4.2 Review

DFT Calculation of Nonperiodic Small Molecular Systems to Predict the Reaction Mechanism of Advanced Oxidation Processes: Challenges and Perspectives

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CHEMICAL ENGINEERING JOURNAL (2022)

Article Chemistry, Physical

Development of Atomic Hydrogen-Mediated Electrocatalytic Filtration System for Peroxymonosulfate Activation Towards Ultrafast Degradation of Emerging Organic Contaminants

Wentian Zheng et al.

Summary: A novel H*-mediated electrocatalytic filtration system was designed to achieve highly efficient degradation of emerging organic contaminants, utilizing an electroactive carbon nanotube filter functionalized with nanoscale Pd. The system demonstrated rapid degradation of sulfamethoxazole, maintained efficacy in complex matrices, and employed both radical and nonradical pathways for organic contaminant degradation.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

Article Engineering, Environmental

Efficient Degradation of Organoarsenic by UV/Chlorine Treatment: Kinetics, Mechanism, Enhanced Arsenic Removal, and Cytotoxicity

Tao Yang et al.

Summary: ROX can be efficiently degraded by UV/chlorine, with the highest degradation rate at pH 7.5, and over 98% of total As can be removed by ferrous after UV/chlorine treatment; cytotoxicity significantly increases during the degradation of ROX, but can be greatly reduced by the combination of UV/chlorine and adsorption.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2021)

Article Engineering, Environmental

Consolidated 3D Co3Mn-layered double hydroxide aerogel for photo-assisted peroxymonosulfate activation in metronidazole degradation

Shaoxiong He et al.

Summary: The novel 3D Co3Mn-layered double hydroxide aerogel (Co3Mn-LDH/rGA) was synthesized for the degradation of aqueous metronidazole (MTZ) with the assistance of photo-activated peroxymonosulfate (PMS). The study showed that Co3Mn-LDH/rGA aerogel exhibited high efficiency in MTZ removal and excellent reusability. The research provided insights into the reaction mechanism of visible light-assisted PMS activation and offered a promising method for continuous pollutant degradation.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Insights into catalytic activation of peroxymonosulfate for carbamazepine degradation by MnO2 nanoparticles in-situ anchored titanate nanotubes: Mechanism, ecotoxicity and DFT study

Fei Pan et al.

Summary: This study successfully degraded and mineralized CBZ using AMnTi composite material, increasing the degradation rate of CBZ. The high catalytic activity of AMnTi is attributed to its unique structure, leading to efficient charge transfer and catalytic activation through Mn-O-Ti linkage, and a Mn-Ti cycle mediating catalytic activation of PMS was discovered. Both hydroxyl and sulfate radicals played key roles in CBZ degradation.

JOURNAL OF HAZARDOUS MATERIALS (2021)

Article Environmental Sciences

Identification of photodegradation product of organophosphorus pesticides and elucidation of transformation mechanism under simulated sunlight irradiation

Luning Lian et al.

Summary: This study found that photolysis can effectively degrade organophosphorus pesticides (OPs), with chlorpyrifos and dimethoate achieving high photodegradation efficiencies under specific conditions (pH 9, xenon lamp as light source). Through experimental and theoretical exploration, the photodegradation mechanisms of chlorpyrifos and dimethoate were revealed.

ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY (2021)

Article Engineering, Environmental

Correlation of Active Sites to Generated Reactive Species and Degradation Routes of Organics in Peroxymonosulfate Activation by Co-Loaded Carbon

Ning Li et al.

Summary: This study investigated the correlation between different active sites in Co-PCN catalysts and reactive oxygen species (ROS) during PMS-AOPs for organic degradation. The findings provided new insights into the reaction mechanisms in PMS-AOP systems and the rational design of catalysts for ROS-oriented degradation of pollutants.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2021)

Article Engineering, Environmental

Degradation of acetaminophen by activated peroxymonosulfate using Co (OH)2 hollow microsphere supported titanate nanotubes: Insights into sulfate radical production pathway through CoOH+ activation

Long Chen et al.

Summary: In this study, CoM/TNTs composites were synthesized and successfully activated PMS for efficient removal of ACE in water. The synergetic effect of Co (OH) (+) from CoM and TNTs promoted PMS activation, leading to the degradation of ACE. The study provided insights into radical production and organics attack mechanisms in cobalt-based PMS activation system.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Full insights into the roles of pH on hydroxylation of aromatic acids/bases and toxicity evaluation

Zexiu An et al.

Summary: This study investigated the mechanistic and kinetic insights into the roles of pH on the hydroxylation of five aromatic acids and bases in UV/H2O2 process. The reactivity of center dot OH towards the species is positively correlated with electron-donating effect of substituents, contributing to the positively pH-dependent reactivity of aromatic acids and bases. The optimal degradation pH values are around 5.5 to 7.5.

WATER RESEARCH (2021)

Article Engineering, Environmental

Exploring key reaction sites and deep degradation mechanism of perfluorooctane sulfonate via peroxymonosulfate activation under electrocoagulation process

Meng Li et al.

Summary: The study successfully utilized the EC technique coupled with PMS activation to deeply degrade PFOS, achieving a removal rate of approximately 100% within 60 minutes with a high kinetic rate. The energy consumption was significantly lower than that of traditional electrodes, confirming the potential application prospects of the EC technique. The results provide a novel alternative for the high-effective treatment of PFOS in contaminated environmental water bodies.

WATER RESEARCH (2021)

Article Chemistry, Physical

Mechanistic insight into the reaction pathway of peroxomonosulfate-initiated decomplexation of EDTA-NiII under alkaline conditions: Formation of high-valent Ni intermediate

Sheng Liang et al.

Summary: This study investigates the reaction mechanism of peroxomonosulfate (PMS) with ethylenediaminetetraacetic acid (EDTA)-NiII under alkaline conditions through experimental tests and density functional theory (DFT) calculations. Experimental evidence shows that PMS can successfully decomplex EDTA-NiII and form Ni hydroxide precipitates at alkaline pH, leading to a significant reduction in aqueous Ni concentration. The proposed alternative reaction pathway suggests that NiII is attacked by PMS to produce high-valent Ni species, which further self-decomplex to NiIII hydroxides, indicating the involvement of NiIV species as a viable redox pathway promoting decomplexation.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

Article Engineering, Environmental

Catalyst-free activation of permanganate under visible light irradiation for sulfamethazine degradation: Experiments and theoretical calculation

Chen Zhang et al.

Summary: This study utilized visible light to activate permanganate for the degradation of sulfamethazine, demonstrating the effective degradation of SMT in the VL/PM system. Factors influencing degradation and degradation mechanisms were investigated through experiments and Density Functional Theory calculations.

WATER RESEARCH (2021)

Article Engineering, Environmental

Mechanistic insights into paracetamol transformation in UV/NH2 Cl process: Experimental and theoretical study

Pin Wang et al.

Summary: This study combined theoretical calculations and experimental studies to investigate the kinetics and mechanism of radical-mediated degradation of paracetamol in the UV/monochloramine process, providing deep insights into the degradation mechanism. The study identified the impact factors and reaction mechanisms of various radicals on the degradation of paracetamol, enriching the understanding of the paracetamol degradation mechanism.

WATER RESEARCH (2021)

Article Chemistry, Physical

Degradation of benzophenone-4 by peroxymonosulfate activated with microwave synthesized well-distributed CuBi2O4 microspheres: Theoretical calculation of degradation mechanism

Yiping Wang et al.

Summary: This study found that well-distributed CuBi2O4 microspheres with active sites and hydroxyl groups on the surface can effectively activate PMS to degrade BP-4. The degradation mechanism of BP-4 was proposed through theoretical calculations and intermediates identification, showing that radical addition reaction is the main pathway for BP-4 oxidation.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

Article Engineering, Environmental

Resistance of alkyl chloride on chloramphenicol to oxidative degradation by sulfate radicals: Kinetics and mechanism

Ying Xue et al.

Summary: This study evaluated the degradation and dechlorination processes of chloramphenicol through the generation of sulfate radicals, indicating that chloramphenicol is degraded mainly by destroying its carbon moiety rather than complete mineralization. The dechlorination on the side chain of the benzene ring was found to be more difficult than that directly on the benzene ring, suggesting that organic pollutants containing chlorine atoms on the side chain may be more resistant to oxidative attack and require more attention.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Further understanding the role of hydroxylamine in transformation of reactive species in Fe(II)/peroxydisulfate system

Zhuo-Yu Li et al.

Summary: Hydroxylamine has been found to transform Fe(IV) into radicals (SO4 center dot- and center dot OH) during potential pollutants oxidation in Fe(II)/hydroxylamine/PDS system. Experimental results indicate that hydroxylamine promotes the production of SO4 center dot- significantly, while inhibiting the production of Fe(IV) as its concentration increases from 0.2 to 1.4 mM.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Confined Fe0@CNTs for highly efficient and super stable activation of persulfate in wide pH ranges: Radicals and non-radical co-catalytic mechanism

Pei Su et al.

Summary: Efficient catalysis in a wide range of pH values remains a major challenge in advanced oxidation processes. This study successfully fabricated confined nano-Fe-0 in carbon nanotubes as a heterogeneous catalyst for persulfate activation, showing exceptional catalytic performance across a wide range of pH values with low leaching iron and improved reusability. This confinement effect on Fe-0-in-CNTs was effective for degrading multiple pollutants and activating other oxidants, representing a significant breakthrough in AOPs.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Multiple catalytic reaction sites induced non-radical/radical pathway with graphene layers encapsulated Fe-N-C toward highly efficient peroxymonosulfate (PMS) activation

Zhiyan Huang et al.

Summary: This study investigated the high activity of graphene layers encapsulated Fe-N-C catalysts in Fenton-like reaction. The Fe2Mn1-Fe@NCs catalyst showed the optimal catalytic degradation performance, with pyrrolic N and Fe-pyridinic N-C playing important roles in promoting the catalytic degradation. The findings provide insights for the design of other Fe-N-C catalysts and efficient organic pollution remediation.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Engineering, Environmental

Facile construction of 2D g-C3N4 supported nanoflower-like NaBiO3 with direct Z-scheme heterojunctions and insight into its photocatalytic degradation of tetracycline

Yixiao Wu et al.

Summary: The composite photocatalyst g-C3N4/NaBiO3 showed superior performance in degrading tetracycline compared to individual g-C3N4 or NaBiO3, attributed to the accumulation of photoinduced electrons on g-C3N4 and holes on NaBiO3 for efficient generation of superoxide and hydroxyl radicals. The built-in electric field between g-C3N4 and NaBiO3 enhanced charge separation, leading to stable photodegradation activity for multiple cycles. This work not only provides a promising photocatalyst for antibiotic contaminants, but also sheds light on the photocatalytic removal of tetracycline.

JOURNAL OF HAZARDOUS MATERIALS (2021)

Article Engineering, Environmental

Motivation of reactive oxidation species in peracetic acid by adding nanoscale zero-valent iron to synergic removal of spiramycin under ultraviolet irradiation: Mechanism and N-nitrosodimethylamine formation potential assessment

Lin Wang et al.

Summary: The study demonstrates that the addition of nanoscale zero-valent iron (nZVI) to peracetic acid (PAA) mixture under ultraviolet (UV) irradiation can significantly enhance the removal of spiramycin and reduce the formation potential of N-nitrosodimethylamine (NDMA). The mechanism involves the generation of hydroxyl radicals and carbon-centered radicals, with a critical role played by Fe2+ released from nZVI. The stability of nZVI in the system allows for effective reuse in the removal process, making the nZVI/UV/PAA process a promising advanced oxidation technology for water treatment.

WATER RESEARCH (2021)

Article Engineering, Environmental

Molybdenum disulfide (MoS2): A novel activator of peracetic acid for the degradation of sulfonamide antibiotics

Jingwen Wang et al.

Summary: In this study, a novel advanced oxidation process using MoS2/PAA was applied to degrade sulfonamide antibiotics (SAs), with sulfamethoxazole (SMX) as the target SA. Results showed that under optimum pH conditions, the degradation efficiency of SMX exceeded 80% after 15 minutes of reaction. Increasing the dosages of PAA or MoS2 facilitated SMX degradation, while the presence of humic acids slowed down the removal of SMX.

WATER RESEARCH (2021)

Article Engineering, Environmental

Fe2+/HClO Reaction Produces FeIVO2+: An Enhanced Advanced Oxidation Process

Sheng Liang et al.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2020)

Article Engineering, Environmental

Piezo-activation of peroxymonosulfate for benzothiazole removal in water

Shenyu Lan et al.

JOURNAL OF HAZARDOUS MATERIALS (2020)

Article Engineering, Environmental

Sulfate radical induced catalytic degradation of metolachlor: Efficiency and mechanism

Chao Liu et al.

CHEMICAL ENGINEERING JOURNAL (2019)

Article Engineering, Environmental

Reactive Nitrogen Species Are Also Involved in the Transformation of Micropollutants by the UV/Monochloramine Process

Zihao Wu et al.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2019)

Article Engineering, Environmental

Degradation of Perfluorooctanesulfonate by Reactive Electrochemical Membrane Composed of Magneli Phase Titanium Suboxide

Huanhuan Shi et al.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2019)

Article Environmental Sciences

OH-initiated transformation and hydrolysis of aspirin in AOPs system: DFT and experimental studies

Lin He et al.

SCIENCE OF THE TOTAL ENVIRONMENT (2017)

Article Chemistry, Physical

Comparing Methods for Predicting the Reactive Site of Electrophilic Substitution

Fu Rong et al.

ACTA PHYSICO-CHIMICA SINICA (2014)

Article Biochemical Research Methods

Quantitative analysis of molecular surface based on improved Marching Tetrahedra algorithm

Tian Lu et al.

JOURNAL OF MOLECULAR GRAPHICS & MODELLING (2012)

Article Chemistry, Multidisciplinary

ATOMIC DIPOLE MOMENT CORRECTED HIRSHFELD POPULATION METHOD

Tian Lu et al.

JOURNAL OF THEORETICAL & COMPUTATIONAL CHEMISTRY (2012)

Review Chemistry, Physical

Comparison of Computational Methods for Atomic Charges

Lu Tian et al.

ACTA PHYSICO-CHIMICA SINICA (2012)

Article Chemistry, Multidisciplinary

The electrostatic potential: an overview

Jane S. Murray et al.

WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE (2011)

Article Biochemistry & Molecular Biology

Average local ionization energy: A review

Peter Politzer et al.

JOURNAL OF MOLECULAR MODELING (2010)

Review Chemistry, Physical

Conceptual Density Functional Theory and Some Recent Developments

Liu Shu-Bin

ACTA PHYSICO-CHIMICA SINICA (2009)

Article Chemistry, Physical

New dual descriptor for chemical reactivity

C Morell et al.

JOURNAL OF PHYSICAL CHEMISTRY A (2005)

Article Multidisciplinary Sciences

Information theory, atoms in molecules, and molecular similarity

RF Nalewajski et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2000)