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ACS Nano. 2015 Jan 27;9(1):931-40. doi: 10.1021/nn506701x. Epub 2015 Jan 8.

Porous C3N4 nanolayers@N-graphene films as catalyst electrodes for highly efficient hydrogen evolution.

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School of Chemical Engineering, The University of Adelaide , Adelaide, South Australia 5005, Australia.


Pt-free electrocatalysts for hydrogen evolution reaction (HER) with high activity and low price are desirable for many state-of-the-art renewable energy devices, such as water electrolysis and photoelectrochemical water splitting cells. However, the design and fabrication of such materials remain a significant challenge. This work reports the preparation of a flexible three-dimensional (3D) film by integrating porous C3N4 nanolayers with nitrogen-doped graphene sheets, which can be directly utilized as HER catalyst electrodes without substrates. This nonmetal electrocatalyst has displayed an unbeatable HER performance with a very positive onset-potential close to that of commercial Pt (8 mV vs 0 mV of Pt/C, vs RHE @ 0.5 mA cm(-2)), high exchange current density of 0.43 mA cm(-2), and remarkable durability (seldom activity loss >5000 cycles). The extraordinary HER performance stems from strong synergistic effect originating from (i) highly exposed active sites generated by introduction of in-plane pores into C3N4 and exfoliation of C3N4 into nanosheets, (ii) hierarchical porous structure of the hybrid film, and (iii) 3D conductive graphene network.


carbon nitride nanolayers; hydrogen evolution reaction; nitrogen doped graphene; two-dimensional materials; van der Waals heterostructure


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