Modulating mesoporous Co3O4 hollow nanospheres with oxygen vacancies for highly efficient peroxymonosulfate activation

Hu, Jifan; Zeng, Xiangkang; Wang, Gen; Qian, Binbin; Liu, Yue; Hu, Xiaoyun; He, Brandon; Zhang, Lian; Zhang, Xiwang

doi:10.1016/j.cej.2020.125869

Cited by 164 publications

(40 citation statements)

References 69 publications

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“…Zhang et al. discovered that Co oxide exhibited high activity to mediate PMS activation via Co (III)/Co (II) cycling . However, the existence of a rate-limiting step of high-valence metal species reduction greatly restrains the efficiency of electron transfer to PMS, which hinders the applicability of a metallic compound in PMS activation .…”

Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Sun

Zhen

et al. 2021

Environ. Sci. Technol.

328

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Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe−Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O 2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O 2 is thermodynamically enabled to capture electrons from Vo to form O 2•− under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1 O 2 . In this case, 1 O 2 and O 2•− act as the indispensable intermediate species to accelerate the circulation of O 2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nanoconfinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.

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Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Sun

Zhen

et al. 2021

Environ. Sci. Technol.

328

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“…As shown in Figures 4E and F, the amount of singlet oxygen increased with the prolonging of time under MF.W hile no hydroxyl radical was generated by d-and l-SPs (Figure S16). Notably,the singlet oxygen content generated from d-SPs was 1.5-fold higher than l-SPs.T he singlet oxygen could be generated from the reaction of O 2 via oxygen vacancy, [36] and MF promoted this reaction, [37] as described in Equation ( 1) and (2). Chiral-induced spin selectivity (CISS) effect could be the other reason that d-SPs showed better thrombolytic efficiencythan l-SPs.Due to the CISS effect, the transport of electrons was spin-dependent, and more electrons were transferred through chiral d-SPs under MF.…”

Section: Methodsmentioning

confidence: 99%

Improved Reactive Oxygen Species Generation by Chiral Co₃O₄ Supraparticles under Electromagnetic Fields

Wang

Sun

et al. 2021

Angew Chem Int Ed

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One of the most common methods to treat thromboembolism is the use of thrombolytic drugs to activate fibrinolytic protease.T he aim of this treatment was to initiate the lysis of fibrin;h owever,t here are many side-effects associated with this form of treatment. Herein, we fabricated chiral Co 3 O 4 supraparticles (SPs) with ag-factor of up to 0.02 at 550 nm and paramagnetic performance applied in the treatment of thromboembolism under an electromagnetic field (MF). In vitro experiments showed that d-SPs degraded blood clot within 8hours under MF.C ompared to l-SPs, d-SPs exhibited muchs tronger thrombolytic ability and effectively enhanced the survival rate of thrombosis model mice more than 70 %inthe 25 dofobservation. The results of mechanism study showed that under MF,t he level of reactive oxygen species (ROS) produced by d-SPs were 1.5 times higher than that of l-SPs,w hichm ight be attributed to the chiral-induced spin selectivity effects. Scheme 1. A) Illustration of chiral Co 3 O 4 SPs@PM preparation process and B) underlying mechanism of thrombolysis therapy by chiral Co 3 O 4 SPs@PM.

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“…From the quantitative perspective, radical quenching experiments and direct quantication of SO 4 c À and HOc were performed. Methanol (MeOH) and tert-butanol (TBA) are used as the radical scavengers, 20,21 and the contribution of SO 4 c À and HOc to iohexol abatement in the Cu 2 S/sulte process can be differentiated, as shown in Fig. 4(c).…”

Section: Mechanistic Insightsmentioning

confidence: 99%

Application of a novel heterogeneous sulfite activation with copper(i) sulfide (Cu₂S) for efficient iohexol abatement

Xing

Zhang

et al. 2022

RSC Adv.

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Modulating mesoporous Co3O4 hollow nanospheres with oxygen vacancies for highly efficient peroxymonosulfate activation

Cited by 164 publications

References 69 publications

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Improved Reactive Oxygen Species Generation by Chiral Co₃O₄ Supraparticles under Electromagnetic Fields

Application of a novel heterogeneous sulfite activation with copper(i) sulfide (Cu₂S) for efficient iohexol abatement

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Modulating mesoporous Co3O4 hollow nanospheres with oxygen vacancies for highly efficient peroxymonosulfate activation

Cited by 164 publications

References 69 publications

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O2) in the Fe–Co LDH/Peroxymonosulfate System

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O2) in the Fe–Co LDH/Peroxymonosulfate System

Improved Reactive Oxygen Species Generation by Chiral Co3O4 Supraparticles under Electromagnetic Fields

Application of a novel heterogeneous sulfite activation with copper(i) sulfide (Cu2S) for efficient iohexol abatement

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Resources

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Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Improved Reactive Oxygen Species Generation by Chiral Co₃O₄ Supraparticles under Electromagnetic Fields

Application of a novel heterogeneous sulfite activation with copper(i) sulfide (Cu₂S) for efficient iohexol abatement