms. Here, I look for the emergence of an artificial-life code in a nonequilibrium physical system undergoing self-organization. I devise a toy model where the onset of self-replication of a quantum artificial organism (a chain of lambda systems) is owing to single-photon pulses added to a zero-temperature environment. I find that spontaneous mutations during self-replication are unavoidable in this model, due to rare but finite absorption of off-resonant photons. I also show that the replication probability is proportional to the absorbed work from the photon, thereby fulfilling a dissipative adaptation (a thermodynamic mechanism underlying lifelike self-organization). These results hint at self-replication as the scenario where dissipative adaptation (pointing towards convergence) coexists with open-ended evolution (pointing towards divergence).



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