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Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes
Authors:Guike Zhang  Xiaotian Li  Kai Chen  Yali Guo  Prof Dongwei Ma  Prof Ke Chu
Institution:1. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070 China

These authors contributed equally to this work.

Contribution: ​Investigation (lead);2. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070 China

These authors contributed equally to this work.

Contribution: ​Investigation (equal);3. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070 China

Contribution: ​Investigation (supporting);4. Key Laboratory for Special Functional Materials of Ministry of Education, School of Materials Science and Engineering, Henan University, Kaifeng, 475004 China;5. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070 China

Abstract: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.
Keywords:Electrocatalytic Nitrate Reduction to Ammonia  MBenes  Operando Electrochemical Characterizations  Tandem Catalysts  Theoretical Computations
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