Accelerating Protonation Kinetics for Ammonia Electrosynthesis on Single Iron Sites Embedded in Carbon with Intrinsic Defects

Yan Kong; Lei Wu; Xiaoxuan YangYan LiSixing ZhengBin YangZhongjian LiQinghua ZhangShaodong ZhouLecheng LeiGang WuYang Hou

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Accelerating Protonation Kinetics for Ammonia Electrosynthesis on Single Iron Sites Embedded in Carbon with Intrinsic Defects

机译：Accelerating Protonation Kinetics for Ammonia Electrosynthesis on Single Iron Sites Embedded in Carbon with Intrinsic Defects

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Electrocatalysts play a vital role in electroreduction of N_2 to NH_3 (NRR); however, large-scale industrial application of electrochemical NRR is still limited by low selectivity and poor activity, owing to the sluggish reaction kinetics. Herein, a high-performance NRR catalyst consisting of atomically dispersed iron single site embedded in porous nitrogen-doped carbon nanofibers with abundant carbon defects (D-FeN/C) is reported. The D-FeN/C catalyst achieves a remarkably high NH_3 yield rate of ≈24.8 μg h~(?1) mg_(cat)~(?1) and Faradaic efficiency of 15.8% at ?0.4 V in alkaline electrolyte, which outperforms almost all reported Fe-based NRR catalysts. Structural characterization manifests that the isolated Fe center is coordinated with four N atoms and assisted by extra carbon defects. In situ attenuated total reflectance-Fourier transform infrared results and kinetics isotope effects demonstrate that the intrinsic carbon defects dramatically enhance the water dissociation process and accelerate the protonation kinetics of D-FeN/C for NRR. Theoretical investigations unveil atomic Fe-N_4 catalytic sites together with intrinsic carbon defects synergistically reduce the energy barrier of the protonation process and promote the proton-coupled reaction kinetics, thus boosting the whole NRR catalytic performance.

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来源
《Advanced functional materials》 |2022年第44期|2205409.1-2205409.9|共9页
作者
Yan Kong; Lei Wu; Xiaoxuan YangYan LiSixing ZhengBin YangZhongjian LiQinghua ZhangShaodong ZhouLecheng LeiGang WuYang Hou;
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Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027, China,Institute of Zhejiang University-Quzhou Quzhou 324000, China;

Department of Chemical and iological Engineering University at Buffalo The State University of New York Buffalo, NY 14260, USA;

Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027, China,Institute of Zhejiang University-Quzhou Quzhou 324000, China,School of Biological and ChemicaKey Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027, China;

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Fe-N4 active sites; intrinsic carbon defects; N2 reduction reactions; protonation kinetics; water dissociation;

Accelerating Protonation Kinetics for Ammonia Electrosynthesis on Single Iron Sites Embedded in Carbon with Intrinsic Defects

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