Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(19), С. 12976 - 12983

Опубликована: Апрель 3, 2024

Electrocatalytic reduction of nitrate to ammonia (NRA) has emerged as an alternative strategy for sewage treatment and generation. Despite excellent performances having been achieved over cobalt-based electrocatalysts, the reaction mechanism well veritable active species across a wide potential range are still full controversy. Here, we adopt CoP, Co, Co3O4 model materials solve these issues. CoP evolves into core@shell structured CoP@Co before NRA. For Co catalysts, three-step relay is carried out superficial dynamical Coδ+ under low overpotential, while continuous hydrogenation from unveiled high overpotential. In comparison, stable steadily catalyze range. As result, exhibit much higher NRA activity than especially Moreover, performance although they experience same mechanism. A series characterizations clarify reason enhancement highlighting that core donates abundant electrons species, leading generation more hydrogen nitrogen-containing intermediates.

Язык: Английский

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Mixed Plastics Wastes Upcycling with High-Stability Single-Atom Ru Catalyst

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(41), С. 22836 - 22844

Опубликована: Окт. 5, 2023

Mixed plastic waste treatment has long been a significant challenge due to complex composition and sorting costs. In this study, we have achieved breakthrough in converting mixed wastes into single chemical product using our innovative single-atom catalysts for the first time. The Ru catalyst can convert ∼90% of real methane products (selectivity >99%). unique electronic structure sites regulates adsorption energy intermediates, leading rapid decomposition plastics superior cycle stability compared traditional nanocatalysts. global warming potential entire process was evaluated. Our proposed carbon-reducing utilizing launches new era valorization.

Язык: Английский

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Dual-Atom Co/Ni Electrocatalyst Anchored at the Surface-Modified Ti₃C₂T_x MXene Enables Efficient Hydrogen and Oxygen Evolution Reactions

ACS Nano, Год журнала: 2024, Номер 18(5), С. 4256 - 4268

Опубликована: Янв. 24, 2024

Dual-atom catalytic sites on conductive substrates offer a promising opportunity for accelerating the kinetics of multistep hydrogen and oxygen evolution reactions (HER OER, respectively). Using MXenes as is strategy depositing those dual-atom electrocatalysts, if efficient surface anchoring ensuring metal-substrate interactions sufficient mass loading established. We introduce surface-modification MXene by preadsorbing L-tryptophan molecules, which enabled attachment Co/Ni electrocatalyst at Ti3C2Tx forming N–Co/Ni-O bonds, with reaching high 5.6 wt %. The electron delocalization resulting from terminated O atoms substrates, N in moieties, metal Co Ni provides an optimal adsorption strength intermediates boosts HER OER kinetics, thereby notably promoting intrinsic activity electrocatalyst. CoNi-Ti3C2Tx displayed overpotentials 31 241 mV 10 mA cm–2, respectively. Importantly, also exhibited operational stability both over 100 h industrially relevant current density 500 cm–2. Our study provided guidance constructing active to synergistically enhance electrochemical efficiency energy conversion storage systems.

Язык: Английский

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Solar-driven photocatalysis for recycling and upcycling plastics

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 341, С. 123357 - 123357

Опубликована: Сен. 30, 2023

Язык: Английский

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Emerging Strategies for the Synthesis of Correlated Single Atom Catalysts

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Фев. 9, 2024

Abstract People have been looking for an energy‐efficient and sustainable method to produce future chemicals decades. Heterogeneous single‐atom catalysts (SACs) with atomic dispersion of robust, well‐characterized active centers are highly desirable. In particular, correlated SACs cooperative interaction between adjacent single atoms allow the switching single‐site pathway dual or multisite pathway, thus promoting bimolecular more complex reactions synthesis fine chemicals. Herein, structural uniqueness SACs, including intermetal distance electronic in homo/heteronuclear metal sites is featured. Recent advances production methods showcasing research status challenges traditional (such as pyrolysis, wet impregnation, confined synthesis) building a comprehensive multimetallic SAC library, summarized. Emerging strategies such process automation continuous‐flow highlighted, minimizing inconsistency laboratory batch allowing high throughput screening upscaling toward next‐stage chemical by SACs.

Язык: Английский

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Plastic Waste Recycling─A Chemical Recycling Perspective

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(33), С. 12270 - 12288

Опубликована: Июль 1, 2024

This article provides an overview of plastic recycling development since the 1970s. It discusses three common options: mechanical recycling, chemical and energetic recycling. Additionally, it considers challenges waste cleaning sorting. The describes processes in detail for main constituents waste, such as polyethylene (PE), polypropylene (PP), polystyrene (PS), polyvinyl chloride (PVC), terephthalate (PET). current rates indicate that only is economically viable, which insufficient a sustainable circular economy. Chemical methods are often too energy-intensive require complex presorting making them unattractive. To become competitive, requirements have been derived this article. In context, splitting polymer chains using low-temperature atmospheric pressure plasma proposed novel technology. date, technology has used surface treatment plastic. However, shows potential processing unsorted, low-value especially PE, PP, mixed would otherwise be sent incineration or to landfills. Mechanical unsuitable these streams, competitive not yet established on industrial scale.

Язык: Английский

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General Design Concept of High‐Performance Single‐Atom‐Site Catalysts for H₂O₂ Electrosynthesis

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 5, 2024

Hydrogen peroxide (H

Язык: Английский

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Covalent Organic Framework with Donor¹‐Acceptor‐Donor² Motifs Regulating Local Charge of Intercalated Single Cobalt Sites for Photocatalytic CO₂ Reduction to Syngas

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 22, 2024

Covalent organic framework (COF) has attracted increasing interest in photocatalytic CO

Язык: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Язык: Английский

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Tandem microplastic degradation and hydrogen production by hierarchical carbon nitride-supported single-atom iron catalysts

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 10, 2024

Abstract Microplastic pollution, an emerging environmental issue, poses significant threats to aquatic ecosystems and human health. In tackling microplastic pollution advancing green hydrogen production, this study reveals a tandem catalytic degradation-hydrogen evolution reaction (MPD-HER) process using hierarchical porous carbon nitride-supported single-atom iron catalysts (FeSA-hCN). Through hydrothermal-assisted Fenton-like reactions, we accomplish near-total ultrahigh-molecular-weight-polyethylene degradation into C 3 -C 20 organics with 64% selectivity of carboxylic acid under neutral pH, leap beyond current capabilities in efficiency, selectivity, eco-friendliness, stability over six cycles. The system demonstrates versatility by degrading various daily-use plastics across different settings. mixture FeSA-hCN plastic products further achieves 42 μmol h ‒1 illumination, outperforming most existing photoreforming methods. This MPD-HER not only provides scalable economically feasible strategy combat but also contributes the economy, far-reaching implications for global sustainability initiatives.

Язык: Английский

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