Transformation of biomass into valuable nitrogen-containing compounds is highly desired, yet limited success has been achieved. Here we report an efficient catalyst system, partially reduced Ru/ZrO , which could catalyze the reductive amination of a variety of biomass-derived aldehydes/ketones in aqueous ammonia. With this approach, a spectrum of renewable primary amines was produced in good to excellent yields. Moreover, we have demonstrated a two-step approach for production of ethanolamine, a large-market nitrogen-containing chemical, from lignocellulose in an overall yield of 10 %. Extensive characterizations showed that Ru/ZrO -containing multivalence Ru association species worked as a bifunctional catalyst, with RuO as acidic promoter to facilitate the activation of carbonyl groups and Ru as active sites for the subsequent imine hydrogenation.
Single-atom Rh catalysts present superior activity relative to homogeneous catalyst in olefins hydroformylation, yet with limited success in regioselectivity control. In the present work, we develop a phosphorus coordinated Rh1 single-atom catalyst with nanodiamond as support. Benefiting from this unique structure, the catalyst exhibits excellent activity and regioselectivity in hydroformylation of arylethylenes with wide substrate generality, i.e., with high conversion (>99%) and high regioselectivity (>90%), which is comparable with the homogeneous counterparts. The coordination interaction between Rh1 and surface phosphorus species is clarified by 31P solid-state NMR and X-ray absorption spectroscopy (XAS). Rh single atoms are firmly anchored over nanodiamond through Rh-P bonds, guaranteeing good stability in the hydroformation of styrene even after six runs. Finally, by using this catalyst, two kinds of pharmaceutical molecules, Ibuprofen and Fendiline, are synthesized efficiently with high yields, demonstrating a new prospect of single-atom catalyst in pharmaceutical synthesis.
The salt effect of Na x A (A = SO 4 2− , Cl − , NO 3 − , etc.) on the hydrothermal carbonization of biomass is reported. It is a new catalyst and recyclable template to more simply and effectively prepare carbon-based materials, such as porous carbon-coated anode materials (e.g., Fe 3 O 4 @porous-C) in lithium-ion battery applications with enhanced performance. † Electronic supplementary information (ESI) available: Experimental part and characterization. Digital pictures of viewable autoclave. CHN analysis. HPLC and GC-MS analysis of the residual solution. Digital and SEM images of carbon materials catalyzed by different kinds of metal salt. Digital pictures of the two types of hydrothermal autoclave. See
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