Shear‐Strained Pd Single‐Atom Electrocatalysts for Nitrate Reduction to Ammonia

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

Опубликована: Июль 16, 2024

Electrochemical nitrate reduction method (NitRR) is a low-carbon, environmentally friendly, and efficient for synthesizing ammonia, which has received widespread attention in recent years. Copper-based catalysts have leading edge due to their good adsorption of *NO

Язык: Английский

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Copper Atom Pairs Stabilize *OCCO Dipole Toward Highly Selective CO2 Electroreduction to C2H4

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(50)

Опубликована: Авг. 13, 2024

Abstract Deeply electrolytic reduction of carbon dioxide (CO 2 ) to high‐value ethylene (C H 4 is very attractive. However, the sluggish kinetics C−C coupling seriously results in low selectivity CO electroreduction C . Herein, we report a copper‐based polyhedron (Cu2) that features uniformly distributed and atomically precise bi‐Cu units, which can stabilize *OCCO dipole facilitate for high selective production. The faradaic efficiency (FE) reaches 51 % with current density 469.4 mA cm −2 , much superior Cu single site catalyst (Cu SAC) (~0 %). Moreover, Cu2 has higher turnover frequency (TOF, ~520 h −1 compared nanoparticles (~9.42 SAC (~0.87 ). In situ characterizations theoretical calculations revealed unique structural configuration could optimize moments adsorbate promote generation

Язык: Английский

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Phosphorus-doped Ti₃C₂T_x MXene nanosheets enabling ambient NH₃ synthesis with high current densities

Chemical Communications, Год журнала: 2024, Номер 60(66), С. 8728 - 8731

Опубликована: Янв. 1, 2024

Herein, we show that P-doped Ti

Язык: Английский

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Efficient Electrochemical Nitrate Reduction to Ammonia Driven by a Few Nanometer-Confined Built-In Electric Field

ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10437 - 10446

Опубликована: Июнь 26, 2024

Converting nitrate (NO3–) to ammonia (NH3) through the electrochemical reduction method offers an appealing approach for wastewater treatment and facilitates nitrogen cycling in nature. However, this electrolytic involves a series of proton-coupled electron transfer processes comes with severe competing reactions. Consequently, there is significant demand catalysts exhibiting good catalytic activities selectivities. Here, copper–cobalt binary sulfide nanosheets varying Cu/Co compositions were prepared investigate synergy effects between components copper cobalt on their performance. As result, volcano-like correlation ratio electrocatalytic performance was built. The optimal catalyst CuxS–Co0.5 exhibited maximum Faradaic efficiency (FE) ∼95.6% at −1.4 V vs Ag/AgCl. highest yield rate 5.36 mg/h·cm2 achieved −1.6 Ag/AgCl, which 6.5- 3.8-fold relative those pure CuxS CoS2, respectively. By combining spectroscopy characterizations theoretical calculations, we revealed that built-in electric field confined few nanometers played critical role enhancing creating more active sites. Besides, its improved water dissociation capability essential hydrogenation intermediates, collectively contributing enhanced

Язык: Английский

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Precise synthesis of dual atom sites for electrocatalysis

Nano Research, Год журнала: 2024, Номер unknown

Опубликована: Сен. 17, 2024

Язык: Английский

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Lignin-based support for metal catalysts: Synthetic strategies, performance boost, and application advances

Coordination Chemistry Reviews, Год журнала: 2025, Номер 528, С. 216426 - 216426

Опубликована: Янв. 10, 2025

Язык: Английский

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Destabilization of Single‐Atom Catalysts: Characterization, Mechanisms, and Regeneration Strategies

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Numerous in situ characterization studies have focused on revealing the catalytic mechanisms of single‐atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, stability SACs under long‐term operating conditions equally important and prerequisite real‐world energy applications, such as fuel cells water electrolyzers. Recently, there has been rise destabilization regeneration SACs; however, timely comprehensive summaries that provide catalysis community with valuable insights directions are still lacking. This review summarizes recent advances strategies SACs, specifically highlighting various state‐of‐the‐art techniques employed studies. The factors induce identified by discussing failure active sites, coordination environments, supports, reaction scenarios. Next, primary introduced, including redispersion, surface poison desorption, exposure subsurface sites. Additionally, advantages limitations both ex discussed. Finally, future proposed, aimed at constructing structure–stability relationships guiding design more stable SACs.

Язык: Английский

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Understanding the Dynamic Evolution of Active Sites among Single Atoms, Clusters, and Nanoparticles

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Abstract Catalysis remains a cornerstone of chemical research, with the active sites catalysts being crucial for their functionality. Identifying sites, particularly during reaction process, is elucidating relationship between catalyst's structure and its catalytic property. However, dynamic evolution within heterogeneous metal presents substantial challenge accurately pinpointing real sites. The advent in situ operando characterization techniques has illuminated path toward understanding changes offering robust scientific evidence to support rational design catalysts. There pressing need comprehensive review that systematically explores among single atoms, clusters, nanoparticles as utilizing techniques. This aims delineate effects various factors on nanoparticles. Moreover, several are elaborated emphases tracking linking them properties. Finally, it discusses challenges future perspectives identifying process advancing

Язык: Английский

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Atomically Dispersed Co–P Moieties via Direct Thermal Exfoliation for Alkaline Hydrogen Electrosynthesis

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

Опубликована: Янв. 25, 2025

The development of highly active and stable cathodes in alkaline solutions is crucial for promoting the commercialization anion exchange membrane (AEM) electrolyzers, yet it remains a significant challenge. Herein, we synthesized atomically dispersed CoP4 moieties (CoP4–SSC) immobilized on ultrathin carbon nanosheets via phosphidation exfoliation strategy at medium temperature. thermodynamic formation process Co–P was elucidated using X-ray absorption spectroscopy (XAS) theoretical calculations. Remarkably, resulting CoP4–SSC electrocatalyst exhibited outstanding activity hydrogen evolution, with low overpotential 52 mV 10 mA cm–2 turnover frequency up to 23.83 s–1. Moreover, AEM electrolyzer fabricated achieved current density 1 A under an applied voltage only 1.94 V, showing negligible degradation after 500 h continuous electrocatalysis. series operando characterizations functional theory calculations revealed that formed nanointerface [P-*H···H2O*-Co], which facilitates water dissociation during Volmer–Heyrovsky pathway.

Язык: Английский

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The Single Atom Anchoring Strategy: Rational Design of MXene‐Based Single‐Atom Catalysts for Electrocatalysis

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 13, 2025

Abstract Single‐atom catalysts (SACs) are a class of with low dosage, cost, and the presence metal atom‐carrier interactions high catalytic activity, which considered to possess significant potential in field electrocatalysis. The most important aspect synthesis SACs is selection suitable carriers. Metal carbides, nitrides, or carbon‐nitrides (MXenes) widely used as new type 2D materials good electrical conductivity tunable surface properties. abundance functional groups vacancy defects on MXenes an ideal anchoring site for single atoms therefore regarded carrier single‐atom loading. In this work, preparation method MXenes, loading mode SACs, characterization catalysts, electrochemical performance described detail, some hot issues current research future directions also summarized. aim work promote development MXene‐based within realm With ongoing innovation, these expected be crucial energy conversion storage solutions.

Язык: Английский

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