Multivariate Approaches Boosting Lithium-Mediated Ammonia Electrosynthesis in Different Electrolytes
Anna Mangini
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Conceptualization (equal), Data curation (lead), Investigation (lead), Methodology (equal), Writing - original draft (lead)
Search for more papers by this authorJon Bjarke Valbæk Mygind
Department of Physics, Technical University of Denmark, Fysikvej, Kongens Lyngby, 2800 Denmark
Contribution: Conceptualization (lead), Data curation (supporting), Formal analysis (supporting), Investigation (equal), Writing - review & editing (equal)
Search for more papers by this authorCorresponding Author
Sara Garcia Ballesteros
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Data curation (equal), Formal analysis (equal), Funding acquisition (equal), Methodology (equal), Project administration (supporting), Supervision (equal), Validation (equal), Writing - original draft (equal)
Search for more papers by this authorAlessandro Pedico
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Istituto Nazionale di Ricerca Metrologica, Strada delle Cacce, 91, 10135 Torino, Italy
Contribution: Data curation (supporting), Formal analysis (supporting), Methodology (supporting)
Search for more papers by this authorMarco Armandi
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Data curation (supporting), Investigation (supporting), Supervision (supporting), Writing - review & editing (equal)
Search for more papers by this authorIb Chorkendorff
Department of Physics, Technical University of Denmark, Fysikvej, Kongens Lyngby, 2800 Denmark
Contribution: Conceptualization (equal), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Federico Bella
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Conceptualization (lead), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorAnna Mangini
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Conceptualization (equal), Data curation (lead), Investigation (lead), Methodology (equal), Writing - original draft (lead)
Search for more papers by this authorJon Bjarke Valbæk Mygind
Department of Physics, Technical University of Denmark, Fysikvej, Kongens Lyngby, 2800 Denmark
Contribution: Conceptualization (lead), Data curation (supporting), Formal analysis (supporting), Investigation (equal), Writing - review & editing (equal)
Search for more papers by this authorCorresponding Author
Sara Garcia Ballesteros
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Data curation (equal), Formal analysis (equal), Funding acquisition (equal), Methodology (equal), Project administration (supporting), Supervision (equal), Validation (equal), Writing - original draft (equal)
Search for more papers by this authorAlessandro Pedico
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Istituto Nazionale di Ricerca Metrologica, Strada delle Cacce, 91, 10135 Torino, Italy
Contribution: Data curation (supporting), Formal analysis (supporting), Methodology (supporting)
Search for more papers by this authorMarco Armandi
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Data curation (supporting), Investigation (supporting), Supervision (supporting), Writing - review & editing (equal)
Search for more papers by this authorIb Chorkendorff
Department of Physics, Technical University of Denmark, Fysikvej, Kongens Lyngby, 2800 Denmark
Contribution: Conceptualization (equal), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Federico Bella
Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino, 10129 Italy
Contribution: Conceptualization (lead), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - review & editing (lead)
Search for more papers by this authorAbstract
Ammonia electrosynthesis through the lithium-mediated approach has recently reached promising results towards high activity and selectivity in aprotic media, reaching high Faradaic efficiency (FE) values and NH3 production rates. To fasten the comprehension and optimization of the complex lithium-mediated nitrogen reduction system, for the first time a multivariate approach is proposed as a powerful tool to reduce the number of experiments in comparison with the classical one-factor-at-a-time approach. Doehlert design and surface response methodology are employed to optimize the electrolyte composition for a batch autoclaved cell. The method is validated with the common LiBF4 salt, and the correlations between the FE and the amount of lithium salt and ethanol as proton donor are elucidated, also discussing their impact on the solid electrolyte interphase (SEI) layer. Moreover, a new fluorinated salt is proposed (i.e., lithium difluoro(oxalate) borate (LiFOB)), taking inspiration from lithium batteries. This salt is chosen to tailor the SEI layer, with the aim of obtaining a bifunctional interfacial layer, both stable and permeable to N2, the latter being an essential characteristic for batch systems. The SEI layer composition is confirmed strategic and its tailoring with LiFOB boosts FE values.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
Supporting Information
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