Boron-Doped Graphene for Electrocatalytic N2 Reduction
2018; Elsevier BV; Volume: 2; Issue: 8 Linguagem: Inglês
10.1016/j.joule.2018.06.007
ISSN2542-4785
AutoresXiao-Min Yu, Peng Han, Zengxi Wei, Linsong Huang, Zhengxiang Gu, Sijia Peng, Jianmin Ma, Gengfeng Zheng,
Tópico(s)Hydrogen Storage and Materials
ResumoElectrochemical N2 reduction in aqueous solutions at ambient conditions is extremely challenging and requires rational design of electrocatalytic centers. We demonstrate a boron-doped graphene as an efficient metal-free N2 reduction electrocatalyst. Boron doping in the graphene framework leads to redistribution of electron density, where the electron-deficient boron sites provide enhanced binding capability to N2 molecules. Density functional theory calculations reveal the catalytic activities of different boron-doped carbon structures, in which the BC3 structure enables the lowest energy barrier for N2 electroreduction to NH3. At a doping level of 6.2%, the boron-doped graphene achieves a NH3 production rate of 9.8 μg·hr−1·cm−2 and one of the highest reported faradic efficiencies of 10.8% at −0.5 V versus reversible hydrogen electrode in aqueous solutions at ambient conditions. This work suggests the strong potential of atomic-scale design for efficient electrocatalysts for N2 reduction.
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