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Abstract Metal-free electrocatalysts represent a main branch of active materials for oxygen evolution reaction (OER), but they excessively rely on functionalized conjugated carbon materials, which substantially restricts the screening of potential efficient carbonaceous electrocatalysts. Herein, we demonstrate that a mesostructured polyacrylate hydrogel can afford an unexpected and exceptional OER activity – on par with that of benchmark IrO 2 catalyst in alkaline electrolyte, together with a high durability and good adaptability in various pH environments. Combined theoretical and electrokinetic studies reveal that the positively charged carbon atoms within the carboxylate units are intrinsically active toward OER, and spectroscopic operando characterizations also identify the fingerprint superoxide intermediate generated on the polymeric hydrogel backbone. This work expands the scope of metal-free materials for OER by providing a new class of polymeric hydrogel electrocatalysts with huge extension potentials. 

Here, we study the upper critical solution temperature triggered phase transition of thermally responsive poly(ethylene glycol)-block-poly(ethylene glycol) methyl ether acrylate-co-poly(ethylene glycol) phenyl ether acrylate-block-polystyrene nanoassemblies in isopropanol. To gain mechanistic insight into the organic solution-phase dynamics of the upper critical solution temperature polymer, we leverage variable temperature liquid-cell transmission electron microscopy correlated with variable temperature liquid resonant soft X-ray scattering. Heating above the upper critical solution temperature triggers a reduction in particle size and a morphological transition from a spherical core shell particle with a complex, multiphase core to a micelle with a uniform core and Gaussian polymer chains attached to the surface. These correlated solution phase methods, coupled with mass spectral validation and modeling, provide unique insight into these thermoresponsive materials. Moreover, we detail a generalizable workflow for studying complex, solution-phase nanomaterials via correlative methods.

 

Abstract Paper-based electrochemical sensors provide the opportunity for low-cost, portable and environmentally friendly single-use chemical analysis and there are various reports of surface-functionalized paper electrodes. Here we report a composite paper electrode that is fabricated through designed papermaking using cellulose, carbon fibers (CF), and graphene oxide (GO). The composite paper has well-controlled structure, stable, and repeatable properties, and offers the electrocatalytic activities for sensitive and selective chemical detection. We demonstrate that this CF/GO/cellulose composite paper can be reduced electrochemically using relatively mild conditions and this GO reduction confers electrocatalytic properties to the composite paper. Finally, we demonstrate that this composite paper offers sensing performance (sensitivity and selectivity) comparable to, or better than, paper-based sensors prepared by small-batch surface-modification (e.g., printing) methods. We envision this coupling of industrialized papermaking technologies with interfacial engineering and electrochemical reduction can provide a platform for single-use and portable chemical detection for a wide range of applications.