Double-atom catalysts: transition metal dimer-anchored C2N monolayers as N2 fixation electrocatalysts

作者：Zhang, Xu; Chen, An; Zhang, Zihe; Zhou, Zhen^*

来源：Journal of Materials Chemistry A, 2018, 6(38): 18599-18604.

DOI：10.1039/c8ta07683a

• NITROGEN-FIXATION
• AMMONIA-SYNTHESIS
• ELECTRIC-FIELD
• REDUCTION
• CONVERSION
• DINITROGEN
• ALGORITHM
• POINTS

Nitrogen fixation is one of the most essential processes in chemistry. Developing more effective nitrogen fixation systems to catalyze the reaction under mild conditions is one of the most attractive but long-standing challenges. In this work, by means of first-principles computations, we systematically investigated the catalytic performance of transition metal atom-anchored C2N monolayer electrocatalysts (TMx@C2N, x = 1 or 2; TM = Ti, Mn, Fe, Co, Cu, Mo, Ru, Rh, Pd, Ag, Ir, Pt, or Au) for N-2 fixation. The natively N edged uniform holes could fix the TM atoms firmly in TM-Nx configurations, which is beneficial for the N-2 fixation. Among them, Mo-2@C2N exhibits the best catalytic performance for the reduction of N-2 to NH3 with a maximum free energy change of 0.41 eV and an energy barrier of 0.51 eV, indicating that Mo-2@C2N is a promising catalyst with high catalytic activity for the reduction of N-2 to NH3. We believe that this work could provide a new idea for the design of N-2 fixation catalysts and shed light on C2N monolayers as excellent substrates for catalysis.

• 出版日期2018-10-14
• 单位南开大学