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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Single‐Atom Bi Alloyed Pd Metallene for Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(12)

Published: Jan. 15, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as highly effective NO RR catalyst, showing near 100% ‐Faradaic efficiency with the corresponding yield 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those almost all ever catalysts. In‐depth theoretical operando spectroscopic investigations unveil that electronically couples its neighboring atoms synergistically activate − destabilize *NO on Pd, leading reduced energy barrier potential‐determining step (*NO→*NOH) enhanced protonation energetics ‐to‐NH pathway.

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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Recent advances in electrocatalytic ammonia synthesis

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 50, P. 6 - 44

Published: July 1, 2023

Language: Английский

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Recent advances on electrocatalytic CO2 reduction to resources: Target products, reaction pathways and typical catalysts

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 453, P. 139663 - 139663

Published: Oct. 8, 2022

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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Metal-coordinated porous polydopamine nanospheres derived Fe ₃N-FeCo encapsulated N-doped carbon as a highly efficient electrocatalyst for oxygen reduction reaction

Deleted Journal, Journal Year: 2022, Volume and Issue: 1, P. e9120027 - e9120027

Published: Aug. 19, 2022

The exploration of high-efficiency, long-durability, and cost-effectiveness transition metal doped carbon materials to replace the commercial Pt/C in oxygen reduction reaction (ORR) is greatly desirable for promoting advancement sustainable energy devices.Herein, Fe 3 N FeCo alloy decorated N-doped hybrid material (denoted N-FeCo@NC) prepared applied as ORR catalyst, which derived from two-step pyrolysis an intriguing complex consisted metal-coordinated porous polydopamine (PDA) nanospheres (i.e., Fe-PDA@Co) melamine.The resulting N-FeCo@NC delivers outstanding activity with onset potential (E on ) 1.05 V, a half-wave 1/2 0.89 well excellent long-term stability methanol resistance over Pt/C.Interestingly, home-made Zn-air battery air-cathode demonstrates much higher open-circuit voltage (1.50 vs. 1.48 V), power density (141 113 mW•cm -2) specific capacity (806.6 660.6mAh•g -1Zn than those counterpart.Such remarkable may stem synergistic effect active species, large surface area, hierarchical structure exceptional sphere/sheet hybridized architecture.

Language: Английский

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Advances in the Electrocatalytic Hydrogen Evolution Reaction by Metal Nanoclusters‐based Materials

Small, Journal Year: 2022, Volume and Issue: 18(52)

Published: Oct. 26, 2022

Abstract With the development of renewable energy systems, clean hydrogen is burgeoning as an optimal alternative to fossil fuels, in which its application promising retarding global and environmental crisis. The evolution reaction (HER), capable producing high‐purity rapidly electrocatalytic water splitting, has received much attention. Abundant research about HER been done, focusing on advanced electrocatalyst design with high efficiency robust stability. As potential catalysts, metal nanoclusters (MNCs) have studied extensively. They are composed several a hundred atoms, sizes being comparable Fermi wavelength electrons, that is, < 2.0 nm. Different from atoms/nanoparticles, they exhibit unique catalytic properties due their quantum size effect low‐coordination environment. In this review, activity‐enhancing approaches MNCs applied electrocatalysis mainly summarized. Furthermore, recent progress classified different stabilization strategies, freestanding MNCs, organic, carbon supports, introduced. Finally, current challenges deficiencies these for prospected.

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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