The exploitation of hierarchical carbon nanocages with superior light-to-heat conversion efficiency, together with their distinct structural, morphological, and electronic properties, in photothermal applications could provide effective solutions to long-standing challenges in diverse areas. Here, we demonstrate the discovery of pristine and nitrogen-doped hierarchical carbon nanocages as superior supports for highly loaded, small-sized Ru particles toward enhanced photothermal CO2 catalysis. A record CO production rate of 3.1 mol·gRu–1·h–1 with above 90% selectivity in flow reactors was reached for hierarchical nitrogen-doped carbon-nanocage-supported Ru clusters under 2.4 W·cm–2 illumination without external heating. Detailed studies reveal that the enhanced performance originates from the strong broadband sunlight absorption and efficient light-to-heat conversion of nanocage supports as well as the excellent intrinsic catalytic reactivity of sub-2 nm Ru particles. Our study reveals the great potential of hierarchical carbon nanocages in photothermal catalysis to reduce the fossil fuel consumption of various industrial chemical processes and stimulates interest in their exploitation for other demanding photothermal applications.
Hengcong Tao,Jingjing Ding,Chao Xie,Yunnan Gao,Jinliang Song,Zhenyu Sun
We demonstrate a facile and versatile method to grow Ru particles uniformly on pristine few-layer graphene (FLG) in supercritical diethylamine. In particular, a large number of Ru subnanometer clusters less than 1.0 nm were observed. The particle size can be tuned by manipulating the loading content of Ru and controlling the reaction temperature. The resulting Ru/FLG showed remarkably high activity, selectivity, and reusability towards the hydrogenation of levulinic acid to γ-valerolactone. This method is flexible, and can be extended to the synthesis of a variety of other ultrafine metal particles supported on FLG.
Constructing dual active sites, adjusting electronic structures at interfaces and optimizing the adsorption energy of intermediates can effectively enhance water electrolysis performance. A novel Fe 3 C-Ru/NFs bifunctional catalyst is successfully synthesized via an electrospinning-carbonization method, in which sub-nanometer Ru particles coupled with Fe 3 C. Experimental results indicate that Fe 3 C-Ru/NFs catalyst delivers exceptional HER (18 mV@10 mA cm −2 , 202 mV@500 mA cm −2 ) and OER (263 mV@10 mA cm −2 , 382 mV@500 mA cm −2 ) performance in 1 M KOH solution. Moreover, Fe 3 C-Ru/NFs catalyst was employed as a bifunctional electrode in an overall water electrolyzer, resulting in a lower cell voltage and excellent stability (1.87 V, 150 h @ 500 mA cm −2 ). Density Functional Theory (DFT) calculation shows that the synergy between Ru and Fe sites can enhance electron transfer, and initiate a hydrogen spillover mechanism, and optimize intermediate adsorption energies, finally accelerating both HER and OER processes. This work offers valuable insights into developing low-cost, high-efficiency water electrolysis catalysts, demonstrating the significant potential for practical applications.
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