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  1. The structural versatility and vibrant surface chemistry of carbon materials offer tremendous opportunities for tailoring the catalytic performance of supported metal nanoparticles through the modulation of interfacial metal-support interactions (MSI). MSI’s geometric and structural effects are well documented for these materials. However, other potential support effects such as electronic metal-carbon interactions remain poorly understood. Such limitations are tied to constraints intrinsic to commonly available carbon materials such as activated carbon (e.g., microporosity) and the top-down approach that is often used for their synthesis. Nonetheless, it is crucial to understand the interplay between the structure, properties, and performance of carbon-supported metal catalysts to take steps toward rationalizing their design. The present study investigates promising and scalable bottom-up synthesis approaches, namely hydrothermal carbonization (HTC) and evaporation-induced self-assembly (EISA), that offer great flexibility for controlling the carbon structure. The opportunities and limitations of the methods are discussed with a particular focus on harnessing the power of oxygen functionalities. A remarkable production yield of 32.8% was achieved for mesoporous carbons synthesized via EISA. Moreover, these carbon materials present similar external surface areas of 316 ± 19 m2/g and average pore sizes of 10.0 ± 0.1 nm while offering flexibility to control the oxygen concentration in the range of 5–26 wt%. This study provides the cornerstone for future investigations of metal-carbon support interactions and the rational design of these catalysts. 
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  3. Abstract

    Biorefineries aim to convert biomass into a spectrum of products ranging from biofuels to specialty chemicals. To achieve economically sustainable conversion, it is crucial to streamline the catalytic and downstream processing steps. In this work, a route that combines bio‐ and electrocatalysis to convert glucose into bio‐based unsaturated nylon‐6,6 is reported. An engineered strain of Saccharomyces cerevisiae was used as the initial biocatalyst for the conversion of glucose into muconic acid, with the highest reported muconic acid titer of 559.5 mg L−1in yeast. Without any separation, muconic acid was further electrocatalytically hydrogenated to 3‐hexenedioic acid in 94 % yield despite the presence of biogenic impurities. Bio‐based unsaturated nylon‐6,6 (unsaturated polyamide‐6,6) was finally obtained by polymerization of 3‐hexenedioic acid with hexamethylenediamine.

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