Tandem Active Sites in Cu/Mo‐WO₃ Electrocatalysts for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Abstract Electrocatalytic NO 3 − reduction to NH is a promising technique for both ammonia synthesis and nitrate wastewater treatment. However, this conversion involves tandem processes of H 2 O dissociation hydrogenation, leading inferior Faraday efficiency (FE) yield rate. Herein, catalyst by anchoring atomically dispersed Cu species on Mo‐doped WO (Cu 5 /Mo 0.6 ‐WO ) the RR constructed, which achieves superior FE N 98.6% rate 26.25 mg h −1 cat at −0.7 V (vs RHE) in alkaline media, greatly exceeding performance Mo /WO counterparts. Systematic electrochemical measurement results reveal that promoted activation sites, accompanying accelerated water producing active hydrogens are responsible performance. In situ infrared spectroscopy theoretical calculation further demonstrate sites accelerate , dopant activates adjacent resulting decreased energy barrier * stepwise hydrogenation processes, making thermodynamically favorable. This work demonstrates critical role atomic level enhancing electrocatalytic paving feasible avenue developing high‐performance electrocatalysts.

Language: Английский

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Purification and Value-Added Conversion of NO_x under Ambient Conditions with Photo-/Electrocatalysis Technology

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 6, 2025

As primary air pollutants from fossil fuel combustion, the excess emission of nitric oxides (NOx) results in a series atmospheric environmental issues. Although selective catalytic reduction technology has been confirmed to be effective for NOx removal, green purification and value-added conversion under ambient conditions are still facing great challenges, especially nitrogen resource recovery. To address that, photo-/electrocatalysis offers sustainable routes efficient upcycling temperature pressure, which received considerable attention scientific communities. In this review, recent advances critically summarized. The target products reaction mechanisms systems, together with responsible active sites, discussed, respectively. Then, realistic practicability is proposed, including strict performance evaluation criteria application by photo-/electrocatalysis. Finally, current challenges future opportunities proposed terms catalyst design, enhancement, mechanism understanding, practical conditions, product separation techniques.

Language: Английский

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Theoretical Insights into the Selectivity of Single-Atom Fe–N–C Catalysts for Electrochemical NO_x Reduction

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

Single-atom Fe-N-C catalysts have attracted significant attention in the NOx reduction reaction (NOxRR). However, origin of their selectivity NOxRR remains unclear, impeding further advancements application. Herein, we investigate potential-driven competitive mechanism for NH3 and NH2OH production over single-atom pyridinic-FeN4 pyrrolic-FeN4 sites using constant-potential density functional theory calculations. The is linked to switching Fe 3d orbitals as they interact with intermediates. between determined by applied potentials. predominantly generates at higher potentials (-0.6 -1.2 V, vs SHE), while favored lower (0.6 -0.6 V). shows a similar potential-dependent product distribution, crossover potential -1.0 V. selectivity-determining intermediates (SDIs) are *NH2OH *NH2 + *OH. governed interacting SDIs, from dumbbell-shaped 3dz2 four-leaf clover-like 3dxz, 3dyz, 3dx2-y2, which plays crucial role controlling distribution based on These findings offer new insights into NOxRR.

Language: Английский

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Advances in electrocatalytic nitrate reduction to ammonia over Cu-based catalysts

Environmental Research, Journal Year: 2025, Volume and Issue: unknown, P. 121123 - 121123

Published: Feb. 1, 2025

Language: Английский

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Persulfate-Based Advanced Oxidation Reforming of Polyethylene Terephthalate Fiber into Formate via Singlet Oxygen Activation

Advanced Fiber Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

Language: Английский

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2D Catalysts for Electrocatalytic Nitrate Reduction and C–N Coupling Reactions

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract Powering the electrochemical nitrate reduction reaction (NO 3 ⁻RR) by renewable energy is a sustainable way to restore environment and produce nitrogen–hydrogen compounds. However, process requires multiple electron transfers complex paths, making it essential understand mechanisms at molecular level. In this regard, 2D materials attract significant interest due their large surface area, tunable electronic structures, suitability as model catalysts for studying structure–activity relationships. Advances in use of electrocatalytic NO ⁻RR C–N coupling reactions are analyzed elucidated influence various catalyst design strategies on mechanisms. Using advanced situ/operando measurement techniques, conducting rigorous theoretical analyses, scaling up industrial electrolyzers pivotal unlocking practical potential beyond. A map developing next‐generation electrocatalysts devices provided enable efficient nitrogen cycle using electrocatalysis.

Language: Английский

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Palladium Married with MBene Multilayers: Enabling Intensified Hydrogen Spillover for Efficient Nitrite‐to‐Ammonia Electroreduction

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 8, 2025

Abstract Electrochemical nitrite reduction reaction (NO 2 RR) has emerged as a promising alternative approach for ammonia (NH 3 ) production, offering both energy efficiency and environmental sustainability. The rational regulation of active hydrogen (*H) is pivotal NO − ‐to‐NH conversion, yet it remains significant challenge in the context RR. In this study, molybdenum boride (MBene) multilayers are introduced an electronic support to integrate with palladium (Pd) nanoparticles, creating dual catalytic sites that effectively balance adsorption *H *NO , thereby enabling synergistic catalysis Theoretical experimental analyses revealed efficiently generated on Pd subsequently undergoes spillover ‐adsorbed MBene surfaces, facilitating accelerated hydrogenation NH synthesis. Consequently, Pd/MBene catalyst demonstrated exceptional performance, achieving high Faradaic 89%, yield rate 16.9 mg h −1 cat remarkable cycling stability at low applied potential ‐0.3 V versus RHE. Motivated by outstanding RR further utilized cathode construct Zn‐nitrite formaldehyde‐nitrite batteries. These systems functionality simultaneous production electricity generation, highlighting versatile efficient sustainable conversion.

Language: Английский

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Efficient nitrate electroreduction to ammonia over Copper catalysts supported on Electron-Delocalized covalent organic frameworks

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 156343 - 156343

Published: Oct. 1, 2024

Language: Английский

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Efficient electrocatalytic nitric oxide reduction to ammonia using manganese spinel oxides

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(31), P. 19988 - 19994

Published: Jan. 1, 2024

CoMn 2 O 4 /C is constructed for the electrochemical NO reduction reaction toward NH 3 , with a maximum faradaic efficiency of 89.3% at −0.7 V vs. RHE. can promote hydrogenation *NO to *NHO (PDS, 0.13 eV) and inhibit HER.

Language: Английский

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Ethylene electrosynthesis from low-concentrated acetylene via concave-surface enriched reactant and improved mass transfer

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 13, 2024

Abstract Electrocatalytic semihydrogenation of acetylene (C 2 H ) provides a facile and petroleum-independent strategy for ethylene 4 production. However, the reliance on preseparation concentration raw coal-derived C hinders its economic potential. Here, concave surface is predicted to be beneficial enriching optimizing mass transfer kinetics, thus leading high partial pressure around active sites direct conversion . Then, porous carbon-supported Cu nanoparticle (Cu-PCC) electrode designed enrich gas sites. As result, as-prepared enables 91.7% Faradaic efficiency 56.31% single-pass under simulated atmosphere (~15%) at current density 0.42 A cm −2 , greatly outperforming counterpart without supports. The strengthened intermolecular π conjugation caused by increased coverage revealed result in delocalization electrons consequently promoting activation, suppressing hydrogen evolution competition enhancing selectivity.

Language: Английский

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