Fe induced geometric/electronic structure engineering in YSZ nanosheets for enhanced electrocatalytic nitrogen reduction reactions
Constructing 2D geometric structure and optimize electronic structure of transition metal oxide have been demonstrated to be effective strategy to reinforce its electrochemical dinitrogen reduction reaction (NRR) performances. But combining these two advantages into metal oxide based electrocatalyst simultaneously to achieve synergic effects remains one technological challenge but very significant. Here, a self-sacrificing template coupling with Fe doped strategy were proposed to optimize the geometric and electronic structure of Zr-based electrocatalyst. Experimental results revealed that the optimal sample 2Fe-YSZ was endowed with uniform 2D heterostructures, rich oxygen vacancy and increased electronic density, which induced by the framework Fe element. These traits thus confer the 2Fe-YSZ produced through extensive exposure to extra active sites, significantly boosting the absorption and activation of N 2 molecules. And the DFT calculation further validates the promotive effect of framework Fe. As expected, in the electrocatalytic NRR test, 2Fe-YSZ demonstrated high Faradaic efficiency (38.89 %) and NH 3 yield rate (19.58 μg h −1 mg −1 ) at − 0.5 V in 0.1 M HCl, comparable to most Zr-based electrocatalytic materials for ambient NRR. This geometric/electronic structure engineering strategy could provide an idea the rational design of efficient NRR catalysts.
危险品化学品经营许可证（带存储）