A General Strategy to Glassy M-Te (M = Ru, Rh, Ir) Porous  Nanorods for Efficient Electrochemical N2  Fixation

Juan Wang^1#, Bolong Huang^2#, Yujin Ji^3#, Mingzi Sun², Tong Wu², Rongguan Yin¹, Xing Zhu⁴, Youyong Li³, Qi Shao¹, and Xiaoqing Huang^1*（黄小青）

¹College of Chemistry Chemical Engineering and Materials Science,Soochow University,Suzhou, Jiangsu 215123, P. R. China

²Department of Applied Biology and Chemical Technology ,The Hong Kong Polytechnic University,Hung Hom, Kowloon, Hong Kong SAR, China

³Institute of Functional Nano & Soft Materials (FUNSOM),Soochow University,Suzhou, Jiangsu 215123, P. R. China

⁴Testing & Analysis Center,Soochow University,Suzhou, Jiangsu 215123, P. R. China

^#J.W., B.H., and Y.J. contributed equally to this work

Adv. Mater. 2020, 32, 1907112

Electrochemical conversion of nitrogen (N₂) into value‐added ammonia (NH₃) is highly desirable yet formidably challenging due to the extreme inertness of the N₂ molecule, which makes the development of a robust electrocatalyst prerequisite. Herein, a new class of bullet‐like M‐Te (M = Ru, Rh, Ir) glassy porous nanorods (PNRs) is reported as excellent electrocatalysts for N₂ reduction reaction (NRR). The optimized IrTe₄ PNRs present superior activity with the highest NH₃ yield rate (51.1 µg h⁻¹ mg⁻¹_cat.) and Faraday efficiency (15.3%), as well as long‐term stability of up to 20 consecutive cycles, making them among the most active NRR electrocatalysts reported to date. Both the N₂ temperature‐programmed desorption and valence band X‐ray photoelectron spectroscopy data show that the strong chemical adsorption of N₂ is the key for enhancing the NRR and suppressing the hydrogen evolution reaction of IrTe₄ PNRs. Density functional theory calculations comprehensively identify that the superior adsorption strength of IrTe₄ adsorptions originates from the synergistic collaboration between electron‐rich Ir and the highly electroactive surrounding Te atoms. The optimal adsorption of both N₂ and H₂O in alkaline media guarantees the superior consecutive NRR process. This work opens a new avenue for designing high‐performance NRR electrocatalysts based on glassy materials.

链接：https://onlinelibrary.wiley.com/doi/full/10.1002/adma.201907112