Architecting Flower-like ZnS/CoS Heterojunction for Efficient N2 Electroreduction to NH3

Electrocatalytic nitrogen reduction reaction (NRR) is a highly promising process for ammonia synthesis and holds great potential to replace the traditional Haber-Bosch process. Unfortunately, current catalysts have encountered significant challenges in the adsorption and activation of N2, which have greatly impeded the NRR progress. The evolution of catalysts with more active sites for nitrogen chemisorption and relative protonation plays a crucial role in achieving nitrogen reduction in ammonia synthesis. In this work, we report a novel flower-like ZnS/CoS composite electrocatalyst that employs CoS as a precursor and introduces ZnS with varying molar content to fabricate heterostructures, thereby creating electron-deficient and electron-rich regions. This design strategy provides abundant sites for N2 attachment and facilitates the interfacial electronic flow. Remarkably, the ZnS/CoS-105 heterojunction catalyst achieves a NH3 yield rate of 20.42 μg h−1 mgcat.−1 and a Faradaic efficiency (FE) of 11.83% at -0.45 V vs. RHE in 0.1 M Na2SO4 aqueous solution. In addition, the ZnS/CoS-105 shows an remarkable stability (up to 24 h) for the NRR process. This work demonstrates the immense potential of transition metal electrocatalysts and provides an alternative pathway in NRR electrocatalysis.

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