Core@shell structured Au@SnO2 nanoparticles with improved N2 adsorption/activation and electrical conductivity for efficient N2 fixation

Pengtang Wang^a,1, Yujin Ji^b,1, Qi Shao^a, Youyong Li^b, Xiaoqing Huang^{a, *}（黄小青）

^aCollege of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China

^bInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China

¹These authors contributed equally to this work.

Science Bulletin 65(2020) 350--358

The design of electrocatalysts with enhanced adsorption and activation of nitrogen (N₂) is critical for boosting the electrochemical N₂reduction (ENR). Herein, we developed an efficient strategy to facilitate N₂adsorption and activation for N₂electroreduction into ammonia (NH₃) by vacancy engineering of core@shell structured Au@SnO₂nanoparticles (NPs). We found that the ultrathin amorphous SnO₂shell with enriched oxygen vacancies was conducive to adsorb N₂as well as promoted the N₂activation, meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N₂reduction reaction, synergistically boosting the N₂electroreduction catalysis. As confirmed by the¹⁵N-labeling and controlled experiments, the core@shell Au@amorphous SnO₂NPs with abundant oxygen vacancies show the best performance for N₂electroreduction with the NH₃yield rate of 21.9 μg h⁻¹mg⁻¹_catand faradaic efficiency of 15.2% at −0.2 V_RHE, which surpass the Au@crystalline SnO₂NPs, individual Au NPs and all reported Au-based catalysts for ENR.

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