Efficient degradation and mineralization of antibiotics via heterogeneous activation of peroxymonosulfate by using graphene supported single-atom Cu catalyst

Chen, Feng; Wu, Xilin; Liu, Yang; Chen, Chaofa; Lin, Hongjun; Chen, Jianrong

doi:10.1016/j.cej.2020.124904

Cited by 141 publications

(45 citation statements)

References 43 publications

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“…Quenching agents of KBrO 3 , isopropanol (IPA), triethanolamine (TEOA), Na 2 C 2 O 4 (EDTA-2Na), and benzoquinone (BQ) were applied for scavenging e − , •OH, h + , h + , and O 2 •− , respectively. [33,34] As shown in Figure 5a, KBrO 3 scavenger has no apparent effect on the degradation of BPA, indicating photoexcited free electrons were not directly involved in the catalytic oxidation. TEOA, EDTA-2Na and BQ inhibited the degradation of BPA by 30.8%, 43.5%, and 39.1%, respectively, indicating both h + and O 2…”

Section: Mechanism Studiesmentioning

confidence: 97%

Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

Chen

Shi

et al. 2021

Adv Funct Materials

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165

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Heterogeneous Fenton‐like reactions (HFLR) are promising alternative strategies to address the inherent limitations of the classic Fenton systems. Herein, a facile and scale‐up approach for the synthesis of transition metal single‐atom sites (SA‐TM, TM = Cr, Mn, Fe, Co, Cu) coordinated onto pyrrolic N‐rich g‐C3N4 (PN‐g‐C3N4) scaffold is developed. The regulated pyrrolic N‐rich SA‐TM catalytic sites exhibit excellent performances for HFLR. As a model of SA‐TM/PN‐g‐C3N4, SA‐Cr/PN‐g‐C3N4 is efficient for the catalytic oxidation of bisphenol A via HFLR under visible light with outstanding cyclic stability and wide effective pH range (3.0–11.0). The synergy of photocatalysis and single‐atom catalysis leads to accelerated production and separation of charge carriers as well as the cycling of Cr3+/Cr2+ couple, consequently boosting the performance in HFLR. Theoretical calculations indicate that the Cr(II)‐N4 sites with the metalloporphyrin‐like structure are more reactive than the doped Cr(II) sites in the g‐C3N4 matrix, which act as the peroxidase‐mimicking nanozyme for efficient and homolytic cleavage of peroxide OO in H2O2. This study expands the family of the iron‐free Fenton‐like systems and provides new strategies to the rational design and precise regulation of on‐demand multifunctional single‐atom catalysts for advanced water remediation.

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Section: Mechanism Studiesmentioning

confidence: 97%

Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

Chen

Shi

et al. 2021

Adv Funct Materials

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165

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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%

“…Recently, the copper (Cu)-based high-density SACs have also been proved to have considerable catalytic activity for the activation of PMS. [229,230,233] For example, Pan et al synthesized highdensity (%6 atoms nm À2 ) Cu atom anchored on the N-dopped biochar (SACu@NBC), which showed excellent catalytic activity for PMS activation and the complete removal of bisphenol A (BPA) within 30 min (see Figure 23H,I). [229] The mechanism of electron transfer in SACu@NBC/PMS system was accurately identified by anodic oxidation analogy, and the Cu single atom is the active center of catalyst, which can obviously improve the electron transfer and reaction activity of carbon carrier.…”

Section: Brief Summary Of Afcs On Electrocatalysismentioning

confidence: 99%

Section: Heterogeneous Catalysis Applications Of Afcsmentioning

confidence: 99%

mentioning

confidence: 99%

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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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Carbonaceous Catalysts for Pollutant Degradation

Kaswan

Khilari

Srivastava

et al. 2023

Carbon Allotropes and Composites

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Efficient degradation and mineralization of antibiotics via heterogeneous activation of peroxymonosulfate by using graphene supported single-atom Cu catalyst

Cited by 141 publications

References 43 publications

Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

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

Carbonaceous Catalysts for Pollutant Degradation

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Efficient degradation and mineralization of antibiotics via heterogeneous activation of peroxymonosulfate by using graphene supported single-atom Cu catalyst

Cited by 141 publications

References 43 publications

Molecular Engineering toward Pyrrolic N‐Rich M‐N4 (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

Molecular Engineering toward Pyrrolic N‐Rich M‐N4 (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

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

Carbonaceous Catalysts for Pollutant Degradation

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Product

Resources

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Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction

Molecular Engineering toward Pyrrolic N‐Rich M‐N₄ (M = Cr, Mn, Fe, Co, Cu) Single‐Atom Sites for Enhanced Heterogeneous Fenton‐Like Reaction