Developing efficient and robust non‐precious‐metal‐based catalysts to accelerate electrocatalytic reaction kinetics is crucial for electrochemical water‐urea splitting. Herein, Fe‐doped NiS–NiS2 heterostructured microspheres, an electrocatalyst, are synthesized via etching Prussian blue analogues following a controlled annealing treatment. The resulting microspheres are constructed by mesoporous nanoplates, granting the virtues of large surface areas, high structural void porosity, and accessible inner surface. These advantages not only provide more redox reaction centers but also strengthen structural robustness and effectively facilitate the mass diffusion and charge transport. Density functional theory simulations validate that the Fe‐doping improves the conductivity of nickel sulfides, whereas the NiS–NiS2 heterojunctions induce interface charge rearrangement for optimizing the adsorption free energy of intermediates, resulting in a low overpotential and high electrocatalytic activity. Specifically, an ultralow overpotential of 270 mV at 50 mA cm−2 for the oxygen evolution reaction (OER) is achieved. After adding 0.33 M urea into 1 M KOH, Fe‐doped NiS–NiS2 obtains a strikingly reduced urea oxidation reaction potential of 1.36 V to reach 50 mA cm−2, around 140 mV less than OER. This work provides insights into the synergistic modulation of electrocatalytic activity of non‐noble catalysts for applications in energy conversion systems.
Image inpainting is a technique that aims to fill in the missing regions with visually plausible content. However, an opposite idea, which is painting outside images, receives little work. In this study, we investigate the issue of image outpainting. Considering that the model needs better prediction ability as there is less neighboring information in image outpainting, the study proposes a novel image outpainting architecture that can obtain both deep model performance and detailed information. To fully take advantage of residual learning, dense residual (DR) learning is proposed and the image generative network is built on DR. To avoid losing subtle information caused by downsampling in encoder-decoder, shortcuts are added for transferring previous knowledge. Different from vanilla U-Net, we propose a skip method of the semicomplete form. Experimental results show that the proposed method achieves excellent performance.
Heteroatom doping and crystal facet engineering are effective strategies to improve the intrinsic activity of catalysts by tuning its chemical composition and electronic structure. Herein, uniform monodispersed CuFe(SxSe1-x)2 nanoplates with...
considered ideal solutions for achieving energy conversion and storage in a sustainable way. [2] Nowadays, the key challenges of using these technologies and devices lie in the developments of more efficient and stable electrode materials. For the electrochemical water splitting, due to the high overpotential and intrinsically sluggish reaction kinetics of the oxygen evolution reaction (OER), low-cost, high efficiency and stable earth-abundant electrocatalysts are required to enhance the energy conversion efficiency. [3] Similarly, the commercial graphite anode materials for LIBs have limited inherent theoretical capacity (≈372 mAh g −1 ), which cannot meet the requirements of high energy density batteries for rapidly growing smartphone, electrical vehicles, and aerospace applications. How to further improve the energy density of LIBs faces great challenges. Therefore, it is urgent to invent competitive multifunctional electrode nanomaterials with suitable components and architectures for highly efficient OER electrocatalysts and highperformance LIBs.Recently, iron-based oxides have been widely studied in the fields of energy storage and conversions owing to their high electrochemical activity, rich redox properties, natural abundance, and simple preparation. [4] However, the electrocatalytic activity of Fe-based oxides is highly dependent on theirThe development of high-efficiency, robust, and available electrode materials for oxygen evolution reaction (OER) and lithium-ion batteries (LIBs) is critical for clean and sustainable energy system but remains challenging. Herein, a unique yolk-shell structure of Fe 2 O 3 nanotube@hollow Co 9 S 8 nanocage@C is rationally prepared. In a prearranged sequence, the fabrication of Fe 2 O 3 nanotubes is followed by coating of zeolitic imidazolate framework (ZIF-67) layer, chemical etching of ZIF-67 by thioacetamide, and eventual annealing treatment. Benefiting from the hollow structures of Fe 2 O 3 nanotubes and Co 9 S 8 nanocages, the conductivity of carbon coating and the synergy effects between different components, the titled sample possesses abundant accessible active sites, favorable electron transfer rate, and exceptional reaction kinetics in the electrocatalysis. As a result, excellent electrocatalytic activity for alkaline OER is achieved, which delivers a low overpotential of 205 mV at the current density of 10 mA cm −2 along with the Tafel slope of 55 mV dec −1 . Moreover, this material exhibits excellent high-rate capability and excellent cycle life when employed as anode material of LIBs. This work provides a novel approach for the design and the construction of multifunctional electrode materials for energy conversion and storage.
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