Interlayer dual-metal atom Ni-Co catalysts for electrochemical CO2 reduction reactions

A practical strategy was proposed to prepare interlayer Ni-Co DACs. • The Ni-Co DACs achieve a high FE CO of 97% at −0.7 V. • The interlayer Ni-Co DACs possess superior catalytic activity, selectivity, and durability. Developing highly efficient, selective, and stable electrocatalysts for the electrochemical CO 2 reduction reaction (CO 2 RR) is crucial for mitigating energy and environmental challenges. This work presents a practical strategy for synthesizing spatially discrete yet strongly synergistic interlayer dual-metal atom catalysts (DACs) with a Ni-Co configuration through pyrolysis of core-shell zeolite imidazolate frameworks (ZIFs). The resulting CoNC@NiNC catalyst features a core-shell structure where CoNC is encapsulated within NiNC. The strong interaction between the layers of NiNC and CoNC increases the density of active sites, ensures the stability of the structure, facilitates mass or charge transfer, and may produce synergistic interaction between the active sites in core and shell, which can effectively catalyze the conversion of CO 2 to CO. Benefiting from the unique interlayer Ni-Co configuration, the CoNC@NiNC electrocatalyst achieved minimal onset overpotential, high CO Faraday efficiency (FE CO = 97%), and robust operational stability at −0.7 V vs. reversible hydrogen electrode ( vs. RHE). This study demonstrates the promising potential of interlayer DACs for efficient CO 2 RR, more importantly, establishes a viable method for developing interlayer DACs, utilizes the strong interlayer interactions to drive this complex reaction, and inspires further exploration of interlayer DACs in energy conversion and beyond. Download: Download high-res image (152KB) Download: Download full-size image The interlayer dual-metal atom catalysts (DACs) with controlled local coordination environments and three-dimensional spatial structures can efficiently convert CO 2 into high-value chemicals or fuels. Herein, a practical strategy was proposed to prepare interlayer Ni-Co DACs, which have core-shell structure consisted of CoNC encapsulated within NiNC (denoted as CoNC@NiNC), by self-assembly and high-temperature pyrolysis core-shell zeolite imidazolate frameworks (ZIFs) precursor. The practice reveal that the interlayer Ni-Co DACs possess superior catalytic activity, selectivity, and durability, which demonstrates the great potential as highly efficient catalysts for CO 2 RR.