Coupling Self-Assembly Mechanisms to Fabricate Molecularly and Electrically Responsive Films

Li, Jinyang; Maniar, Drishti; Qu, Xue; Liu, Huan; Tsao, Chen‐Yu; Kim, Eunkyoung; Bentley, William E.; Liu, Changsheng

doi:10.1021/acs.biomac.8b01592

Cited by 16 publications

(15 citation statements)

References 104 publications

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“…As was observed with Urs hydrogel , glucose conversion to gluconic acid could be observed in the electrodeposited Cat‐GOx hydrogel (Figure 3 a, bottom) as has been reported, [34] with the kinetics essentially identical to the GOx CS,aq + Cat CS,aq case. A key difference compared to the Urs hydrogel was that a two layer Cat‐GOx hydrogel was generated for this experiment.…”

Section: Resultssupporting

confidence: 82%

Real‐Time NMR Monitoring of Spatially Segregated Enzymatic Reactions in Multilayered Hydrogel Assemblies**

et al. 2021

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Compartmentalized chemical reactions at the microscale are important in biotechnology, yet monitoring the molecular content at these small scales is challenging. To address this challenge, we integrate a compact, reconfigurable reaction cell featuring electrochemical functionality with high‐resolution NMR spectroscopy. We demonstrate the operation of this system by monitoring the activity of enzymes immobilized in chemically distinct layers within a multi‐layered chitosan hydrogel assembly. As a benchmark, we observed the parallel activities of urease (Urs), catalase (Cat), and glucose oxidase (GOx) by monitoring reagent and product concentrations in real‐time. Simultaneous monitoring of an independent enzymatic process (Urs) together with a cooperative process (GOx + Cat) was achieved, with chemical conversion modulation of the GOx + Cat process demonstrated by varying the order in which the hydrogel was assembled.

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Section: Resultssupporting

confidence: 82%

Real‐Time NMR Monitoring of Spatially Segregated Enzymatic Reactions in Multilayered Hydrogel Assemblies**

et al. 2021

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“…For example, films have been deposited in a layer‐by‐layer approach with targeting motifs on the penultimate layer that disassembled at endosomal pH, thus allowing for the release of entrapped cargo such as doxorubicin . Similar approaches were used to construct chitosan, Con‐A, and glycogen layer‐by‐layer films ( Figure A–C) that can respond (Figure D) and disassemble to enzymatic and electrical cues . Zhang et al developed systems of mesoporous silica nanoparticles that were sequentially coated by Con‐A and glycogen, and with galactomannan as the final coating (Figure E), which allowed for enhanced interaction with liver cells.…”

Section: Glycogen As a Building Block Of Nanostructured Materialsmentioning

confidence: 99%

“…D) Nyquist plot indicates increasing impedance with the assembly of each added glycogen‐Con A layer and the final GO x layer. A–D) Reproduced with permission . Copyright 2019, American Chemical Society.…”

Section: Glycogen As a Building Block Of Nanostructured Materialsmentioning

confidence: 99%

Glycogen as a Building Block for Advanced Biological Materials

2019

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complex drug delivery systems that are challenging to scale up and therefore have limited clinical and commercial translation. Although numerous nanoparticles have been widely developed and used for various applications, including biomedical applications, [2] there is a growing interest in nontoxic and degradable alternatives to first-generation synthetic nanomaterials. Ideally the synthesis of such nanoparticles needs to be cost effective, simple, green, reproducible, scalable, and the constitutive building blocks of the nanoparticles should be nontoxic, functional, biodegradable, and available on a large scale. Naturally occurring nanoparticles could be such a valid alternative. These nanoparticles include intracellular structures, such as magnetosomes [3] and glycogen, and extracellular assemblies such as lipoproteins and viruses. [3] Among these, glycogen is the most abundant and versatile biological nanoparticle, which fulfils the requirements for the fabrication of nanostructured biomaterials. Glycogen is nature's prime nanoparticle that exists in most organisms, from bacteria and archaea to humans, [4,5] as a vital component of the cellular energy machinery. It is a highly branched polysaccharide comprising repeating units of glucose connected by linear α-d-(1,4) glycosidic linkages with α-d-(1,6) branching, structured into roughly spherical nanoparticles that have a high water solubility and molecular weight.The use of polysaccharides as components for advanced materials has been an attractive concept for decades. [6,7] A key motive is that polysaccharides, as a natural biomaterial, are endowed with a level of biodegradability and biocompatibility. In addition, they can be easily modified chemically or biochemically to produce functional derivatives, which are important for various therapeutic applications. [8] The structures of polysaccharides vary considerably but span from linear to highly branched polymers with molecular weights ranging from thousands to millions, composed of mono-or disaccharides, or short-chain oligomers bound together by glycosidic linkages. [9] There is a rich history of research on the use of polysaccharides in a range of therapeutic applications including: i) soft tissue engineering, [10,11] where the materials can be designed to mimic the mechanical properties of the extracellular matrix in the tissue; ii) as drug, protein, or gene delivery systems, [7,12,13] where polysaccharides have a large number of reactive groups [14] that allow for tunable properties [12] such as pH-responsiveness; [15] and iii) as nanoprobes for cellular Biological nanoparticles found in living systems possess distinct molecular architectures and diverse functions. Glycogen is a unique biological polysaccharide nanoparticle fabricated by nature through a bottom-up approach. The biocatalytic synthesis of glycogen has evolved over time to form a nanometer-sized dendrimer-like structure (20-150 nm) with a highly branched surface and a dense core. This makes glycogen markedly different from other natur...

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“…Payne and co-workers have shown how pH switch gels formed by the reduction of water can be removed from the surface of the electrode by reversing the potential where the oxidation of water occurs causing acidification. This induced acidification of chitosan gels can induce multilayer disassembly [67]. Potential reversal has also been used to remove gels from a patterned microelectrode surface as shown in Fig.…”

Section: Removing the Gel From The Electrode Surfacementioning

confidence: 99%