A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution

Nature Synthesis, Год журнала: 2024, Номер 3(7), С. 878 - 890

Опубликована: Июнь 3, 2024

Язык: Английский

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Modulating Electronic Structure Engineering of Atomically Dispersed Cobalt Catalyst in Fenton-like Reaction for Efficient Degradation of Organic Pollutants

Environmental Science & Technology, Год журнала: 2023, Номер 57(37), С. 14071 - 14081

Опубликована: Сен. 8, 2023

Currently, the lack of model catalysts limits understanding catalytic essence. Herein, we report functional group modification single atom (SACs) with an accurately regulated electronic structure for accelerating sluggish kinetics Fenton-like reaction. The amino-modified cobalt phthalocyanine anchored on graphene (CoPc/G-NH2) shows superior performance in peroxymonosulfate (PMS) based reaction Co mass-normalized pseudo-first-order rate constants (kobs, 0.2935 min-1), which is increased by 4 and 163 times compared to those CoPc/G (0.0737 min-1) Co3O4/G (0.0018 min-1). Density theory (DFT) calculations demonstrate that -NH2 narrows gap between d-band center Fermi level a atom, strengthens charge transfer at interface reduces free energy barrier activation PMS. Moreover, scale-up experiment realizes 100% phenol removal 7200-bed volumes during 240 h continuous operation without obvious decline performance. This work provides in-depth insight into mechanism reactions demonstrates engineering SACs as effective strategy improving activity achieve goal practical application.

Язык: Английский

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Ambient Electrosynthesis toward Single‐Atom Sites for Electrocatalytic Green Hydrogen Cycling

Advanced Materials, Год журнала: 2023, Номер 35(14)

Опубликована: Фев. 17, 2023

With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting further utilization via hydrogen-oxygen fuel cells, such that a vast majority synthetic strategies toward SAS-based (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers novel, safe, effective route to access SASs. Herein, recent progress in ambient SASs sustainable future opportunities discussed. A systematic summary is started on three kinds electrochemically routes SASs, including electrochemical etching (ECE), direct electrodeposition (DED), leaching-redeposition (ELR), associated advanced characterization techniques. Next, their applications energy conversion evolution reaction, oxygen overall splitting, reduction reaction reviewed. Finally, brief conclusion remarks challenges regarding development high-performance cost-effective SASCs many other presented.

Язык: Английский

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Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

JACS Au, Год журнала: 2023, Номер 3(3), С. 736 - 755

Опубликована: Фев. 16, 2023

Single-atom catalysts (SACs) are emerging as the most promising for various electrochemical reactions. The isolated dispersion of metal atoms enables high density active sites, and simplified structure makes them ideal model systems to study structure–performance relationships. However, activity SACs is still insufficient, stability usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, catalytic mechanism on a single site unclear, leading development rely trial-and-error experiments. How can one break current bottleneck sites density? further increase activity/stability sites? In this Perspective, we discuss underlying reasons challenges identify precisely controlled synthesis involving designed precursors innovative heat-treatment techniques key high-performance SACs. addition, advanced operando characterizations theoretical simulations essential uncovering true electrocatalytic an site. Finally, future directions that may arise breakthroughs discussed.

Язык: Английский

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Metal Alloys‐Structured Electrocatalysts: Metal–Metal Interactions, Coordination Microenvironments, and Structural Property–Reactivity Relationships

Advanced Materials, Год журнала: 2023, Номер 35(51)

Опубликована: Апрель 24, 2023

Metal alloys-structured electrocatalysts (MAECs) have made essential contributions to accelerating the practical applications of electrocatalytic devices in renewable energy systems. However, due complex atomic structures, varied electronic states, and abundant supports, precisely decoding metal-metal interactions structure-activity relationships MAECs still confronts great challenges, which is critical direct future engineering optimization MAECs. Here, this timely review comprehensively summarizes latest advances creating MAECs, including interactions, coordination microenvironments, relationships. First, fundamental classification, design, characterization, structural reconstruction are outlined. Then, merits modulation strategies recent breakthroughs for noble non-noble metal-structured thoroughly discussed, such as solid solution alloys, intermetallic single-atom alloys. Particularly, unique insights into bond theoretical understanding, operando techniques mechanism disclosure given. Thereafter, current states diverse with a focus on property-reactivity relationships, reaction pathways, performance comparisons discussed. Finally, challenges perspectives systematically It believed that comprehensive can offer substantial impact stimulating widespread utilization metal materials electrocatalysis.

Язык: Английский

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