High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C<sub>3</sub>N<sub>4</sub>) for Highly Efficient Catalytic Advanced Oxidation Processes

An, Sufeng; Zhang, Guanghui; Wang, Tingwen; Zhang, Wenna; Li, Keyan; Song, Chunshan; Miller, Jeffrey T.; Miao, Shu; Wang, Junhu; Guo, Xinwen

doi:10.1021/acsnano.8b04693

Cited by 489 publications

(274 citation statements)

References 64 publications

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“…In a modified strategy reported by Chen et al, the as‐prepared silver tricyanomethanide was used as a miscible and reactive metal precursor to cocondensation with cyanamide, which ensured the homogeneity of the single atom dispersed Ag coordinated with g‐C 3 N 4 . An et al synthesized ultrasmall clusters and single atom Fe sites embedded in g‐C 3 N 4 through the pyrolysis of melamine and Fe salts at 600 °C . In some thinner g‐C 3 N 4 , only uniformly dispersed single‐atom Fe can be found, as confirmed by high‐angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) and extended X‐ray absorption fine structure (EXAFS).…”

Section: Synthesis Of Sacs In 2d Materialsmentioning

confidence: 93%

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Zhu

Peng

et al. 2019

Small Methods

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Single‐atom catalysts (SACs) on 2D nanomaterials have great potential as efficient and low‐cost electrocatalysts for clean energy technologies. The coordination environments, as well as the physicochemical properties of the 2D supports, play key roles in tuning the catalytic activity and reaction mechanism of the single‐atom centers. This review first summarizes the suitable synthetic strategies of single‐atom on different 2D supports. The methods that facilitate the formation of relative homogeneous structure and enable the regulation of the surrounding atomic environment of metal center are discussed. Furthermore, the recent progress of SACs for energy‐related electrochemical applications is reviewed, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. The strategies about modulation of the electronic structure of single‐atom for enhanced performance are highlighted, together with a discussion of the current issues and the prospects of this field.

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Section: Synthesis Of Sacs In 2d Materialsmentioning

confidence: 93%

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Zhu

Peng

et al. 2019

Small Methods

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“…Additionally, according to the charge density analysis (inset in Figure F), the significant electron transfer existed in peroxymonosulfate (PMS) and Co‐N 4 sites, which implied the strong chemisorption between reactants and active sites. In addition, Guo and co‐workers recently synthesized single‐atom Fe sites supported in g‐C 3 N 4 with dispersed Fe‐N x sites for catalytic oxidation reactions . Notedly, the excellent catalytic activity was attributed to the coordination effects.…”

Section: Defects‐based Single Atomic Electrocatalystmentioning

confidence: 99%

Defect‐Based Single‐Atom Electrocatalysts

et al. 2018

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Single‐atom catalysts (SACs) have attracted great attention owing to their maximum atomic utilization and high catalytic performance in electrochemical reactions. But the synthesis of SACs is not easy due to large surface energies of single atomic metal sites which often lead to their aggregation. The defects on supports can serve as anchor sites to stabilize single metal atoms and prevent them from aggregation, which has become an effective method to fabricate SACs. This review summarizes the meaningful findings about the defects on supports stabilizing single metal atoms, and their applications in electrocatalytic reaction. Various defects, including the intrinsic defects or heteroatom doping of carbon‐based materials, cation or anion vacancies of metal compound supports, and other defects (step edges, lattice defects, and caves), are comprehensively summarized, and the effects of defects on designing SACs are discussed. Although there are still many challenges to fully explore the SACs, it is believed that the newly established defect sites stabilized single atoms mechanism will be helpful for designing and fabricating highly powerful single atomic electrocatalysts for practical applications.

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“…Based on the identical geometric configurations and electronic structures of single‐atom active sites, SACs have demonstrated unpresented catalytic behaviors with enhanced catalytic activity and selectivity distinct from sub‐nanometer clusters or nanosized counterparts in diverse catalytic reactions including CO 2 reduction, electrocatalysis, Fenton‐like reaction, oxidase‐mimicking reaction, etc. More importantly, the homogeneous dispersion of single metal atoms on the supports facilitates the identification of active sites, thus elucidating the underlying reaction mechanism and providing the guidance for further designing high‐performance SACs.…”

Section: Biomedical Applications Of Sacsmentioning

confidence: 99%

Single‐Atom Catalysts in Catalytic Biomedicine

2020

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The intrinsic deficiencies of nanoparticle‐initiated catalysis for biomedical applications promote the fast development of alternative versatile theranostic modalities. The catalytic performance and selectivity are the critical issues that are challenging to be augmented and optimized in biological conditions. Single‐atom catalysts (SACs) featuring atomically dispersed single metal atoms have emerged as one of the most explored catalysts in biomedicine recently due to their preeminent catalytic activity and superior selectivity distinct from their nanosized counterparts. Herein, an overview of the pivotal significance of SACs and some underlying critical issues that need to be addressed is provided, with a specific focus on their versatile biomedical applications. Their fabrication strategies, surface engineering, and structural characterizations are discussed briefly. In particular, the catalytic performance of SACs in triggering some representative catalytic reactions for providing the fundamentals of biomedical use is discussed. A sequence of representative paradigms is summarized on the successful construction of SACs for varied biomedical applications (e.g., cancer treatment, wound disinfection, biosensing, and oxidative‐stress cytoprotection) with an emphasis on uncovering the intrinsic catalytic mechanisms and understanding the underlying structure–performance relationships. Finally, opportunities and challenges faced in the future development of SACs‐triggered catalysis for biomedical use are discussed and outlooked.

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High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C₃N₄) for Highly Efficient Catalytic Advanced Oxidation Processes

Cited by 489 publications

References 64 publications

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Defect‐Based Single‐Atom Electrocatalysts

Single‐Atom Catalysts in Catalytic Biomedicine

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High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes

Cited by 489 publications

References 64 publications

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Defect‐Based Single‐Atom Electrocatalysts

Single‐Atom Catalysts in Catalytic Biomedicine

Contact Info

Product

Resources

About

High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C₃N₄) for Highly Efficient Catalytic Advanced Oxidation Processes