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  1. Non-aqueous organic redox flow batteries (NAORFBs) are considered emerging large-scale energy storage systems due to their larger voltage window as compared to aqueous systems and their metal-free nature. However, low solubility, sustainability, and crossover of redox materials remain major challenges for the development of NAORFBs. Here, we report the use of redox active α-helical polypeptides suitable for NAORFBs. The polypeptides exhibit less crossover than small molecule analogs for both Daramic 175 separator and FAPQ 375 PP membrane, with FAPQ 375 PP preventing crossover most effectivley. Polypeptide NAORFBs assembled with a TEMPO-based polypeptide catholyte and viologen-based polypeptide anolyte exhibit low capacity fade ( ca. 0.1% per cycle over 500 cycles) and high coulombic efficiency (>99.5%). The polypeptide NAORFBs exhibit an output voltage of 1.1 V with a maximum capacity of 0.53 A h L −1 (39% of the theoretical capacity). After 500 charge–discharge cycles, 60% of the initial capacity was retained. Post cycling analysis using spectral and electrochemical methods demonstrate that the polypeptide backbone and the ester side chain linkages are stable during electrochemical cycling. Taken together, these polypeptides offer naturally-derived, deconstructable platforms for addressing the needs of metal-free energy storage.
    Free, publicly-accessible full text available August 15, 2023
  2. Free, publicly-accessible full text available May 11, 2023
  3. The development of next-generation smart nanocarriers that can be tailored for specific applications requires precise control over physiochemical properties, yet modulation of nanostructures solely through synthetic routes is a time-consuming and labor-intensive process. In this work, co-assembly of two degradable glucose-based amphiphilic block polymers is demonstrated as a means to control nanoparticle size, surface charge, and stimuli-responsive properties, allowing optimization of these constructs for cytosolic drug delivery applications. Polymeric particles with varying weight fractions of carboxylate- and histamine-modified poly( dl- lactide)- b -poly( d -glucose carbonate)s (PDLLA- b -PDGC) were obtained with diameters ranging from ca. 30 nm to 3 μm and zeta potential values ranging from ca. −35 mV to −1.6 mV in nanopure water. Histamine moieties imparted pH-responsive behavior due to protonation below pH 7, whereas the carboxylates imparted colloidal stability and anionic character. Blending the acid- and histamine-functionalized polymers produced co-assemblies with different pH-dependent surface charge profiles. In particular, co-assemblies with 60 wt% histamine-modified PDLLA- b -PDGC ( f histamine = 0.6) swelled upon acidification from physiological pH (7.4) to endolysosomal pH (5.5), which is anticipated to enable drug release within endolysosomal compartments. The accessible procedures presented here for engineering highly tunable nanoparticles from glucose-based, functional, degradablemore »polymers offer versatile strategies for accelerating the development and clinical implementation of such stimuli-responsive, tailored nanocarriers.« less