Activity Trends and Mechanisms in Peroxymonosulfate‐Assisted Catalytic Production of Singlet Oxygen over Atomic Metal‐N‐C Catalysts

Gao, Yun; Wu, Tongwei; Yang, Chengdong; Ma, Chao; Zhao, Zhenyang; Wu, Zihe; Cao, Sujiao; Wang, Geng; Wang, Yi; Yao, Yongyi; Zhang, Yanning; Cheng, Chong

doi:10.1002/anie.202109530

Cited by 334 publications

(144 citation statements)

References 48 publications

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“…To clarify the active site of p‐CoSi 1 N 3 @D during PMS activation, the potassium thiocyanate (KSCN) poison experiment was firstly carried out. [ 56 ] As shown in Figure S37 in the Supporting Information, the remarkably inhibition of BPA removal in the presence of KSCN demonstrates the dominant role of CoSi 1 N 3 moiety in PMS activation. Which site (Co, N, or Si site) plays the major role in p‐CoSi 1 N 3 @D/PMS system was further evidenced by first principles density‐function theory (DFT) calculations.…”

Section: Resultsmentioning

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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Section: Resultsmentioning

confidence: 99%

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Dong

Chen

Tang

et al. 2022

Adv Funct Materials

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“…[225] By adjusting coordination structures and active site densities of SACs, it is expected to realize the nonfree radical persulfate activation, which lays a structural foundation for studying the intrinsic activity and simplifying descriptors of catalysts (see Figure 23 and Table 5 for details). [226][227][228][229][230][231] Generally, in advanced oxidation processes (AOPs), inexpensive and high-abundance Fe-based catalysts show the persulfate activation mechanism dominated by free radicals. Among nonfree radical mechanisms, the singlet oxygenation ( 1 O 2 ), high-valence Fe species (HV-Fe), and mediated electron transfer are the three most prominent mechanisms.…”

Section: Brief Summary Of Afcs On Electrocatalysismentioning

confidence: 99%

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Liao

et al. 2022

Small Structures

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In recent years, single‐atom catalysts (SACs) with high metal loading have emerged in different heterogeneous catalysis fields and shown extraordinary catalytic properties. When there are enough coordination atoms (or functional groups) on the supports, it is possible to achieve a limit monolayer atom loading on the surface of supports with ultrahigh atom density (5–15 atoms nm−2) and extremely close site distance (0.2–0.5 nm), by using appropriate synthesis methods and procedures. These high‐density metal atoms usually have no or less metal bonds, which are mostly isolated by support atoms to form 3D foam‐like atomic constructions. Herein, a new notion of metal atomic foam catalysts (AFCs) is propsed to redefine these ultrahigh‐density SACs accommodated by specific supports. This new paradigm of 3D atomic construction for SACs has potential significance for both theoretical research and industrial applications. The latest major advancements in the controllable synthesis of AFCs on various supports (e.g., polymer, carbon, and metallic compound) via different methods (bottom‐up or top‐down approaches) are summarized. The latent catalytic principles and typical application cases of AFCs are emphasized in a wide range of heterogeneous catalysis fields (e.g., thermocatalysis, photocatalysis, electrocatalysis, etc.). The challenges and prospects of this newly 3D ultrahigh‐density AFCs materials in practical industrial application are pointed out as well.

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Section: Porous Structure Designmentioning

confidence: 99%

“…In short, selecting suitable precursors and coordination compounds is pivotal to achieving a high density of M–N x sites, because they can remarkably populate the activity sites of M–N–C electrocatalysts for ORR. [ 130 ]…”

Section: Strategies To Increase the Catalytic Activity Of M–n–cmentioning

confidence: 99%

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Recent Advances in ZIF‐Derived Atomic Metal–N–C Electrocatalysts for Oxygen Reduction Reaction: Synthetic Strategies, Active Centers, and Stabilities

Chen

Yan

et al. 2022

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oxidation reaction on the anode, while the oxygen undergoes a reduction reaction on the cathode. However, the sluggish kinetics and instability of oxygen reduction reaction (ORR) electrocatalysts, especially in the practical acidic and oxidation environments, have severely hindered their further developments. Therefore, engineering ORR electrocatalysts with high activity and good stability is desired to promote energy transformation efficiency. By far, the most popular ORR electrocatalysts are the costly platinum group metal (PGM)-derived ones. However, the use of expensive, unsatisfied stability, and scarce PGM materials as ORR electrocatalyst limits the developments of this field. [8][9][10][11][12][13][14][15][16][17][18] To improve catalytic efficiency and cut the high expenditure, various strategies have been studied in recent years. Among them, electrocatalysts based on the metal-N-C (M-N-C) structures have attracted extensive attention in recent years due to their unique electronic structure to bind with the intermediates, abundant substitutional metal elements, maximum atomic utilization efficiency, as well as excellent stability. [19][20][21][22][23][24][25] Besides, compared to ORR electrocatalysts loaded with nanoclusters or nanoparticles, the M-N-C presents unambiguous catalytic sites and facile synthesis, which help the understanding of ORR mechanisms by precise theoretical calculations and in Exploring highly active, stable electrocatalysts with earth-abundant metal centers for the oxygen reduction reaction (ORR) is essential for sustainable energy conversion. Due to the high cost and scarcity of platinum, it is a general trend to develop metal-N-C (M-N-C) electrocatalysts, especially those prepared from the zeolite imidazolate framework (ZIF) to replace/minimize usage of noble metals in ORR electrocatalysis for their amazingly high catalytic efficiency, great stability, and readily-tuned electronic structure. In this review, the most pivotal advances in mechanisms leading to declined catalytic performance, synthetic strategies, and design principles in engineering ZIF-derived M-N-C for efficient ORR catalysis, are presented. Notably, this review focuses on how to improve intrinsic ORR activity, such as M-N x -C y coordination structures, doping metal-free heteroatoms in M-N-C, dual/ multi-metal sites, hydrogen passivation, and edge-hosted M-N x . Meanwhile, how to increase active sites density, including formation of M-N complex, spatial confinement effects, and porous structure design, are discussed. Thereafter, challenges and future perspectives of M-N-C are also proposed. The authors believe this instructive review will provide experimental and theoretical guidance for designing future, highly active ORR electrocatalysts, and facilitate their applications in diverse ORR-related energy technologies.

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Activity Trends and Mechanisms in Peroxymonosulfate‐Assisted Catalytic Production of Singlet Oxygen over Atomic Metal‐N‐C Catalysts

Cited by 334 publications

References 48 publications

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Recent Advances in ZIF‐Derived Atomic Metal–N–C Electrocatalysts for Oxygen Reduction Reaction: Synthetic Strategies, Active Centers, and Stabilities

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