Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 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.

Язык: Английский

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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

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Recent Progress of Amorphous Nanomaterials

Chemical Reviews, Год журнала: 2023, Номер 123(13), С. 8859 - 8941

Опубликована: Июнь 26, 2023

Amorphous materials are metastable solids with only short-range order at the atomic scale, which results from local intermolecular chemical bonding. The lack of long-range typical crystals endows amorphous nanomaterials unconventional and intriguing structural features, such as isotropic environments, abundant surface dangling bonds, highly unsaturated coordination, etc. Because these features ensuing modulation in electronic properties, display potential for practical applications different areas. Motivated by elements, here we provide an overview unique general synthetic methods, covered contemporary research nanomaterials. Furthermore, discussed possible theoretical mechanism nanomaterials, examining how properties configurations contribute to their exceptional performance. In particular, benefits well enhanced electrocatalytic, optical, mechanical thereby clarifying structure–function relationships, highlighted. Finally, a perspective on preparation utilization establish mature systems superior hierarchy various is introduced, outlook future challenges opportunities frontiers this rapidly advancing field proposed.

Язык: Английский

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Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys

Advanced Materials, Год журнала: 2024, Номер 36(30)

Опубликована: Июнь 14, 2024

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable efficient urea production. Herein, diatomic alloy catalyst (CuPd 1 Rh –DAA), with mutually isolated Pd atoms alloyed on Cu substrate, is theoretically designed experimentally confirmed to be highly active selective UENC catalyst. Combining theoretical computations operando spectroscopic characterizations reveals the synergistic effect –Cu sites promote via tandem catalysis mechanism, where site triggers early C–N coupling promotes *CO –to–*CO NH steps, while facilitates subsequent protonation step *COOHNH toward formation. Impressively, CuPd –DAA assembled in flow cell presents highest Faradaic efficiency 72.1% yield rate 53.2 mmol h −1 g cat at −0.5 V versus RHE, representing nearly performance among all reported catalysts.

Язык: Английский

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Pd₁Cu Single-Atom Alloys for High-Current-Density and Durable NO-to-NH₃ Electroreduction

Nano Letters, Год журнала: 2024, Номер 24(2), С. 541 - 548

Опубликована: Янв. 8, 2024

Electrochemical reduction of NO to NH3 (NORR) offers a prospective method for efficient electrosynthesis. Herein, we first design single-atom Pd-alloyed Cu (Pd1Cu) as an and robust NORR catalyst at industrial-level current densities (>0.2 A cm–2). Operando spectroscopic characterizations theoretical computations unveil that Pd1 strongly electronically couples its adjacent two atoms (Pd1Cu2) enhance the activation while promoting NO-to-NH3 protonation energetics suppressing competitive hydrogen evolution. Consequently, flow cell assembled with Pd1Cu exhibits unprecedented yield rate 1341.3 μmol h–1 cm–2 NH3–Faradaic efficiency 85.5% density 210.3 mA cm–2, together excellent long-term durability 200 h electrolysis, representing one highest performances on record.

Язык: Английский

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Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie, Год журнала: 2023, Номер 135(13)

Опубликована: Фев. 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.

Язык: Английский

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

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(13), С. 6814 - 6819

Опубликована: Янв. 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.

Язык: Английский

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Strategies and applications of electrocatalytic nitrate reduction towards ammonia

Coordination Chemistry Reviews, Год журнала: 2024, Номер 506, С. 215723 - 215723

Опубликована: Фев. 26, 2024

Язык: Английский

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Direct Eight-Electron N₂O Electroreduction to NH₃ Enabled by an Fe Double-Atom Catalyst

Nano Letters, Год журнала: 2024, Номер 24(28), С. 8502 - 8509

Опубликована: Июль 1, 2024

N2O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of has gained increasing attention to remove N2O, but its product worthless N2. Here, we propose direct eight-electron (8e) pathway electrochemically convert into NH3. As proof concept, using density functional theory calculation, an Fe2 double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe2@NG) was screened out be the most active selective for electroreduction toward NH3 via novel 8e pathway, which benefits from unique bent adsorption configuration. Guided theoretical prediction, Fe2@NG DAC fabricated experimentally, it can achieve high N2O-to-NH3 Faradaic efficiency 77.8% with large yield rate 2.9 mg h–1 cm–2 at −0.6 V vs RHE in neutral electrolyte. Our study offers feasible strategy synthesize pollutant simultaneous removal.

Язык: Английский

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

ACS Catalysis, Год журнала: 2023, Номер 13(14), С. 9550 - 9557

Опубликована: Июль 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.

Язык: Английский

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