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Rapidly sequence-controlled electrosynthesis of organometallic polymers.

ABSTRACT: Single rich-stimuli-responsive organometallic polymers are considered to be the candidate for ultrahigh information storage and anti-counterfeiting security. However, their controllable synthesis has been an unsolved challenge. Here, we report the rapidly sequence-controlled electrosynthesis of organometallic polymers with exquisite insertion of multiple and distinct monomers. Electrosynthesis relies on the use of oxidative and reductive C-C couplings with the respective reaction time of 1?min. Single-monomer-precision propagation does not need protecting and deprotecting steps used in solid-phase synthesis, while enabling the uniform synthesis and sequence-defined possibilities monitored by both UV-vis spectra and cyclic voltammetry. Highly efficient electrosynthesis possessing potentially automated production can incorporate an amount of available metal and ligand species into a single organometallic polymer with complex architectures and functional versatility, which is proposed to have ultrahigh information storage and anti-counterfeiting security with low-cost coding and decoding processes at the single organometallic polymer level.

SUBMITTER: Zhang J

PROVIDER: S-EPMC7242481 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Rapidly sequence-controlled electrosynthesis of organometallic polymers.

Zhang Jian J Wang Jinxin J Wei Chang C Wang Yanfang Y Xie Guanyu G Li Yongfang Y Li Mao M

Nature communications 20200521 1

Single rich-stimuli-responsive organometallic polymers are considered to be the candidate for ultrahigh information storage and anti-counterfeiting security. However, their controllable synthesis has been an unsolved challenge. Here, we report the rapidly sequence-controlled electrosynthesis of organometallic polymers with exquisite insertion of multiple and distinct monomers. Electrosynthesis relies on the use of oxidative and reductive C-C couplings with the respective reaction time of 1 min. ...[more]

PMID: 32439856

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Project description:UNLABELLED:Recent studies reveal many biomaterial vaccine carriers are able to activate immunostimulatory pathways, even in the absence of other immune signals. How the changing properties of polymers during biodegradation impact this intrinsic immunogenicity is not well studied, yet this information could contribute to rational design of degradable vaccine carriers that help direct immune response. We use degradable poly(beta-amino esters) (PBAEs) to explore intrinsic immunogenicity as a function of the degree of polymer degradation and polymer form (e.g., soluble, particles). PBAE particles condensed by electrostatic interaction to mimic a common vaccine approach strongly activate dendritic cells, drive antigen presentation, and enhance T cell proliferation in the presence of antigen. Polymer molecular weight strongly influences these effects, with maximum stimulation at short degradation times--corresponding to high molecular weight--and waning levels as degradation continues. In contrast, free polymer is immunologically inert. In mice, PBAE particles increase the numbers and activation state of cells in lymph nodes. Mechanistic studies reveal that this evolving immunogenicity occurs as the physicochemical properties and concentration of particles change during polymer degradation. This work confirms the immunological profile of degradable, synthetic polymers can evolve over time and creates an opportunity to leverage this feature in new vaccines. STATEMENT OF SIGNIFICANCE:Degradable polymers are increasingly important in vaccination, but how the inherent immunogenicity of polymers changes during degradation is poorly understood. Using common rapidly-degradable vaccine carriers, we show that the activation of immune cells--even in the absence of other adjuvants--depends on polymer form (e.g., free, particulate) and the extent of degradation. These changing characteristics alter the physicochemical properties (e.g., charge, size, molecular weight) of polymer particles, driving changes in immunogenicity. Our results are important as many common biomaterials (e.g., PLGA) are now known to exhibit immune activity that alters how vaccines are processed. Thus, the results of this study could contribute to more rational design of biomaterial carriers that also actively direct the properties of responses generated by vaccines.

Dataset Information

Rapidly sequence-controlled electrosynthesis of organometallic polymers.

Publications

Rapidly sequence-controlled electrosynthesis of organometallic polymers.

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