Intermetallic compounds for nitrogen electrochemistry

Green Energy & Environment, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

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Lattice Oxygen-Driven Co-Adsorption of Carbon Dioxide and Nitrate on Copper: A Pathway to Efficient Urea Electrosynthesis

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 10, 2025

The electrochemical coupling of CO2 and NO3– on copper-based catalysts presents a sustainable strategy for urea production while simultaneously addressing wastewater denitrification. However, the inefficient random adsorption copper surface limits interaction key carbon nitrogen intermediates, thereby impeding efficient C–N coupling. In this study, we demonstrate that residual lattice oxygen in oxide-derived nanosheets (OL-Cu) can effectively tune electron distribution, thus activating neighboring atoms generating electron-deficient (Cuδ+) sites. These Cuδ+ sites enhance stabilize *CO which enables directional at adjacent This mechanism shortens pathway achieves yield up to 298.67 mmol h–1 g–1 −0.7 V versus RHE, with an average Faradaic efficiency 31.71% high current density ∼95 mA cm–2. situ spectroscopic measurements confirmed formation tracked evolution intermediates (i.e., *CO, *NO, *OCNO, *NOCONO) during synthesis. Density functional theory calculations revealed promote coadsorption *NO3, as well *OCNO significantly improving kinetics. study underscores critical role facilitating selectivity.

Язык: 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, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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.

Язык: Английский

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Incorporating Ordered Indium Sites into Rhodium for Ultra‐Low Potential Electrocatalytic Conversion of Ethylene Glycol to Glycolic Acid

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 3, 2025

Abstract The upcycling of polyethylene terephthalate (PET)‐derived ethylene glycol (EG) to glycolic acid (GA, a biodegradable polymer monomer) via electrocatalysis not only produces valuable chemicals but also mitigates plastic pollution. However, the current reports for electrooxidation EG‐to‐GA usually operate at reaction potentials >1.0 V vs reversible hydrogen electrode (RHE), much higher than theoretical potential (0.065 RHE), resulting in substantial energy wastage. Herein, body‐centered cubic RhIn intermetallic compounds (IMCs) anchored on carbon support (denoted as RhIn/C) are synthesized, which shows excellent performance with an onset 0.35 RHE, lower values reported literature. catalyst possesses satisfactory GA selectivity (85% 0.65 RHE). Experimental results combined density functional theory calculations demonstrate that IMCs enhance adsorption EG and OH − , facilitating generation reactive oxygen species thereby improving catalytic performance. RhIn/C exhibits electrocatalytic evolution reaction, ensuring it can be used bifunctional two‐electrode system coupled production. This work opens new avenues reducing consumption PET‐derived clean

Язык: Английский

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Engineering Nickel Dopants in Atomically Thin Molybdenum Disulfide for Highly Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 16, 2024

Abstract The electrocatalytic nitrate reduction reaction (NO 3 − RR) presents a promising pathway for achieving both ammonia (NH ) electrosynthesis and water pollutant removal simultaneously. Among various electrocatalysts explored, 2D materials have emerged as candidates due to their ability regulate electronic states active sites through doping. However, the impact of doping effects in on mechanism NO RR remains relatively unexplored. Here, Ni‐doped MoS 2 (Ni‐MoS nanosheets are investigated model system, demonstrating enhanced performance compared undoped counterparts. By controlling concentration, Ni‐MoS achieve remarkable faradic efficiency (FE) 92.3% NH at −0.3 V RHE with excellent stability. mechanistic studies reveal that elevation performances originates from generation more hydrogen acceleration nitrite facilitated by Ni Combining experimental observations theoretical calculations it is revealed appropriate level can enhance *NO adsorption strength, thereby facilitating subsequent steps. Together demonstration Zn−NO battery devices, work provides new insights into design regulation material catalysts efficient RR.

Язык: Английский

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Suppression of Structural Heterogeneity in High‐Entropy Intermetallics for Electrocatalytic Upgrading of Waste Plastics

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 29, 2024

Abstract The key to fully realizing the potential of high‐entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with long‐range ordering required for electrochemical applications. Herein, we synthesized a distinctive L1 0 ‐(PtIr)(FeMoBi) intermetallics (HEIs) exhibiting nanoscale order and atomic scale short‐range disorder via lattice compensation strategy mitigate entropy reduction tendency. (PtIr)(FeMoBi) catalyst exhibited remarkable activity selectivity glycollic acid (GA) production electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR). With mass 5.2 A mg Pt −1 Faradaic efficiency (FE) GA 95 %, it outperformed most previously reported electrocatalysts selective production. lattice‐compensation effect promotes homogeneity Fe actives sites, facilitating co‐adsorption EG OH reducing energy barriers dehydrogenation OH‐combination processes. This approach effectively avoids formation low‐active sites commonly encountered HEA solid solutions, offering promising avenue exploring complex interplay between catalytic HEI structures.

Язык: Английский

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Alloying effect-triggered electron polarization in PdCu metallene for simultaneous electrocatalytic upcycling of nitrate and polyethylene terephthalate to value-added chemicals

Chemical Engineering Journal, Год журнала: 2024, Номер 498, С. 155557 - 155557

Опубликована: Сен. 7, 2024

Язык: Английский

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Boosting Active Hydrogen Generation via Ruthenium Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер unknown, С. 124943 - 124943

Опубликована: Дек. 1, 2024

Язык: Английский

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Transition Metal‐Gallium Intermetallic Compounds with Tailored Active Site Configurations for Electrochemical Ammonia Synthesis

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(49)

Опубликована: Сен. 4, 2024

Abstract Gallium (Ga) with a low melting point can serve as unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy transition metal‐Ga IMCs endows them high catalytic stability. Meanwhile, their tunable crystal structures offer possibility to tailor configurations active sites meet requirements for specific applications. Herein, we present general method preparing range IMCs, including Co−Ga, Ni−Ga, Pt−Ga, Pd−Ga, and Rh−Ga IMCs. structurally ordered CoGa body‐centered cubic ( bcc ) structure are uniformly dispersed on nitrogen‐doped reduced graphene oxide substrate (O‐CoGa/NG) deliver outstanding nitrate reduction reaction (NO 3 RR) performance, making excellent catalysts construct highly efficient rechargeable Zn‐NO − battery. Operando studies theoretical simulations demonstrate that electron‐rich environments around Co atoms enhance adsorption strength *NO intermediate simultaneously suppress hydrogen, thus improving NO RR activity selectivity.

Язык: Английский

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Advances in Electrocatalytic Nitrate Reduction: Insights into Mechanisms and Reaction Optimization

Advanced Sustainable Systems, Год журнала: 2025, Номер unknown

Опубликована: Янв. 20, 2025

Abstract Electrocatalytic nitrate reduction (NO 3 RR) offers a promising approach to address pollution by converting harmful nitrates into environment‐benign or valuable products like nitrogen gas (N 2 ) ammonia (NH ). This review explores the mechanisms, challenges, and catalysts involved in NO RR, highlighting role of catalyst selectivity, stability, external reaction conditions. The discussion also covers environmental economic benefits RR for water treatment, alongside potential future directions scaling‐up, system integration, expanding research tackling related nitrogen‐based pollutants as well real world applications.

Язык: Английский

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