Constructing monodispersed metal sites in heterocatalysis is an efficient strategy to boost their catalytic performance. Herein, a new strategy using monodispersed metal sites to tailor Pt-based nanocatalysts is addressed by engineering unconventional p-d orbital hybridization. Thus, monodispersed Ga on Pt 3 Mn nanocrystals (Ga-O-Pt 3 Mn) with high-indexed facets was constructed for the first time to drive ethanol electrooxidation reaction (EOR). Strikingly, the Ga-O-Pt 3 Mn nanocatalyst shows an enhanced EOR performance with achieving 8.41 times of specific activity than that of Pt/C. The electrochemical in situ Fourier transform infrared spectroscopy results and theoretical calculations disclose that the Ga-O-Pt 3 Mn nanocatalyst featuring an unconventional pd orbital hybridization not only promote the CÀ C bondbreaking and rapid oxidation of -OH of ethanol, but also inhibit the generation of poisonous CO intermediate species. This work discloses a promising strategy to construct a novel nanocatalysts tailored by monodispersed metal site as efficient fuel cell catalysts.
The electroreduction of carbon dioxide is a promising strategy to synthesize value‐added feedstocks and realize carbon neutralization. Copper catalysts are well‐known to be active for selective electroreduction of CO2 to multicarbon products, although the role played by the surface architecture is not fully understood. Herein, mesoporous Cu nanoribbons are constructed via in‐situ electrochemical reduction of Cu based metal organic frameworks for the highly selective synthesis of C2+ chemicals. With the mesoporous structure, a high C2+ Faradaic efficiency of 82.3% with a partial current density of 347.9 mA cm−2 is achieved in a flow‐cell electrolyzer. Controlled electroreduction of CO2 with Cu nanoribbons exhibited clearly greater selectivity towards C2+ products than Cu nanoleaves and Cu nanorods without porous structures. Finite difference time domain results indicate that the mesoporous structure can enhance the electric field on the catalyst surface, which increases the concentration of K+ and OH−, thus allowing the authors to promote CO2 reduction pathways towards C2+ products.
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