Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3RR). As a proof of concept, FeB2 is first employed as a model MBene catalyst for the NO3RR, showing a maximum NH3‐Faradaic efficiency of 96.8 % with a corresponding...

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Vydáno v:Angewandte Chemie International Edition Ročník 62; číslo 13; s. e202300054 - n/a
Hlavní autoři: Zhang, Guike, Li, Xiaotian, Chen, Kai, Guo, Yali, Ma, Dongwei, Chu, Ke
Médium: Journal Article
Jazyk:angličtina
Vydáno: Germany Wiley Subscription Services, Inc 20.03.2023
Vydání:International ed. in English
Témata:
Ammonia
Catalysis
Catalysts
Electrocatalytic Nitrate Reduction to Ammonia
Intermediates
MBenes
Nitrate reduction
Operando Electrochemical Characterizations
Reduction
Tandem Catalysts
Theoretical Computations
Electrocatalytic Nitrate Reduction to Ammonia
MBenes
Tandem Catalysts
Operando Electrochemical Characterizations
Theoretical Computations
ISSN:1433-7851, 1521-3773, 1521-3773
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Popis
Shrnutí:We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3RR). As a proof of concept, FeB2 is first employed as a model MBene catalyst for the NO3RR, showing a maximum NH3‐Faradaic efficiency of 96.8 % with a corresponding NH3 yield of 25.5 mg h−1 cm−2 at −0.6 V vs. RHE. Mechanistic studies reveal that the exceptional NO3RR activity of FeB2 arises from the tandem catalysis mechanism, that is, B sites activate NO3− to form intermediates, while Fe sites dissociate H2O and increase *H supply on B sites to promote the intermediate hydrogenation and enhance the NO3−‐to‐NH3 conversion. MBenes are demonstrated to be a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3RR). Taking FeB2 as the proof‐of‐concept paradigm, mechanistic studies unveil that the synergistic tandem effect of Fe and B atoms promotes NO3− activation and intermediate hydrogenation to enhance the NO3RR activity and selectivity.
Bibliografie:These authors contributed equally to this work.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202300054