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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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. 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.
AbstractList	We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO RR). As a proof of concept, FeB is first employed as a model MBene catalyst for the NO RR, showing a maximum NH -Faradaic efficiency of 96.8 % with a corresponding NH yield of 25.5 mg h cm at -0.6 V vs. RHE. Mechanistic studies reveal that the exceptional NO RR activity of FeB arises from the tandem catalysis mechanism, that is, B sites activate NO to form intermediates, while Fe sites dissociate H O and increase H supply on B sites to promote the intermediate hydrogenation and enhance the NO -to-NH conversion. 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. 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. We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As a proof of concept, FeB2 is first employed as a model MBene catalyst for the NO3 RR, 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 NO3 RR activity of FeB2 arises from the tandem catalysis mechanism, that is, B sites activate NO3 - to form intermediates, while Fe sites dissociate H2 O and increase H supply on B sites to promote the intermediate hydrogenation and enhance the NO3 - -to-NH3 conversion.We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As a proof of concept, FeB2 is first employed as a model MBene catalyst for the NO3 RR, 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 NO3 RR activity of FeB2 arises from the tandem catalysis mechanism, that is, B sites activate NO3 - to form intermediates, while Fe sites dissociate H2 O and increase H supply on B sites to promote the intermediate hydrogenation and enhance the NO3 - -to-NH3 conversion. We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO 3 RR). As a proof of concept, FeB 2 is first employed as a model MBene catalyst for the NO 3 RR, showing a maximum NH 3 ‐Faradaic efficiency of 96.8 % with a corresponding NH 3 yield of 25.5 mg h −1 cm −2 at −0.6 V vs. RHE. Mechanistic studies reveal that the exceptional NO 3 RR activity of FeB 2 arises from the tandem catalysis mechanism, that is, B sites activate NO 3 − to form intermediates, while Fe sites dissociate H 2 O and increase H supply on B sites to promote the intermediate hydrogenation and enhance the NO 3 − ‐to‐NH 3 conversion.
Author	Guo, Yali Chu, Ke Zhang, Guike Chen, Kai Ma, Dongwei Li, Xiaotian
Author_xml	– sequence: 1 givenname: Guike surname: Zhang fullname: Zhang, Guike organization: Lanzhou Jiaotong University – sequence: 2 givenname: Xiaotian surname: Li fullname: Li, Xiaotian organization: Lanzhou Jiaotong University – sequence: 3 givenname: Kai surname: Chen fullname: Chen, Kai organization: Lanzhou Jiaotong University – sequence: 4 givenname: Yali surname: Guo fullname: Guo, Yali organization: Lanzhou Jiaotong University – sequence: 5 givenname: Dongwei surname: Ma fullname: Ma, Dongwei email: madw@henu.edu.cn organization: Henan University – sequence: 6 givenname: Ke orcidid: 0000-0002-0606-2689 surname: Chu fullname: Chu, Ke email: chuk630@mail.lzjtu.cn organization: Lanzhou Jiaotong University
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/36734975$$D View this record in MEDLINE/PubMed
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Keywords	Electrocatalytic Nitrate Reduction to Ammonia MBenes Tandem Catalysts Operando Electrochemical Characterizations Theoretical Computations
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Snippet	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... We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO 3 RR). As a proof of... We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO RR). As a proof of... We demonstrate the great feasibility of MBenes as a new class of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As a proof of...
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SubjectTerms	Ammonia Catalysis Catalysts Electrocatalytic Nitrate Reduction to Ammonia Intermediates MBenes Nitrate reduction Operando Electrochemical Characterizations Reduction Tandem Catalysts Theoretical Computations
Title	Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes
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