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Article
Chemistry, Physical
Xinyu Song et al.
Summary: This study explores the discriminative activities and mechanisms for activation of O-O bond in peroxy compounds via single-atom catalysts (SACs) with higher coordination numbers (M-N5). The atomic catalyst (Fe-SAC) with Fe-N5 as the active center was constructed, effectively activating peroxymonosulfate (PMS), peroxydisulfate (PDS), and hydrogen peroxide (H2O2). The study demonstrates the degradation efficiencies of acyclovir are related to the O-O bond length in different peroxy compounds, and reveals the discriminative mechanisms for activation of O-O bond in different Fenton-like systems.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Engineering, Environmental
Zelin Wu et al.
Summary: The catalytic activity of Fe-NxC4-x sites with different coordination environments was predicted through theoretical calculations. Substituting N with C to coordinate with Fe atom resulted in inferior Fenton-like catalytic efficiency. Three configurations of Fe-SACs (Fe-N2C2, Fe-N3C1, and Fe-N4) were fabricated and showed that optimized Fe-NxC4-x coordination environments significantly promoted Fenton-like catalytic activity. The coordination dependency of Fe-SACs was also observed in terms of catalytic stability and actual hospital sewage treatment capacity. This strategy of local coordination engineering provides an example of how to modulate SACs with well-regulated coordination environments to maximize their catalytic efficiency.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Bingkun Huang et al.
Summary: This study reports the functional group modification of model single atom catalysts (SACs) to improve the catalytic performance in Fenton-like reactions. The modified cobalt phthalocyanine catalyst exhibited superior catalytic activity and the mechanism was revealed through density functional theory (DFT) calculations. Scale-up experiments also demonstrated the stability and efficiency of the catalyst.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Bingkun Huang et al.
Summary: This study proposes a novel peroxymonosulfate (PMS) activation system that utilizes the surface-confinement effect to accelerate the catalytic oxidation process. The generation of high-valent iron-oxo species is confirmed through experiments, and the surface-confinement effect is shown to enhance the charge transfer rate and reduce the free energy barrier for PMS activation. The system exhibits excellent pollutant degradation efficiency, resistance to coexisting matter, and adaptability to a wide pH range and temperature environments.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Kexin Yin et al.
Summary: Two coordination structures (Co-N4 or Co-N3) of cobalt single-atom catalysts (Co-SACs) were prepared using chitosan as a starting precursor to evaluate their effect on organic degradation. The performance of degrading carbamazepine (CBZ) and the radical/nonradical pathways in Co-N4/PMS and Co-N3/PMS systems were evaluated. Results showed that the Co-N3 catalyst produced more radicals due to stronger PMS adsorption and subsequent peroxide bond cleavage of PMS. The Co-N3 coordination also enhanced the electron-transfer process for CBZ. This study provides insights into the versatile catalytic pathways of carbon-based SACs for high-efficiency PMS activation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Xinhao Wang et al.
Summary: Rationally regulating reaction mechanisms in Fenton-like reactions by tuning the properties of catalysts is challenging but significant. Various catalysts with different active center sizes were synthesized to realize the switching of reaction mechanisms and pollutant degradation routes in peroxymonosulfate (PMS) activation systems. The transformation of reaction mechanism from radical oxidation to nonradical oxidation was observed with the decrease of active center size. The toxicity tests indicated that the conversion from non-selective to selective oxidation resulted in lower toxicity of effluent after reaction, reducing environmental risks.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Yanan Shang et al.
Summary: Metal-based catalysts with different sizes, including metal nanoparticles and single atom catalysts, exhibit excellent catalytic activities in various Fenton-like reactions. However, the instability of their surface/structure is a critical issue, leading to rapid deactivation and failure in long-term operation. It is necessary to analyze the catalytic stability of these catalysts in the presence of versatile peroxides (H2O2, peroxymonosulfate (PMS), and peroxodisulfate (PDS)). Additionally, strategies for catalyst regeneration and recyclability improvement are important for practical applications of metal-based catalysts.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Xiongbo Dong et al.
Summary: Single atom catalysts (SACs) have emerged as a hot topic in environmental remediation. This study presents a novel Si, N co-coordinated cobalt SAC with a 3D free-standing architecture, which is tailored using natural mineral diatomite as a Si source and porous template. The catalyst exhibits excellent performance in peroxymonosulfate activation for wastewater treatment, surpassing previously reported catalysts. The work provides a new strategy for SACs development and enhances the understanding of the role of templates in spatial coordination configuration of SACs.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Review
Engineering, Environmental
Wei Ren et al.
Summary: This review discusses the use of persulfate-based nonradical oxidation processes (PS-NOPs) in wastewater purification, focusing on recent advances in nonradical electron-transfer regimes, including design of catalysts, in situ/operando characterization/analytics, and understanding the origins of electron-transfer mechanisms. The study found that persulfate is activated by a catalyst to form surface activated complexes, which interact directly or indirectly with target pollutants for oxidation.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Engineering, Environmental
Bingkun Huang et al.
Summary: This study presents a Co2+/PMS/H3BO3 system that can effectively generate ROS with ultra-low Co2+ dosage, showing fast reactivity towards various pollutants. The introduction of borate buffer significantly promotes the generation of ROS, with the key substance inferred as H2BO3--MS. Through theoretical and experimental analyses, the system's high performance is attributed to a turnover frequency much higher than current research.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Multidisciplinary Sciences
Xiao Zhou et al.
Summary: Controlling the electronic structure of Cu-N-4 sites through heteroatom doping engineering can optimize the activation ability of peroxymonosulfate (PMS). Experimental results show that the electron-deficient Cu-N-4/C-B exhibits the highest oxidation capacity, while the electron-enriched Cu-N-4/C-P leads to a decrease in activation ability. This study provides a new approach to finely control the electronic structure of Cu-N-4 sites at the atomic level and guide the design of smart Fenton-like catalysts.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Yu Xiong et al.
Summary: Recognizing and controlling the structure-activity relationships of single-atom catalysts is crucial for manipulating their catalytic properties. The study on Fe single-atom catalysts supported on nitrogen-doped carbon reveals high catalytic reactivity, stability, and wide pH suitability in Fenton-like reactions, with the roles of different N species further explored both experimentally and theoretically. Density functional theory calculations highlight how the location of d-band center of Fe sites affects the generation of Fe-oxo intermediates, leading to excellent catalytic properties.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Cancan Ling et al.
Summary: By constructing a dual Cu-Fe site, selective and efficient activation of H2O2 can be achieved, enabling effective oxidation of various toxic pollutants across a broad pH range. This work has significant implications for environmental control and other applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Environmental
Jingjing Jiang et al.
Summary: This study successfully generated high-valent cobalt-oxo species (Co(IV)???O) by introducing nitrogen vacancies into graphite carbon nitride. The developed synergistic system showed remarkable selectivity and contaminant removal performance in various aqueous matrices. This provides a novel mechanistic perspective for refractory contaminant treatment through defect engineering.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Engineering, Environmental
Yiyuan Yao et al.
Summary: Single oxygen-based advanced oxidation processes show great promise in selectively degrading organic pollutants. However, achieving efficient production of O-1(2) through tailored catalyst design for selective oxidation of contaminants remains challenging.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Engineering, Environmental
Zelin Wu et al.
Summary: Metal leaching and catalytic stability are important issues in Fenton-like reactions. In this study, a hollow yolk-shell nanoreactor (HYSCN) was fabricated to activate peroxymonosulfate (PMS) for the degradation of carbamazepine (CBZ). The HYSCN showed reduced metal leaching and improved catalytic stability compared to a solid structure (SCSCN). The mechanism of the HYSCN/PMS system was investigated and the degradation pathway of CBZ was proposed using UPLC-Q-TOF-MS/MS.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Multidisciplinary Sciences
Ying-Jie Zhang et al.
Summary: Removal of organic micropollutants from water through advanced oxidation processes is hindered by excessive energy and/or chemical input, as well as the generation of large amounts of residuals. The authors propose a new water purification technology called the direct oxidative transfer process (DOTP) that can achieve complete and efficient decontamination at low oxidant dosage. DOTP differs from traditional methods in pollutant removal behavior and mechanisms, and offers favorable features such as low energy consumption, no residual byproducts, and robust performance in real environmental matrices.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yan Bao et al.
Summary: In this study, we propose the construction of a neutral microenvironment on the surface of Zn-Fe layered double hydroxide for activating PMS. By utilizing the amphoteric properties of zinc hydroxide, equivalent to Fe-IV=O can be continuously generated over a wide pH range. The neutral microenvironment mitigates the self-decomposition of Fe-IV=O and the hydrolysis reaction of iron, resulting in stable and efficient treatment of wastewater.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Environmental
Mengxue Yang et al.
Summary: In this study, the origins of selectivity in single-atom catalysts (SACs) based peroxymonosulfate (PMS) systems were investigated using experimental and theoretical approaches. The results showed that pollutants with high redox potential were primarily degraded by free radicals, while pollutants with low redox potential were predominantly degraded through the nonradical electron transfer pathway (ETP). Furthermore, the contribution of radical and nonradical pathways could be controlled by the loading of PMS.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Renfeng Huang et al.
Summary: In this study, the effect of pollutant electron property on the peroxymonosulfate (PMS) activation mechanism was investigated using manganese dioxide octahedral molecular sieve (Mn-OMS) as the catalyst. The degradation of electron-rich pollutants was found to rely on catalyst-mediated electron transfer, while the removal of electron-poor pollutants depended on singlet oxygen and/or radicals. This work provides mechanistic insights into the effect of pollutants type on PMS activation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Engineering, Environmental
Liwei Yang et al.
Summary: In this study, Fe-based graphite catalyst (Fe-0.6@N-GC) was successfully synthesized for the degradation of sulfisoxazole (SIZ) using peroxymonosulfate (PMS) activation. The Fe-0.6@N-GC catalyst showed excellent adsorption capacity for SIZ and complete degradation of SIZ could be achieved within 20 minutes. The study also provided insights into the nonradical pathways of organic pollutants oxidation by iron-based catalysts.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Engineering, Environmental
Chiheng Chu et al.
Summary: The study introduces a highly efficient peroxide-activation catalyst composed of pyridine-coordinated Co single atoms embedded in a polyaromatic macrostructure. The catalyst demonstrates rapid removal of environmental pollutants and shows a significantly higher turnover frequency compared to benchmark catalysts. Experiment results and density functional theory simulation suggest that the unique structure and electronic interaction of the catalyst contribute to its effectiveness in peroxide precursor activation.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Engineering, Environmental
Penghui Shao et al.
Summary: Experimental and theoretical studies show that the activity of nanodiamonds is influenced by the degree of graphitization, with intensified surface graphitization altering the degradation mechanism. A self-constructed time-resolved phosphorescence detection system was used for the first time to provide direct evidence of singlet oxygen production in the PMS-based system.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Engineering, Environmental
Kun Qian et al.
Summary: In this study, FeN4 structures were constructed on carbon nanotubes to obtain single-atom catalysts, which successfully generated reactive iron species (RFeS) for the selective degradation of emerging organic contaminants (EOCs) over a wide pH range. The results revealed the mechanism of RFeS generation and the important role of carbon nanotubes in enhancing the reactivity of FeN4=O intermediates.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Multidisciplinary Sciences
Dongpeng Zhang et al.
Summary: Surface substitutional doping with Pt has significant effects on the electronic and surface characteristics of atomically thin layers of Bi3O4Br, enhancing the generation of O-1(2). The introduced Pt impurity states can trap photoinduced singlet excitons, reducing the singlet-triplet energy gap and facilitating the generation of triplet excitons. Chemisorption state of O-2 causes changes in the magnetic moment of O-2 through electron-mediated triplet energy transfer, resulting in specific O-1(2) generation.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Engineering, Environmental
Yangke Long et al.
Summary: Pollutant degradation via IO4--based AOPs can be optimized using single-atomic metal activation, as demonstrated by the successful activation of IO4- for organic pollutant degradation using N-rGO-CoSA activators. The efficient activation process is mediated by Co-N coordination sites and the conductive graphene matrix, enhancing the overall oxidation capacity.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Long-Shuai Zhang et al.
Summary: A novel catalyst Fe-1/CN was developed to achieve 100% selective production of O-1(2) through activation of PMS, enabling highly selective and efficient degradation of organic pollutants.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yun Gao et al.
Summary: A series of carbon-supported atomic metal-N-C catalysts were synthesized to investigate their catalytic activity trends and mechanisms, with Fe-SAC demonstrating the best catalytic performance for organic pollutant degradation. The study provides atomic-scale understanding of catalytic trends and mechanisms for PMS-assisted reactive oxygen species production via M-SACs, guiding the development of efficient catalytic materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Lijng Peng et al.
Summary: Enteromorpha, a seawater pollutant, was converted into a functional carbocatalyst for Fenton-like reactions. The Enteromorpha-derived Fe-N-C exhibited high activity in activating peroxymonosulfate for organic pollutant degradation. Single Fe atoms played a crucial role as dominant reactive sites in forming highly oxidizing Fe-IV=O and Fe-V=O species.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Jie Miao et al.
Summary: Transition metal catalysts anchored on carbon nanotubes were developed to efficiently activate peroxymonosulfate for nonradical oxidation. The study found that the spin state of the catalyst strongly influenced its catalytic activity, with higher spin states promoting electron transfer and enhancing the oxidation capacity of reactive species. These findings advance the mechanistic understanding of transition metal-mediated persulfate activation and contribute to the development of efficient spintronic catalysts for environmental applications.
Review
Chemistry, Multidisciplinary
Yanan Shang et al.
Summary: Carbon-based single atom catalysts show high performances and efficiency in environmental catalysis, but there is a lack of comprehensive research on their catalytic sites and mechanisms in advanced oxidation processes, which is necessary for further exploration.
CHEMICAL SOCIETY REVIEWS
(2021)
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(2020)
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2019)
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2019)
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Wen Liu et al.
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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
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ADVANCED FUNCTIONAL MATERIALS
(2018)
Review
Chemistry, Multidisciplinary
Lichen Liu et al.
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(2018)
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(2017)
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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(2015)