Activating the synergistic effect in Ni-Co bimetallic MOF for enhanced plasma-assisted ammonia synthesis.

[Display omitted] • Novel strategy of bimetallic MOFs for enhanced PAAS is designed. • The enhanced PAAS is ascribed to the improved mass transfer in MOFs. • Sustainable NH 3 production rate achieves 77.5 μmol g−1·min−1 in 36 h or ∼ 30 cycles. • Hypothetical zero-carbon ammonia plant exhibits notable competitiveness. Plasma-assisted ammonia synthesis (PAAS) can produce ammonia using highly energetic, electronically excited nitrogen and Hydrogen radicals at low temperatures and atmospheric pressure, which has been regarded as a prospective alternative to the Haber − Bosch process. PAAS can exclusively use renewable power (solar, wind, etc.) to achieve green, decentralized and efficient ammonia synthesis. However, current catalysts for PAAS are suffering from low efficiency, poor stability and cyclability. Herein, we demonstrate a one-step hydrothermal synthesis of Ni-Co bimetallic metal–organic frameworks (MOFs) for PAAS. Attributed to the amplified gas transport capability and bimetallic coupling, the Ni-Co-MOF exhibits significantly improved PAAS performance: 88.21 μmol g−1·min−1, above 30 % increase over 5 wt% Ni/Al 2 O 3. The high stability of Ni-Co-MOF under the harsh electric field enables its durable performance (36 h) and excellent cyclability (24 cycles). Finally, to determine the viability of PAAS for industrial applications, we construct a hypothetical zero-carbon ammonia plant using only renewable energy sources, and the outcomes indicate that PAAS has significant competitiveness for future ammonia production. [ABSTRACT FROM AUTHOR]