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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS	Designed TiS 2 nanosheets for efficient electrocatalytic reductive amination of biomass-derived furfurals Man Zhang , Shaojun Xu , Mebrouka Boubeche , Donato Decarolis , Yizhe Huang , Biying Liu , Emma K. Gibson , Xin Li , Yuchen Wang , Huixia Luo , C. Richard A. Catlow , Kai Yan Green Chemistry 9 DOI: 10.1039/D2GC03234A Diamond Proposal Number(s): [19850] Show Abstract ▼ Abstract: Green and highly selective synthesis of organonitrogen chemicals (ONCs) using the renewable energy source biomass over noble-metal free solid catalysts under common room temperature and pressure conditions is still a major challenge. Here, we report a sustainable electrochemical method for selective synthesis of several valuable ONCs with high yields using biomass-derived furanic aldehydes over greenly fabricated TiS2 nanosheets through a facile synthesis. Based on a range of characterization techniques including high-resolution transmission electron microscopy and X-ray absorption fine structure, a well-defined structure of the TiS2 nanosheets (3.86 nm with 1T phase) was constructed. These as-prepared catalysts were applied to the electrochemical reductive amination (ERA) of three biomass-derived aldehydes, i.e. furfural (FF), 5-methylfurfural (MF) and 5-hydroxymethylfurfural (HMF), and exhibited superior performance whereby over 95% conversion of each furanic aldehyde and nearly perfect selectivity of ONCs were achieved. TiS2 nanosheets, in particular, exhibited a marked ∼2-fold increase in conversion (∼49%) compared with the monometallic Ti electrode. Besides, the reaction kinetics and rational pathway were also studied. In addition, these exfoliated TiS2 nanosheets maintained high durability over 6 h, providing a promising and versatile route for the sustainable upgrading of biomass-derived sources.	Nov 2022
B18-Core EXAFS	Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina Bingqiao Xie , Roong Jien Wong , Tze Hao Tan , Michael Higham , Emma K. Gibson , Donato Decarolis , June Callison , Kondo-Francois Aguey-Zinsou , Michael Bowker , C. Richard A. Catlow , Jason Scott , Rose Amal Nature Communications 11 DOI: 10.1038/s41467-020-15445-z Diamond Proposal Number(s): [19850] Open Access Show Abstract ▼ Abstract: Although photoexcitation has been employed to unlock the low-temperature equilibrium regimes of thermal catalysis, mechanism underlining potential interplay between electron excitations and surface chemical processes remains elusive. Here, we report an associative zinc oxide band-gap excitation and copper plasmonic excitation that can cooperatively promote methanol-production at the copper-zinc oxide interfacial perimeter of copper/zinc oxide/alumina (CZA) catalyst. Conversely, selective excitation of individual components only leads to the promotion of carbon monoxide production. Accompanied by the variation in surface copper oxidation state and local electronic structure of zinc, electrons originating from the zinc oxide excitation and copper plasmonic excitation serve to activate surface adsorbates, catalysing key elementary processes (namely formate conversion and hydrogen molecule activation), thus providing one explanation for the observed photothermal activity. These observations give valuable insights into the key elementary processes occurring on the surface of the CZA catalyst under light-heat dual activation.	Mar 2020

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