In the context of the energy crisis and sustainable development, the electrocatalytic nitrogen reduction reaction (NRR) for ammonia synthesis with zero-carbon emission characteristics holds great promise. Developing highly efficient electrocatalysts with high ammonia yield and Faradaic efficiency (FE) for the nitrogen reduction reaction process(NRR) is crucial for enhancing the efficiency of ammonia synthesis. The modulation of electronic structure through interface engineering and vacancy engineering is a new approach to enhance the performance of catalyst. In this paper, we propose an efficient Cu2S@Co3S4/CF catalyst with core-shell heterojunction structure and sulfur vacancies, which exhibited an ammonia yield of 122 μg·h-1·cm-2 and a Faradaic efficiency of 34.6%, with the ammonia synthesis rate remaining consistently stable over 6 cycles of testing, outperforming most reported similar catalysts. Comprehensive experiments and characterization demonstrate that the high performance of the catalyst is attributed to the Cu2S core will donate electrons to the Co3S4 shell through a uniform interface, which can promote the hydrogenation reactions of NRR while retarding the coupling of *H to form byproduct hydrogen, which contribute to a more optimal balance between the rate of ammonia production and the Faraday efficiency, additionly, the formation of abundant sulfur vacancies significantly enhancing nitrogen adsorption performance in this material. Moreover, the Zn‐N2 battery assembled with Cu2S@Co3S4/CF shows an excellent power density of 14.6 mW cm-2, which enables the simultaneous ammonia production and energy supply. This work demonstrates a promising approach to develop highly efficient electrocatalysts for sustainable ammonia production, with significant implications for addressing the energy crisis and promoting the transition towards a low-carbon economy.
Guo Chaofan
,
Su jinzhan
,
Guo Liejin
. Nitrogen reduction properties of Cu2S@Co3S4/CF core-shell heterojunction catalysts with built-in electric field effect[J]. Acta Chimica Sinica, 0
: 2
-2
.
DOI: 10.6023/A25030091
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