Atomically dispersed cobalt on graphitic carbon nitride as a robust catalyst for selective oxidation of ethylbenzene by peroxymonosulfate

Li, Jiaquan; Zhao, Shiyong; Yang, Shize; Wang, Shaobin; Sun, Hongqi; Jiang, San Ping; Johannessen, Bernt; Liu, Shaomin

doi:10.1039/d0ta11503g

Cited by 53 publications

(49 citation statements)

References 45 publications

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“…[ 11–17 ] Such unique properties make Co SACs an attractive platform to bridge the gap between homogeneous and heterogeneous PMS activation. [ 1,11,17–20 ]…”

Section: Introductionmentioning

confidence: 99%

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Dong

Chen

Tang

et al. 2022

Adv Funct Materials

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Single atom catalysts (SACs) have been growing as an emerging "hot" topic in environmental remediation. Their performance can be rationally optimized via modulating spatial coordination configuration and the porous structure of SACs, which is still challenging. Herein, a novel Si, N co-coordinated cobalt SAC (p-CoSi 1 N 3 @D) with 3D free standing architecture is tailored via employing natural mineral (diatomite) as a Si source and porous template. Theoretical calculations and experimental analysis reveal that the substitution of N by Si dramatically accelerates the interaction and electron transfer between peroxymonosulfate and the Co single atom center. Moreover, p-CoSi 1 N 3 @D inherits the hierarchically porous architecture of diatomite, providing more accessible cobalt sites and open diffusion channels for peroxymonosulfate and contaminants in water treatment applications. Thanks to optimal coordination structure and porous architecture, p-CoSi 1 N 3 @D can serve as a highly active catalyst for peroxymonosulfate activation, with a turnover frequency of 299.8 min −1 for bisphenol A degradation, surpassing those of catalysts with transition metal SACs or oxides in the disclosed literature. This work provides a novel strategy for the development of SACs for wastewater reclamation, and deepens the understanding of the significant role of templates in spatial coordination configuration of SACs.

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“…[ 11–17 ] Such unique properties make Co SACs an attractive platform to bridge the gap between homogeneous and heterogeneous PMS activation. [ 1,11,17–20 ]…”

Section: Introductionmentioning

confidence: 99%

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Dong

Chen

Tang

et al. 2022

Adv Funct Materials

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show abstract

“…The process of electron transfer is further con rmed by the obviously increased cathodic current densities for the p-CoSi 1 N 3 @D electrode with the addition of PMS in the LSV analysis (Supplementary Fig. 27) 18,50,51 . In comparison to CoN 4 , the CoSi 1 N 3 moieties possess a larger electron density difference of PMS adsorbed on the Co single atoms.…”

Section: Radical (Somentioning

confidence: 80%

“…Catalyst structure during PMS activation. The electron transfer between PMS molecules and Co active centers was regarded as the rate determining process in the nonradical pathway 14,18 . To gain further insights into the relationship between electron transfer, PMS activation properties and spatial coordination con guration of cobalt single atom active sites, rst principles density-function theory (DFT) calculations were further carried out.…”

Section: Radical (Somentioning

confidence: 99%

“…The Co isolated single atoms grafted to a carbon basal plane with CoN x moieties have been proven as desirable catalysts for PMS activation 11,14,18,[20][21][22] . In most cases, the reactive site structure was reported as the planar four-coordinated con guration of CoN 4 moieties 12,13,[23][24][25] .…”

Section: Introductionmentioning

confidence: 99%

“…In recent years, Co single atom catalysts (SACs), as one of the most emerging kinds of heterogeneous catalysts, possess special electronic structure, utmost Co atom utilization e ciency, and uniformly isolated Co active sites [11][12][13][14][15][16][17] . Such unique properties make Co SACs an attractive platform to bridge the gap between homogeneous and heterogeneous PMS activation 1,11,[17][18][19][20] .…”

Section: Introductionmentioning

confidence: 99%

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Natural mineral modulated single atom catalyst for effective water treatment

Dong¹,

Chen²,

Tang³

et al. 2021

Preprint

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Single atom catalysts (SACs) have been growing as an emerging “hot” topic in environmental remediation. Their performance can be rationally optimized via modulating spatial coordination configuration and porous structure of SACs, which is still challenging. Herein, a novel Si, N co-coordinated cobalt SACs (p-CoSi1N3@D) with 3D freestanding architecture was tailored via employing natural mineral (diatomite) as Si source and porous template. Theoretical calculations and experimental analysis reveal that Si substitution dramatically decreases electronegativity of CoN4 moieties and thus accelerates interaction and electron transfer between peroxymonosulfate and Co single atom center. Moreover, p-CoSi1N3@D inherits hierarchically porous architecture of diatomite, providing more accessible cobalt sites and open diffusion channels for peroxymonosulfate and contaminants in water treatment applications. Thanks to optimal coordination structure and porous architecture, p-CoSi1N3@D can serve as highly active catalyst toward peroxymonosulfate activation, with a turn-over frequency of 299.8 min− 1 for bisphenol A degradation, surpassing those of catalysts with transition metal SACs or oxides in disclosed literature. This work provides a novel vision for development of SACs towards wastewater reclamation.

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Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

Wang

et al. 2023

Adv Funct Materials

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Photocatalytic generation of •OH from O3 is an intriguing avenue for aqueous organics degradation due to the high utilization of photogenerated electrons, but ambiguous information about charge transfer and surface‐active sites hinders the optimization of photocatalysts. In this work, a series of cobalt single‐atom catalysts (SACs) anchored on graphitic carbon nitride to improve •OH generation from O3 via electron reduction and catalytic activation dual pathway is synthesized. Various characterization and density functional theory calculations reveal that cobalt single atoms can introduce trap states for holes, which improve the light‐harvesting ability and accelerate the transfer of electrons and holes. Meanwhile, Co single atoms can also act as active sites to accelerate ozone decomposition and produce •OH directly. Particularly, the influence of different surface densities of Co single atoms on photogenerated electron supply and surface reaction is disclosed. A higher density of Co provided more active sites for O3 catalytic activation, but the narrowed distance between oxidation and reduction centers reduces the supply of available electrons by worsening the charge recombination. This work offers an atomic‐level correlation of the isolated metal density and photocatalytic properties, and can scientifically guide the design of high‐performance photocatalysts for organic synthesis and water purification.

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Atomically dispersed cobalt on graphitic carbon nitride as a robust catalyst for selective oxidation of ethylbenzene by peroxymonosulfate

Abstract: The development of highly efficient strategy for the activation C-H bond in hydrocarbons for organic synthesis is one of the most challenging tasks facing the chemical industries. Novel catalyst with...

Cited by 53 publications

References 45 publications

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Natural mineral modulated single atom catalyst for effective water treatment

Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

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