Unusual electrochemical N2 reduction activity in an earth-abundant iron catalyst via phosphorous modulation

Xiaojuan Zhu; Tongwei Wu; Lei Ji; Qian Liu; Yonglan Luo; Guanwei Cui; Yimo Xiang; Yanning Zhang; Baozhan Zheng; Xuping Sun

doi:10.1039/C9CC08352A

Unusual electrochemical N₂ reduction activity in an earth-abundant iron catalyst via phosphorous modulation†

Xiaojuan Zhu,‡^ab Tongwei Wu,‡^a Lei Ji,^a Qian Liu,

^a Yonglan Luo,

^b Guanwei Cui,^c Yimo Xiang,^d Yanning Zhang,

^a Baozhan Zheng

*^e and Xuping Sun

*^a

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* Corresponding authors

^a Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
E-mail: xpsun@uestc.edu.cn

^b Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China

^c College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, Shandong, China

^d No. 12 Middle School, Chengdu 610041, Sichuan, China

^e College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China
E-mail: zhengbaozhan@scu.edu.cn

Abstract

Fe-enabled high-performance ambient electrochemical N₂ reduction still remains a big challenge. Here, we report the unusual role of phosphorous in modulating the electrochemical N₂ reduction activity of an Fe catalyst. An FeP₂ nanoparticle–reduced graphene oxide hybrid (FeP₂–rGO) attains a large NH₃ yield of 35.26 μg h⁻¹ mg_cat.⁻¹ (7.06 μg h⁻¹ cm⁻²) and a high faradaic efficiency of 21.99% at −0.40 V vs. reversible hydrogen electrode in 0.5 M LiClO₄, outperforming the FeP–rGO hybrid (17.13 μg h⁻¹ mg_cat.⁻¹; 8.57%). Theoretical calculations reveal that FeP₂ possesses decreased catalytic activity for the hydrogen evolution reaction, higher N₂ adsorption energy, and a larger number of active sites than FeP.

Chemical Communications

Unusual electrochemical N₂ reduction activity in an earth-abundant iron catalyst via phosphorous modulation†

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Unusual electrochemical N₂ reduction activity in an earth-abundant iron catalyst via phosphorous modulation

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