Platinum-nanoparticle-based catalysts are widely used in many important chemical processes and automobile industries. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their use efficiency, however, very challenging. Here we report a practical synthesis for isolated single Pt atoms anchored to graphene nanosheet using the atomic layer deposition (ALD) technique. ALD offers the capability of precise control of catalyst size span from single atom, subnanometer cluster to nanoparticle. The single-atom catalysts exhibit significantly improved catalytic activity (up to 10 times) over that of the state-of-the-art commercial Pt/C catalyst. X-ray absorption fine structure (XAFS) analyses reveal that the low-coordination and partially unoccupied densities of states of 5d orbital of Pt atoms are responsible for the excellent performance. This work is anticipated to form the basis for the exploration of a next generation of highly efficient single-atom catalysts for various applications.

Micropores are largely responsible for Fe/N/C catalytic activity, but are also intrinsically responsible for the rapid initial performance loss in PEMFC.

Rechargeable aqueous zinc‐ion batteries (ZIBs) have been emerging as potential large‐scale energy storage devices due to their high energy density, low cost, high safety, and environmental friendliness. However, the commonly used cathode materials in ZIBs exhibit poor electrochemical performance, such as significant capacity fading during long‐term cycling and poor performance at high current rates, which significantly hinder the further development of ZIBs. Herein, a new and highly reversible Mn‐based cathode material with porous framework and N‐doping (MnOx@N‐C) is prepared through a metal–organic framework template strategy. Benefiting from the unique porous structure, conductive carbon network, and the synergetic effect of Zn2+ and Mn2+ in electrolyte, the MnOx@N‐C shows excellent cycling stability, good rate performance, and high reversibility for aqueous ZIBs. Specifically, it exhibits high capacity of 305 mAh g−1 after 600 cycles at 500 mA g−1 and maintains achievable capacity of 100 mAh g−1 at a quite high rate of 2000 mA g−1 with long‐term cycling of up to 1600 cycles, which are superior to most reported ZIB cathode materials. Furthermore, insight into the Zn‐storage mechanism in MnOx@N‐C is systematically studied and discussed via multiple analytical methods. This study opens new opportunities for designing low‐cost and high‐performance rechargeable aqueous ZIBs.

No abstract