Enhanced Interfacial Electron Transfer by Asymmetric Cu‐Ov‐In Sites on In2O3 for Efficient Peroxymonosulfate Activation

Zhao, Zhiyong; Wang, Pengfei; Song, Chunlin; Zhang, Tao; Zhan, Sihui; Li, Yang

doi:10.1002/anie.202216403

Cited by 78 publications

(22 citation statements)

References 58 publications

(48 reference statements)

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“…), high-valent metal-oxo complexes, mediated electron transfer mechanisms, and singlet oxygen ( 1 O 2 )]. 6−10 Among them, 1 O 2 behaves as a versatile and universal oxidation species with a lifetime much longer than that of radicals in AOPs. 11,12 However, apparent drawbacks of traditional M−N−C catalysts such as the poor production of 1 O 2 , slow catalytic kinetics, and low metal utilization greatly restrict their application in actual wastewater treatment.…”

Section: •−mentioning

confidence: 99%

“…11,12 However, apparent drawbacks of traditional M−N−C catalysts such as the poor production of 1 O 2 , slow catalytic kinetics, and low metal utilization greatly restrict their application in actual wastewater treatment. Developing novel processes to efficiently produce potent reactive 1 O 2 is highly desired.…”

Section: •−mentioning

confidence: 99%

“…Application of the Catalyst in Real Wastewater Treatment. The nonradical mechanism dominated by 1 O 2 has robust abilities to resist the interference of environmental media. Cl − , H 2 PO 4 − , and HA have minor effects on the degradation of contaminants in Fe−N x C 4−x systems (Figure S36).…”

Section: Catalytic Performance and Identification Of Rosmentioning

confidence: 99%

“…22−25 Significant progress has been made in the field of single-atom catalysis in the past decade, but a profound understanding of the structure−property correlation of SACs at the atomic scale remains a challenging task. Nitrogen-doped carbon-supported (NC) SACs have been extensively used to convert PMS into 1 O 2 to efficiently degrade organic pollutants. 26−29 The pyrolysis strategy remains the most commonly used method for preparing carbon-supported SACs.…”

Section: •−mentioning

confidence: 99%

“…Realizing water pollution control and the sustainable development of ecological environments depend on many critical catalytic processes. Specifically, peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) have been recognized as an efficient way of treating recalcitrant organic pollutants from wastewater by generating robust reactive oxygen species (ROS). – Compared with the homogeneous catalytic processes initiated by transition metal ions (Fe 2+ , Co 2+ , and Cu 2+ ), heterogeneous Fenton catalytic processes have great advantages regarding catalyst recovery and catalytic stability. Especially, abundant carbon-supported transition metal–N–C catalysts (M–N–C: M = Fe, Co, Mn, and Cu) have gained considerable interest in PMS activation for generating numerous ROS [i.e., hydroxyl radicals ( • OH), sulfate radicals (SO 4 •– ), high-valent metal-oxo complexes, mediated electron transfer mechanisms, and singlet oxygen ( 1 O 2 )]. – Among them, 1 O 2 behaves as a versatile and universal oxidation species with a lifetime much longer than that of radicals in AOPs. , However, apparent drawbacks of traditional M–N–C catalysts such as the poor production of 1 O 2 , slow catalytic kinetics, and low metal utilization greatly restrict their application in actual wastewater treatment.…”

Section: Introductionmentioning

confidence: 99%

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Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Wu,

Huang,

Wang

et al. 2023

Environ. Sci. Technol.

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Precisely identifying the atomic structures in single-atom sites and establishing authentic structure–activity relationships for single-atom catalyst (SAC) coordination are significant challenges. Here, theoretical calculations first predicted the underlying catalytic activity of Fe–N x C4–x sites with diverse first-shell coordination environments. Substituting N with C to coordinate with the central Fe atom induces an inferior Fenton-like catalytic efficiency. Then, Fe-SACs carrying three configurations (Fe–N2C2, Fe–N3C1, and Fe–N4) fabricate facilely and demonstrate that optimized coordination environments of Fe–N x C4–x significantly promote the Fenton-like catalytic activity. Specifically, the reaction rate constant increases from 0.064 to 0.318 min–1 as the coordination number of Fe–N increases from 2 to 4, slightly influencing the nonradical reaction mechanism dominated by 1O2. In-depth theoretical calculations unveil that the modulated coordination environments of Fe-SACs from Fe–N2C2 to Fe–N4 optimize the d-band electronic structures and regulate the binding strength of peroxymonosulfate on Fe–N x C4–x sites, resulting in a reduced energy barrier and enhanced Fenton-like catalytic activity. The catalytic stability and the actual hospital sewage treatment capacity also showed strong coordination dependency. This strategy of local coordination engineering offers a vivid example of modulating SACs with well-regulated coordination environments, ultimately maximizing their catalytic efficiency.

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Section: •−mentioning

confidence: 99%

Section: •−mentioning

confidence: 99%

Section: Catalytic Performance and Identification Of Rosmentioning

confidence: 99%

Section: •−mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Wu,

Huang,

Wang

et al. 2023

Environ. Sci. Technol.

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Revealing the Role of Binary Distortion in PMS Activation over Spinel toward Efficient New Pollutants Removal

Wang,

Zhao,

Zhang

et al. 2024

Adv Funct Materials

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Improving peroxymonosulfate (PMS) activation efficiency to enhance simultaneous generation of radicals and non‐radicals is essential for removing new pollutants (NPs) in complex waters. However, achieving this with standard lattice‐structured heterogeneous catalysts remains challenging due to inefficient electron transfer. Here, CuCo2O4 properties are successfully tuned by controlling lattice distortion, enabling simultaneous PMS oxidation and reduction. Unlike the slow rate of electron transfer in heterogeneous metal catalysts with standard lattice structures, the highly active binary lattice distortion in CuCo2O4 alters the structure and electron distribution, exposes more Cu and Co sites, lowers the PMS adsorption barriers, and realizes the synergistic production of SO4•−/•OH), and 1O2. The k‐value for ciprofloxacin is as high as 17.83 min−1 M−1, 29.42 times higher than that with non‐binary lattice distortion. Additionally, the developed intermittent reactor consistently maintains a removal rate above 95% over five cycles in actual wastewater treatment scenarios. This work provides a new avenue for achieving the removal of new pollutants in complex water bodies.

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Intensify Mass Transfer and Molecular Oxygen Activation by Defect‐Bridged Asymmetric Catalytic Sites Toward Efficient Membrane‐Based Nanoconfined Catalysis

Ye,

Xue,

Wang

et al. 2024

Adv Funct Materials

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Efficient spontaneous molecular oxygen (O2) activation is expected in advanced oxidation processes. However, it remains a great challenge to promote the reactants adsorption and accelerate the interfacial electron transfer to boost the activation kinetic of O2. Herein, defect‐rich N‐doped reduced graphene oxide/CoFe2O4 (NGCF‐OV) membrane containing asymmetric Co‐OV‐Fe sites is prepared for O2 activation. The intrinsic catalytic activity is that the asymmetric Co‐OV‐Fe sites regulate the O─O bond length, promoting more and faster electron transfer to O2 for selectively producing 1O2. Meanwhile, the adjacent graphitic N sites help confine organics to the surface and thus greatly shorten the reaction distance of 1O2 and improve its utilization efficiency. The NGCF‐OV membrane demonstrates complete degradation of bisphenol A within a retention time of 86 ms, achieving a k‐value of 0.047 ms−1, which exceeds the performance of most Fenton‐like systems. This work provides new horizons for designing an efficient and stable catalytic membrane, enriching the domain of advanced wastewater treatment strategies.

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Enhanced Interfacial Electron Transfer by Asymmetric Cu‐O_v‐In Sites on In₂O₃ for Efficient Peroxymonosulfate Activation

Cited by 78 publications

References 58 publications

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification

Revealing the Role of Binary Distortion in PMS Activation over Spinel toward Efficient New Pollutants Removal

Intensify Mass Transfer and Molecular Oxygen Activation by Defect‐Bridged Asymmetric Catalytic Sites Toward Efficient Membrane‐Based Nanoconfined Catalysis

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