Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(13)

Published: Feb. 3, 2023

We demonstrate the great feasibility of MBenes as a new class tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As proof concept, FeB2 is first employed model MBene catalyst NO3 RR, showing maximum NH3 -Faradaic efficiency 96.8 % with corresponding yield 25.5 mg h-1 cm-2 at -0.6 V vs. RHE. Mechanistic studies reveal that exceptional RR activity arises from catalysis mechanism, is, B sites activate NO3- form intermediates, while Fe dissociate H2 O and increase *H supply on promote intermediate hydrogenation enhance -to-NH3 conversion.

Language: Английский

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Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

ACS Nano, Journal Year: 2023, Volume and Issue: 17(2), P. 1081 - 1090

Published: Jan. 11, 2023

The electrochemical nitrate reduction to ammonia reaction (NO3RR) has emerged as an appealing route for achieving both wastewater treatment and production. Herein, sub-nm RuOx clusters anchored on a Pd metallene (RuOx/Pd) are reported highly effective NO3RR catalyst, delivering maximum NH3-Faradaic efficiency of 98.6% with corresponding NH3 yield rate 23.5 mg h–1 cm–2 partial current density 296.3 mA at −0.5 V vs RHE. Operando spectroscopic characterizations combined theoretical computations unveil the synergy enhance energetics through mechanism hydrogen spillover hydrogen-bond interactions. In detail, activates NO3– form intermediates, while dissociates H2O generate *H, which spontaneously migrates RuOx/Pd interface via process. Further interactions between spillovered *H intermediates makes desorb from participate in intermediate hydrogenation, contributing enhanced activity NO3–-to-NH3 conversion.

Language: Английский

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Lewis Acid Fe‐V Pairs Promote Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(13)

Published: Jan. 18, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) has been recognized as an appealing approach realize both sustainable NH production and waste removal. Herein, from the perspective Lewis acid‐base interaction, a single‐atom Fe‐doped V 2 O 5 (Fe‐V ) catalyst enriched is designed with acid sites, which present maximum ‐Faradaic efficiency 97.1% corresponding yield 12.5 mg h −1 cm −2 at –0.7 versus RHE. Mechanistic studies based on theoretical calculations operando spectroscopic characterizations identify creation Fe‐V pairs , can synergetically activate NO − promote hydrogenation energetics, restrain hydrogen evolution, leading enhanced RR activity selectivity.

Language: Английский

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Iridium single-atom catalyst for highly efficient NO electroreduction to NH3

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 8737 - 8742

Published: March 8, 2023

Language: Английский

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p-Block Antimony Single-Atom Catalysts for Nitric Oxide Electroreduction to Ammonia

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(3), P. 1281 - 1288

Published: Feb. 3, 2023

Electrocatalytic NO reduction to NH3 (NORR) offers a prospective approach attain both harmful removal and efficient electrosynthesis. Main-group p-block metals are promising NORR candidates but still lack adequate exploration. Herein, Sb single atoms confined in amorphous MoO3 (Sb1/a-MoO3) designed as an catalyst, exhibiting the highest yield rate of 273.5 μmol h–1 cm–2 NO-to-NH3 Faradaic efficiency 91.7% at −0.6 V vs RHE. In situ spectroscopic characterizations theoretical computations reason that outstanding performance Sb1/a-MoO3 arises from isolated Sb1 sites, which can optimize adsorption *NO/*NHO lower reaction energy barriers simultaneously exhibit higher affinity than H2O/H species. Moreover, our strategy be extended prepare Bi1/a-MoO3, showing high property, demonstrating immense potential metal single-atom catalysts toward high-performing electrocatalysis.

Language: Английский

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Self-Tandem Electrocatalytic NO Reduction to NH₃ on a W Single-Atom Catalyst

Nano Letters, Journal Year: 2023, Volume and Issue: 23(5), P. 1735 - 1742

Published: Feb. 14, 2023

We design single-atom W confined in MoO3-x amorphous nanosheets (W1/MoO3-x) comprising W1-O5 motifs as a highly active and durable NORR catalyst. Theoretical operando spectroscopic investigations reveal the dual functions of to (1) facilitate activation protonation NO molecules (2) promote H2O dissociation while suppressing *H dimerization increase proton supply, eventually resulting self-tandem mechanism W1/MoO3-x greatly accelerate energetics NO-to-NH3 pathway. As result, exhibits highest NH3-Faradaic efficiency 91.2% NH3 yield rate 308.6 μmol h-1 cm-2, surpassing that most previously reported catalysts.

Language: Английский

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Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie, Journal Year: 2023, Volume and Issue: 135(13)

Published: Feb. 3, 2023

Abstract We demonstrate the great feasibility of MBenes as a new class tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO 3 RR). As proof concept, FeB 2 is first employed model MBene catalyst NO RR, showing maximum NH ‐Faradaic efficiency 96.8 % with corresponding yield 25.5 mg h −1 cm −2 at −0.6 V vs. RHE. Mechanistic studies reveal that exceptional RR activity arises from catalysis mechanism, is, B sites activate − form intermediates, while Fe dissociate H O and increase *H supply on promote intermediate hydrogenation enhance ‐to‐NH conversion.

Language: Английский

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Main-group indium single-atom catalysts for electrocatalytic NO reduction to NH₃

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(13), P. 6814 - 6819

Published: Jan. 1, 2023

In single atoms confined in amorphous MoO 3 (In 1 /a-MoO ) are reported to be an efficient catalyst for NO electroreduction NH , attributed the ability of single-site inhibit hydrogen evolution and optimize NO-to-NH hydrogenation energetics.

Language: Английский

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Ce-doped MoS_2−xnanoflower arrays for electrocatalytic nitrate reduction to ammonia

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(5), P. 1543 - 1551

Published: Jan. 1, 2023

Ce-doped and MoS 2−x nanoflower arrays exhibit a high activity for electrocatalytic nitrate-to-ammonia conversion (NO 3 RR), attributed to the synergy of S-vacancy Ce-dopant enhance NO − activation reduce reaction energy barriers.

Language: Английский

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Atomically Dispersed W₁–O₃ Bonded on Pd Metallene for Cascade NO Electroreduction to NH₃

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(14), P. 9550 - 9557

Published: July 5, 2023

Electrocatalytic NO reduction to NH3 (NORR) offers a prospective method for removing hazardous and producing valuable simultaneously. Herein, we demonstrate that atomically dispersed W on Pd metallene (W1Pd) can be an efficient robust NORR catalyst. Atomic coordination characterizations unravel single atoms exist as W1–O3 moieties bonded metallene. In situ spectroscopic measurements theoretical calculations reveal the synergistic cascade effect of promote energetics W1Pd, in which activation hydrogenation occur W1–O3, while dissociates H2O donates protons required NH3. Consequently, W1Pd exhibits yield rate 758.5 μmol h–1 cm–2 with NH3-Faradaic efficiency 91.3% flow cell (272.1 93.7% H-type cells), ranking almost highest performance among all reported catalysts.

Language: Английский

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