Dry reforming of methane (DRM) can simultaneously convert two critical greenhouse gases CH4 and CO2 into high-value syngas. However, the catalyst deactivation caused by sintering and carbon deposition of Ni-based catalysts at high temperature is a significant problem to be solved for DRM industrialization. Herein, we represent a hierarchical Ni-La@S-1 catalyst for DRM reaction, showing high anti-sintering/coke capacity to improve DRM stability. The La and Ni nitrates were first grinded into the pores of SBA-15 followed by N2-treatment; the sample was then recrystallized by a unique template assisted-uniformly dispersed strategy to obtain the hierarchical Ni-La@S-1 catalyst. This strategy achieves uniform encapsulation of stabilized Ni-La bimetallic nanoparticles in S-1 with high loading, exhibiting high DRM activity and stability at 700 °C and 36,000 mL·g–1·h–1. Moreover, La addition promoted CO2 to form bidentate carbonate, a critical intermediate in DRM, which greatly ameliorated carbon deposition in Ni catalysts. This work offers promising clue for tailoring the industrial DRM catalysts.
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Carbon materials featuring hierarchical pores and atomically dispersed metal sites are promising catalysts for energy storage and conversion applications. Herein, we developed a facile strategy to construct functional carbon materials with a fluffy peony-like structure and dense binary FeCo-Nx active sites (termed as f-FeCo-CNT). By regulating the metal content in precursors, a three-dimensional (3D) interconnected conductive carbon nanotubes network was in-situ formed throughout the atomically dispersed FeCo-NC matrix during pyrolysis. Taking advantage of rich pore hierarchy and co-existence of highly active FeCo-Nx sites and beneficial FeCo alloy nanoparticles, the f-FeCo-CNT material exhibited excellent bifunctional performance towards oxygen reduction reaction/oxygen evolution reactions (ORR/OER) with respect to the atomically dispersed FeCo-NC (SA-f-FeCo-NC) and commercial Pt/C+RuO2 mixture, surpassing the SA-f-FeCo-NC with a 20 mV higher ORR half-wave potential and a 100 mV lower OER overpotential (at 10.0 mA/cm2). Remarkably, the f-FeCo-CNT-assembled Zn-air battery (ZAB) possessed a maximum specific power of 195.8 mW/cm2, excellent rate capability, and very good cycling stability at large current density of 20.0 mA/cm2. This work provides a facile and feasible synthetic strategy of constructing low-cost cathode materials with excellent comprehensive ZAB performance.
The careful design of nano-architectures and smart hybridization of expected active materials can lead to more advanced properties. Here we have engineered a novel hierarchical branching Cu/Cu2O/CuO heteronanostructure by combining a facile hydrothermal method and subsequent controlled oxidation process. The fine structure and epitaxial relationship between the branches and backbone are investigated by high-resolution transmission electron microscopy. Moreover, the evolution of the branch growth has also been observed during the gradual oxidation of the Cu nanowire surface. The experimental results suggest that the surface oxidation needs to be performed via a two-step exposure process to varying humidity in order to achieve optimized formation of a core-shell structured branching architecture. Finally, a proof-of-concept of the function of such a hierarchical framework as the anode material in lithium-ion batteries is demonstrated. The branching core-shell heterostructure improves battery performance by several means: (i) The epitaxially grown branches provide a high surface area for enhanced electrolyte accessibility and high resistance to volume change induced by Li+ intercalation/extraction; (ii) the core-shell structure with its well-defined heterojunction increases the contact area which facilitates effective charge transport during lithiation; (iii) the copper core acts as a current collector as well as providing structural reinforcement.