Modulation of surface properties on cobalt phosphide for high-performance ambient ammonia electrosynthesis

Hou, Yunpeng ¹Yang, Fangqi ²Cao, Chenliang ²Zou, Zhi ²Luo, Junhui ²Zhou, Weizhen ²Tong, Zhikun ²Chen, Shixia ²Zhou, Shaodong ¹Wang, Jun ²Deng, Shuguang ³Meng, Qiangguo²

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作者信息

1. Zhejiang Univ
2. Nanchang Univ
3. Arizona State Univ
折叠

Abstract

Tuning surface properties of electrocatalysts for sustainable electrocatalytic nitrogen reduction reaction (NRR) with high selectivity and activity is highly demanded but still lacks fundamental understanding and modulation methods. Herein, we report the transformation of hydrogen evolution reaction (HER)-favorable cobalt phosphide (CoP) to NRR-favorable electrocatalyst via modulation of surface properties. The oxidized CoP particles encapsulated in carbon nanotubes (O-CoP/CNT) exhibits a high NH3 yield of 39.58 mu g h(-1) mg(-1 cat) as well as high Faradaic efficiency (FE) of 19.4% at -0.5 V vs. reversible hydrogen electrode (RHE), which is confirmed by N-15(2) isotope-labeling tests. In-situ Raman spectra identify that N-2 molecules are preferentially captured by Co ions, while the surface-adsorbed H+ are gradually eliminated. The hydrophobic surface of CNT can limit the contact of protons with the catalyst surface to inhibit HER, and the formation of hydrogen bond facilitates a more efficient NRR process. The surface modulation effects are confirmed by density functional theory calculations.

Key words

N-2 fixation/in-situ Raman/Surface modulation/Cobalt phosphide/DFT calculation/HYDROGEN EVOLUTION/BIFUNCTIONAL ELECTROCATALYST/NITROGEN/EFFICIENT/CARBON/REDUCTION/WATER/CO2/NANOSHEETS/VACANCIES

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出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量25

参考文献量60

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