Single atomic metal–N–C materials have attracted immense interest as promising candidates to replace noble metal‐based electrocatalysts for the oxygen reduction reaction (ORR). The coordination environment of metal–N–C active centers plays a critical role in determining their catalytic activity and durability, however, attention is focused only on the coordination of metal atoms. Herein, Fe single atoms and clusters co‐embedded in N‐doped carbon (Fe/NC) that deliver the synergistic enhancement in pH‐universal ORR catalysis via the four‐electron pathway are reported. Combining a series of experimental and computational analyses, the geometric and electronic structures of catalytic sites in Fe/NC are revealed and the neighboring Fe clusters are shown to weaken the binding energies of the ORR intermediates on Fe–N sites, hence enhancing both catalytic kinetics and thermodynamics. This strategy provides new insights into the understanding of the mechanism of single atom catalysis.
Sulfur powder was coated with poly(3,4-ethylenedioxythiophene)-polystyrenesulfonic acid (PEDOT:PSS) using a wet mixing process in water. The modified sulfur material was investigated for use as a cathode in lithium-sulfur (Li-S) batteries. The surface modification with the conducting polymer was identified with Fourier transform infrared (FTIR) spectra, scanning electron microscopy (SEM), and high-resolution transmission electron microscopy (HR-TEM) analyses. Electrochemical evaluation revealed that surface modification with PEDOT:PSS leads to increases in initial capacity and improvements in the rate capability and cyclability of sulfur electrodes. Electrochemical impedance spectroscopy (EIS) measurements certified a decreased resistance of the PEDOT:PSS-coated sulfur electrode compared to a pure sulfur electrode, indicating that surface modification with a conducting polymer effectively enhanced the electrochemical performance of sulfur electrodes in Li-S batteries.
It is still a challenging task to develop a facile and scalable process to synthesize porous hybrid materials with high electrochemical performance. Herein, a scalable strategy is developed for the synthesis of few-layer MoS2 incorporated into hierarchical porous carbon (MHPC) nanosheet composites as anode materials for both Li- (LIB) and Na-ion battery (SIB). An inexpensive oleylamine (OA) is introduced to not only serve as a hinder the stacking of MoS2 nanosheets but also to provide a conductive carbon, allowing large scale production. In addition, a SiO2 template is adopted to direct the growth of both carbon and MoS2 nanosheets, resulting in the formation of hierarchical porous structures with interconnected networks. Due to these unique features, the as-obtained MHPC shows substantial reversible capacity and very long cycling performance when used as an anode material for LIBs and SIBs, even at high current density. Indeed, this material delivers reversible capacities of 732 and 280 mA h g(-1) after 300 cycles at 1 A g(-1) in LIBs and SIBs, respectively. The results suggest that these MHPC composites also have tremendous potential for applications in other fields.
Few‐layer black phosphorus (BP) is an emerging 2D material suitable for energy applications. However, its controllable preparation remains challenging. Herein, a highly efficient route is presented for the scalable production of few‐layered BP nanosheets using a pulsed laser in low‐boiling point solvents. Changing the laser irradiation time, energy, and solvent type leads to precise control over the layer number and lateral size of the nanosheets with a narrow distribution. The process is understood by a plasma quenching mechanism and interlayer interaction weakened by the in situ generated vapor bubbles. The excellent control of the BP nanosheets enables morphological effects on Li‐ion battery performance to be studied. Low layer numbers benefit both charge transfer and Li+ ion diffusion, while a high aspect ratio can not only improve the charge transfer but also increase the Li+ ion diffusion path. This study delivers insights on the tailored fabrication of thin 2D materials using lasers for morphology‐dependent electrochemical energy conversion and storage.
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