Phenol as proton shuttle and buffer for lithium-mediated ammonia electrosynthesis

Xianbiao Fu, Aoni Xu, Jakob B. Pedersen, Shaofeng Li, Rokas Sažinas, Yuanyuan Zhou, Suzanne Z. Andersen, Mattia Saccoccio, Niklas H. Deissler, Jon Bjarke Valbæk Mygind, Jakob Kibsgaard, Peter C. K. Vesborg, Jens K. Nørskov () and Ib Chorkendorff ()
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Xianbiao Fu: Technical University of Denmark
Aoni Xu: Technical University of Denmark
Jakob B. Pedersen: Technical University of Denmark
Shaofeng Li: Technical University of Denmark
Rokas Sažinas: Technical University of Denmark
Yuanyuan Zhou: Technical University of Denmark
Suzanne Z. Andersen: Technical University of Denmark
Mattia Saccoccio: Technical University of Denmark
Niklas H. Deissler: Technical University of Denmark
Jon Bjarke Valbæk Mygind: Technical University of Denmark
Jakob Kibsgaard: Technical University of Denmark
Peter C. K. Vesborg: Technical University of Denmark
Jens K. Nørskov: Technical University of Denmark
Ib Chorkendorff: Technical University of Denmark

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Ammonia is a crucial component in the production of fertilizers and various nitrogen-based compounds. Now, the lithium-mediated nitrogen reduction reaction (Li-NRR) has emerged as a promising approach for ammonia synthesis at ambient conditions. The proton shuttle plays a critical role in the proton transfer process during Li-NRR. However, the structure-activity relationship and design principles for effective proton shuttles have not yet been established in practical Li-NRR systems. Here, we propose a general procedure for verifying a true proton shuttle and established design principles for effective proton shuttles. We systematically evaluate several classes of proton shuttles in a continuous-flow reactor with hydrogen oxidation at the anode. Among the tested proton shuttles, phenol exhibits the highest Faradaic efficiency of 72 ± 3% towards ammonia, surpassing that of ethanol, which has been commonly used so far. Experimental investigations including operando isotope-labelled mass spectrometry proved the proton-shuttling capability of phenol. Further mass transport modeling sheds light on the mechanism.

Date: 2024
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DOI: 10.1038/s41467-024-46803-w

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