Oxygen-defective MnO2−x rattle-type microspheres mediated singlet oxygen oxidation of organics by peroxymonosulfate activation

Yu, Jie; Zeng, Tao; Wang, He; Zhang, Hui; Sun, Yanping; Chen, Lei; Li, Lingxiangyu; Shi, Huixiang

doi:10.1016/j.cej.2020.124458

Cited by 99 publications

(34 citation statements)

References 88 publications

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“…The latter is consistent with the spectrum of Mn 3+ oxidation states of Mn as reported in [62]. Three peaks with binding energies of 640.7 eV, 641.7 eV and 643.6 eV were fitted for the Mn 2p3/2 spectrum, corresponding to Mn 2+ , Mn 3+ and Mn 4+ , respectively [63], the relative intensities of which were 23:57:20 in fresh Mn 2 O 3 . After the reactions, the relative intensities of Mn 2+ /Mn 3+ /Mn 4+ changed to 22:44:34, which suggests that redox reactions between the Mn 2+ /Mn 3+ /Mn 4+ occurred during the PMS activation process.…”

Section: Roles Of Manganese and Oxygen Speciessupporting

confidence: 88%

A Comprehensive Assessment of Catalytic Performances of Mn2O3 Nanoparticles for Peroxymonosulfate Activation during Bisphenol A Degradation

Chen

Hou

et al. 2021

Catalysts

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Catalytic performances of Mn2O3 nanoparticles for peroxymonosulfate (PMS) activation in bisphenol A (BPA) degradation were comprehensively investigated in this study. Experimental results showed that 10 mg/L BPA could be 100% degraded within 20 min with the dosages of 0.2 g/L Mn2O3 and 0.1 mM PMS. Moreover, Mn2O3 showed remarkable activity in activation of PMS and excellent adaptability in various real water matrices, including river water, tap water and secondary effluents. Based on the radical detection and scavenging experiments, it was found that both radical and non-radical oxidation contributed to the degradation of BPA and 1O2 was the dominant species in the degradation compared to •OH, SO4•− and O2•−. A total of 15 transformation products were identified by LC/MS-MS during BPA degradation in the Mn2O3/PMS system, and degradation pathways via three routes are proposed. Compared with lab-made catalysts reported in the literature, the Mn2O3 catalyst demonstrated its superiority in terms of its high TOC removal, low PMS consumption and fast degradation rate for BPA.

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Section: Roles Of Manganese and Oxygen Speciessupporting

confidence: 88%

A Comprehensive Assessment of Catalytic Performances of Mn2O3 Nanoparticles for Peroxymonosulfate Activation during Bisphenol A Degradation

Chen

Hou

et al. 2021

Catalysts

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“…107 Furthermore, introducing vacancies into a crystal plane can also optimize the catalytic reactivity. Shi et al 108 reported that PMS adsorption on intact δ-MnO 2 (001) was undesirable as an endothermic reaction (E ads = 1.24 eV). A moderate population of O vacancies on MnO 2 (001) was helpful to PMS adsorption (E ads = −1.53 eV) and dissociation (Figure 16a,b,d,e,g,h).…”

Section: Transition Metals and Metalmentioning

confidence: 99%

“…DFT dynamic simulations revealed that the O vacancy could accommodate one O atom of the peroxy-bond in PMS, leading Nevertheless, overabundant O vacancies were not beneficial for PMS activation as more O vacancies would result in strong attractions to PMS, which would prohibit PMS dissociation and radical generation (Figure 16c,f,i). 108 Based on the above research, the introduction of another kind of metal with a different electronegativity or a small content of vacancies in transition metals and metal oxides is a feasible way to increase the area of active sites in persulfate activation, which can optimize the local charge distribution and the interaction between catalysts and persulfate. This quickens persulfate activation.…”

Section: Transition Metals and Metalmentioning

confidence: 99%

Density Functional Theory Calculations for Insight into the Heterocatalyst Reactivity and Mechanism in Persulfate-Based Advanced Oxidation Reactions

et al. 2021

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Advanced oxidation processes (AOPs) based on persulfates such as peroxymonosulfate and peroxydisulfate via heterogeneous catalysts have been a research hotspot due to their outstanding performances in removing emerging organic contaminants (OCs). In this Review, we highlight the recent advances in theoretical simulations for persulfate-based AOPs (PS-AOPs) using density functional theory (DFT), with the emphasis on the catalyst properties and the mechanism of persulfate activation over a variety of heterogeneous catalysts (including nanocarbons, metals, and metal oxides). Moreover, the properties of OCs and their degradation mechanism by diverse reactive oxygen species investigated by theoretical computations are also summarized. The descriptors in computational studies and the related structure−performance relationships are discussed. Finally, the challenges and future research focuses of DFT simulations in PS-AOPs are proposed, including the evaluation of catalyst properties, elucidation of the persulfate activation mechanism, especially the nonradical pathway, and the rational design of on-demand catalysts.

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“…Oxygen vacancies could be important active site for Mn oxides (P3 in Figure 5 ). For instance, Jie et al manufactured the MnO 2-x rattle-type microspheres that a large number of oxygen-defective MnO 2 nanoflakes vertically arranged on the surface (OD-MnO 2-x -RM), and altered the amount of oxygen vacancies by H 2 reduction treatment for various treatment times (20, 40, 60 and 80 min) [ 115 ]. PMS was activated to form 1 O 2 due to the presence of oxygen vacancies and unique nanoarchitecture of the MnO 2-x rattle-type microspheres catalyst.…”

Section: Evolution Of 1 O 2 mentioning

confidence: 99%

Evolution of Singlet Oxygen by Activating Peroxydisulfate and Peroxymonosulfate: A Review

Xiao

Faheem

et al. 2021

IJERPH

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Advanced oxidation processes (AOPs) based on peroxydisulfate (PDS) or peroxymonosulfate (PMS) activation have attracted much research attention in the last decade for the degradation of recalcitrant organic contaminants. Sulfate (SO4•−) and hydroxyl (•OH) radicals are most frequently generated from catalytic PDS/PMS decomposition by thermal, base, irradiation, transition metals and carbon materials. In addition, increasingly more recent studies have reported the involvement of singlet oxygen (1O2) during PDS/PMS-based AOPs. Typically, 1O2 can be produced either along with SO4•− and •OH or discovered as the dominant reactive oxygen species (ROSs) for pollutants degradation. This paper reviews recent advances in 1O2 generation during PDS/PMS activation. First, it introduces the basic chemistry of 1O2, its oxidation properties and detection methodologies. Furthermore, it elaborates different activation strategies/techniques, including homogeneous and heterogeneous systems, and discusses the possible reaction mechanisms to give an overview of the principle of 1O2 production by activating PDS/PMS. Moreover, although 1O2 has shown promising features such as high degradation selectivity and anti-interference capability, its production pathways and mechanisms remain controversial in the present literatures. Therefore, this study identifies the research gaps and proposes future perspectives in the aspects of novel catalysts and related mechanisms.

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Oxygen-defective MnO2−x rattle-type microspheres mediated singlet oxygen oxidation of organics by peroxymonosulfate activation

Cited by 99 publications

References 88 publications

A Comprehensive Assessment of Catalytic Performances of Mn2O3 Nanoparticles for Peroxymonosulfate Activation during Bisphenol A Degradation

A Comprehensive Assessment of Catalytic Performances of Mn2O3 Nanoparticles for Peroxymonosulfate Activation during Bisphenol A Degradation

Density Functional Theory Calculations for Insight into the Heterocatalyst Reactivity and Mechanism in Persulfate-Based Advanced Oxidation Reactions

Evolution of Singlet Oxygen by Activating Peroxydisulfate and Peroxymonosulfate: A Review

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