Domino Effect: Gold Electrocatalyzing Lithium Reduction to Accelerate Nitrogen Fixation

Green production of NH3, especially the Li‐mediated electrochemical N2 reduction reaction (NRR) in non‐aqueous solutions, is attracting research interest. Controversies regarding the NRR mechanism greatly impede its optimization and wide applications. To understand the electrocatalytic process, we t...

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Published inAngewandte Chemie International Edition Vol. 60; no. 10; pp. 5257 - 5261
Main Authors Gao, Lin‐Feng, Cao, Yuan, Wang, Cheng, Yu, Xi‐Wen, Li, Wen‐Bo, Zhou, Yong, Wang, Bing, Yao, Ying‐Fang, Wu, Cong‐Ping, Luo, Wen‐Jun, Zou, Zhi‐Gang
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 01.03.2021
EditionInternational ed. in English
Subjects
Ammonia
Aqueous solutions
Catalysts
Chemical reduction
domino effect
Electrocatalysts
Electrochemistry
Electron transfer
Gold
Gold coatings
gold electrocatalysis
in situ XRD
Intermediates
Lithium
lithium ion reduction
Nitrogen fixation
Nitrogenation
non-aqueous nitrogen reduction
Optimization
Reaction kinetics
non-aqueous nitrogen reduction
lithium ion reduction
domino effect
gold electrocatalysis
in situ XRD
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Summary:Green production of NH3, especially the Li‐mediated electrochemical N2 reduction reaction (NRR) in non‐aqueous solutions, is attracting research interest. Controversies regarding the NRR mechanism greatly impede its optimization and wide applications. To understand the electrocatalytic process, we treated Au coated carbon fibrous paper (Au/CP) as the model catalyst. In situ XRD confirmed the transformation of lithium intermediates during NRR. Au greatly improved electron transfer kinetics to catalyze metallic Li formation, and accordingly highly accelerated spontaneous NRR. The Faradaic efficiency of NRR on Au/CP reached 34.0 %, and NH3 yield was as high as 50 μg h−1 cm−2. Our research shows that the key step of Li‐mediated non‐aqueous NRR is electrocatalytic Li reduction and offers a novel electrocatalyst design method for Li reduction. The key step of Li‐mediated non‐aqueous NRR is electrocatalytic Li reduction. Gold greatly improved Li adsorption energy and thus highly accelerated the domino‐like nitrogen reduction reaction (NRR).
Bibliography:These authors contributed equally to this work.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202015496