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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AuCu Nanodendrite for Enhancing Electrocatalytic Nitrate Reduction Applications via Two-stage Microfluidic Fabrication Strategy

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 1230 - 1241

Published: Jan. 7, 2025

The electrocatalytic nitrate reduction reaction (NitrRR) has attracted great attention in clean ammonia production, but it unsatisfactory selectivity and sluggish dynamics, owing to the complex eight-electron transfer process. While dendritic AuCu alloy is anticipated offer competitive performance, significant challenges remain terms of insufficient structural regulation an unelucidated enhancement mechanism because complexity involved its preparation. To address these issues, we have developed a two-stage microfluidic platform that facilitates stable fabrication controllable nano dendrites (NDs). Notably, Cu content resultant NDs reaches impressive 35.34 At%, surpassing traditional liquid-phase limitations. Furthermore, dendrite structure been thoroughly validated, revealing clear structure–activity relationship. By employing precise manipulation, determined optimal composition NDs, achieving remarkable yield 21.93 mg h–1 cm–2 faradic efficiency 93.30%. Additionally, DFT calculations further elucidate performance mechanism, showing Au3Cu1 sites significantly reduce energy barrier (0.28 eV) rate-determining step (RDS: *NO → *HNO), while excessive deposition adverse effect. Our work contributes innovative guidance for design high-performance electrocatalysts.

Language: Английский

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Electro‐Reconstructed Transition Metal Electrodes for Coupled‐Upgrading of Nitrate Pollution and Waste Poly(Ethylene Terephthalate) Plastics

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

Published: Jan. 28, 2025

Abstract Two unrelated forms of pollution, nitrate‐containing wastewater and waste poly(ethylene terephthalate) (PET) plastics, can be converted into high‐value chemicals by electrochemical reduction oxidation reactions. Herein, coupled electrocatalysis is used for the co‐production ammonia (NH 3 ) formic acid (FA) with a cathode formed reconstructing Co on copper foam (R‐Co/CF) as catalyst nitrate reaction (NO RR) an anode NiCo nickel (R‐NiCo/NF) ethylene glycol (EGOR). The Faraday efficiency R‐Co/CF 96.2% that R‐NiCo/NF catalysts 98.2%. By coupling NO RR PET hydrolysate reaction, cell voltage required at current density 50 mA cm −2 202 mV lower than traditional electrolytic system, indicating electrocatalytic upcycling plastics energy‐saving cost‐effective strategy producing value‐added chemicals. Techno‐economic analysis indicates compared RR//OER RR//PET system save 2.8 × 10 kW h −1 in electricity generate ≈6 900 USD revenue per tonne NH .

Language: Английский

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FeIr Alloy Optimizes the Trade‐Off Between Nitrate Reduction and Active Hydrogen Generation for Efficient Electro‐Synthesis of Ammonia in Neutral Media

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

Published: Feb. 10, 2025

Abstract Electrochemically promoted nitrate reduction reaction (NITRR) holds great potential for the “green” synthesis of ammonia (NH 3 ). However, NITRR in neutral media, though close to practical scenario, is often limited by an insufficient supply active hydrogen (*H) due sluggish water cleavage. In this work, it demonstrated that a bimetallic alloy FeIr can optimize trade‐off between and *H formation media. As result, exhibits excellent catalytic performance toward with Faradaic efficiency NH up 97.3% high yield rate 11.67 mg h −1 cm −2 at low working −0.6 V (versus reversible electrode (RHE)), surpassing monometallic catalysts as well majority Fe‐based state‐of‐the‐art. It also found displays remarkable electron rearrangement hetero‐atoms their significant orbital hybridization, which benefits not only but process. Moreover, coupling FeIr‐based methanol oxidation (MOR) results sustainable productions formate combined FE nearly 200% cell‐voltage 2 V. This work thus demonstrates promising strategy designing efficient NITRR.

Language: Английский

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Recent Breakthroughs in Electrocatalytic Reduction of Nitrogen-Oxyanions for Environmentally Benign Ammonia Synthesis

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110683 - 110683

Published: Jan. 1, 2025

Language: Английский

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A Transition‐Metal‐Based Bifunctional Electrocatalyst for Coupling Glucose Upgrade with Nitrate Reduction

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

Published: Feb. 10, 2025

Abstract The integration of glucose oxidation reaction (GOR) and nitrate reduction (NO 3 − RR) in an electrolyzer affords a sustainable approach to produce high value‐added products remove pollutants. Herein, 3D hierarchical architecture consisting defect‐rich copper–cobalt nanosheets immobilized by cobalt phosphide‐modified nickel foam (D‐CuCo/CoP/NF) is rationally designed as bifunctional electrocatalyst for GOR NO RR. resulting self‐standing electrode displayed remarkable activity. Only 1.29 V vs. RHE required yield current density 100 mA cm −2 . Glucose efficiently converted into formate with selectivity value 93.4% Faraday efficiency (FE) 90.3%. as‐prepared D‐CuCo/CoP/NF also capable transforming nitrates valuable ammonia, leading FE 96.9% rate 802.9 µmol h −1 Such performance renders it the best electrocatalysts Mechanistic studies revealed that defects catalyst greatly facilitated adsorption both Cu(OH) 2 Co 3+ ‐O/Co 4+ ‐O species served active sites reaction. A GOR||NO RR hybrid flow cell constructed using electrode, at voltage 1.35 V.

Language: Английский

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Surface reconstruction regulation of catalysts for cathodic catalytic electrosynthesis

Applied Catalysis O Open, Journal Year: 2025, Volume and Issue: unknown, P. 207036 - 207036

Published: March 1, 2025

Language: Английский

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Coupling Layered Spraying with Joule Heating to Achieve Efficient CuZn Alloy Synthesis for Self-Powered Nitrate Reduction to Ammonia

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110843 - 110843

Published: March 1, 2025

Language: Английский

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Highly selective electrocatalytic reduction of nitrate to ammonia over a copper–cobalt bimetallic catalyst

RSC Advances, Journal Year: 2025, Volume and Issue: 15(12), P. 9461 - 9466

Published: Jan. 1, 2025

The electrocatalytic nitrate reduction reaction (NitRR) is a promising alternative to the traditional Haber-Bosch process. However, competitive hydrogen evolution results in poor NH3 selectivity (S NH3). Here, Cu-Co bimetallic catalyst supported on biomass-derived porous carbon (Cu-Co/BPC) designed and synthesized. Interestingly, presents high yield rate of 9114.1 ± 244.8 μg h-1 cm-2 at -1.4 V (vs. RHE) faradaic efficiency (FE) 84.5 1.6% -1.0 RHE). Notably, S Cu-Co/BPC kept above 94.2% under broad range from RHE), indicating NitRR-to-NH3 Cu-Co/BPC. combination situ characterization experimental indicates that electron transfer occurs between Cu Co, many active sites are generated for adsorption activation N[double bond, length as m-dash]O double bonds, hydrogenation reactions occur with adjacent H protons improve NH3.

Language: Английский

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Nanoporous Copper–Palladium-Based Catalyst for Electrocatalytic Nitrate-to-Ammonia Conversion

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: April 23, 2025

Electrochemical nitrate reduction reaction (NO3RR) is a green and environmentally friendly process with great potential for sustainable nitrogen cycle management ecofriendly ammonia production. Development of catalysts high Faradaic efficiency (FE) yield still challenge the large-scale industrial application NO3RR. In this work, self-supported nanoporous bimetallic Cu-Pd-based catalyst (np Cu-Pd@ZrCuAl) prepared by dealloying galvanic replacement. The np Cu-Pd@ZrCuAl exhibits excellent electrocatalytic performance introduction tiny amount Pd effectively enhances H2O dissociation to provide sufficient H atoms NH3 production, while suppressing competitive hydrogen evolution reaction, leading remarkable FE 95% rate 21.46 mg h-1 cm-2. Theoretical calculations show that Cu/Pd heterostructure modifies electronic structure Cu, optimizes adsorption behavior intermediates, reduces energy barrier rate-determining desorption step, fast generation. This work provides valuable strategy design synthesis electrocatalysts NO3RR via construction.

Language: Английский

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