Nuclear Density Functional Theory Research Articles

Nuclear Magnetic Resonance (NMR) and Density Functional Theory (DFT) Study of Water Clusters of Hydrogen-Rich Water (HRW)

The present study investigated the 1H Nuclear Magnetic Resonance (NMR) spectra of hydrogen-rich water (HRW) produced using the EVObooster device. The analyzed HRW has pH = 7.1 ± 0.11, oxidation–reduction potential (ORP) of (−450 ± 11) mV, and a dissolved hydrogen concentration of 1.2 ppm. The control sample was tap water filtered by patented technology. A 600 NMR spectrometer was used to measure NMR spectra. Isotropic 1H nuclear magnetic shielding constants of the most stable clusters (H2O)n with n from 3 to 28 have been calculated by employing the gauge-including-atomic-orbital (GIAO) method at the MPW1PW91/6-311+G(2d,p) density function level of theory (DFT). The HRW chemical shift is downfield (higher chemical shifts) due to increased hydrogen bonding. More extensive formations were formed in HRW than in control filtered tap water. The exchange of protons between water molecules is rapid in HRW, and the 1H NMR spectra are in fast exchange mode. Therefore, we averaged the calculated chemical shifts of the investigated water clusters. As the size of the clusters increases, the number of hydrogen bonds increases, which leads to an increase in the chemical shift. The dependence is an exponential saturation that occurs at about N = 10. The modeled clusters in HRW are structurally stabilized, suggesting well-ordered hydrogen bonds. In the article, different processes are described for the transport of water molecules and clusters. These processes are with aquaporins, fusion pores, gap-junction channels, and WAT FOUR model. The exponential trend of saturation shows the dynamics of water molecules in clusters. In our research, the chemical shift of 4.257 ppm indicates stable water clusters of 4–5 water molecules. The pentagonal rings in dodecahedron cage H3O+(H2O)20 allow for an optimal arrangement of hydrogen bonds that minimizes the potential energy.

Stereoselective synthesis of geminal bromofluoroalkenes by kinetically controlled selective conversion of oxaphosphetane intermediates.

Geminal bromofluoroalkenes are an important subclass of versatile organic interhalide, which can serve as useful synthetic precursors to monofluoroalkenes that are valuable amide group isosteres. Nonetheless, despite the vast advancement of olefination methodologies, the broadly applicable stereoselective synthesis remained elusive for geminal bromofluoroalkenes before our work. In particular, the seemingly straightforward Wittig-type approach with interhalogenated phosphorus ylide has been unsuccessful because of the difficulty in the diastereoselective oxaphosphetane formation. Here, we describe a conceptually distinctive strategy, by which the stereoselectivity is gained via the selective decomposition of the oxaphosphetane intermediates. The suitably identified phosphorus(III) reagent and reaction medium enabled efficient kinetic differentiation, which was supported by nuclear magnetic resonance analysis and density functional theory calculation. Through our method, the highly diastereoselective synthesis of geminal E-bromofluoroalkenes was accomplished in one step. Furthermore, the generality was demonstrated by accommodating a wide range of readily available carbonyl compounds, including ketones and pharmaceutical substrates.

Highly selective and sensitive N-amidothiourea-based fluorescence chemosensor for detecting Zn2+ ions and cell Imaging: Potential applications for plasma membrane detection

A “turn-on” fluorescent sensor L was developed for the selective detection of Zn2+ ions in biological settings. This sensor exhibited a specific response to Zn2+ ions, with a detection limit of 39 nM. Analyses through titration and Job’s plot confirmed that the formed complex has a 2:1 stoichiometry (L: Zn2+). The sensor displayed strong selectivity for Zn2+ over other metal ions, demonstrating a robust binding affinity while effectively reducing interference from heavy metals. The identification process was validated by Fourier transform infrared spectroscopy (FT-IR), proton nuclear magnetic resonance (1H NMR) titrations, mass spectrometry (MS), and Density Functional Theory (DFT) calculations. Maximum fluorescence intensity was achieved upon interaction with Zn2+ ions within a physiological pH range of 7.0–7.5. Moreover, successful imaging experiments in HEK293 cells highlighted the sensor’s potential as a powerful tool for monitoring interactions at the plasma membrane.

Synthesis and characterization of a chiral spirobifluorene cyclic hexamer

Abstract A new chiral macrocycle 1-[6], consisting of six chiral spirobifluorene units linked in a cyclic arrangement, was successfully synthesized via a homo-coupling of the corresponding acyclic trimer. Notably, this chiral cyclic hexamer exhibited flexibility in solution, and both low-temperature nuclear magnetic resonance (NMR) experiments and density functional theory (DFT) calculations suggest that its stable structure is not the hexagonal D6-symmetric structure but rather the figure-eight-shaped D2-symmetric structure. In this D2-symmetric structure, the opposing bifluorenyl units are π-stacked, and it is suggested that this π-stacked region undergoes rapid dissociation and reformation at room temperature. The HOMO is distributed over the π-stacked region, with a HOMO-LUMO gap of 4.02 eV. The macrocycle exhibited strong violet fluorescence. The absorption dissymmetry factor |gabs| was 7.4 × 10−3, which is larger compared to the series of chiral smaller macrocycles 1-[n] (n = 3 to 5). Additionally, the CPL efficiency, indicated by a BCPL value of 189 M−1 cm−1, is relatively high among chiral organic luminescent molecules.

Extended Fayans energy density functional: optimization and analysis

The Fayans energy density functional (EDF) has been very successful in describing global nuclear properties (binding energies, charge radii, and especially differences of radii) within nuclear density functional theory. In a recent study, supervised machine learning methods were used to calibrate the Fayans EDF. Building on this experience, in this work we explore the effect of adding isovector pairing terms, which are responsible for different proton and neutron pairing fields, by comparing a 13D model without the isovector pairing term against the extended 14D model. At the heart of the calibration is a carefully selected heterogeneous dataset of experimental observables representing ground-state properties of spherical even–even nuclei. To quantify the impact of the calibration dataset on model parameters and the importance of the new terms, we carry out advanced sensitivity and correlation analysis on both models. The extension to 14D improves the overall quality of the model by about 30%. The enhanced degrees of freedom of the 14D model reduce correlations between model parameters and enhance sensitivity.

Quasi-particle–vibration coupling approach for nuclear β-decay

The study of β-decay is important to answer open questions in physics and astrophysics; however, theoretical predictions of the associated half-lives are still plagued by uncertainties. In this short review, we argue that a reliable model for this study is nuclear density functional theory (DFT), complemented by further specific correlations; the quasi-particle–vibration coupling (QPVC) model has been successful in predicting half-lives in a number of spherical nuclei, and its extension to deformed systems should be envisioned. Some remaining open questions are addressed.

Capturing Mercury-197m/g for Auger Electron Therapy and Cancer Theranostic with Sulfur-Containing Cyclen-Based Macrocycles.

The interest in mercury radioisotopes, 197mHg (t1/2 = 23.8 h) and 197gHg (t1/2 = 64.14 h), has recently been reignited by the dual diagnostic and therapeutic nature of their nuclear decays. These isotopes emit γ-rays suitable for single photon emission computed tomography imaging and Auger electrons which can be exploited for treating small and metastatic tumors. However, the clinical utilization of 197m/gHg radionuclides is obstructed by the lack of chelators capable of securely binding them to tumor-seeking vectors. This work aims to address this challenge by investigating a series of chemically tailored macrocyclic platforms with sulfur-containing side arms, namely, 1,4,7,10-tetrakis[2-(methylsulfanyl)ethyl]-1,4,7,10-tetraazacyclododecane (DO4S), 1,4,7-tris[2-(methylsulfanyl)ethyl]-1,4,7,10-tetraazacyclododecane (DO3S), and 1,7-bis[2-(methylsulfanyl)ethyl]-1,4,7,10-tetraazacyclododecane-4,10-diacetic acid (DO2A2S). 1,4,7,10-Tetrazacyclododecane-1,4,7,10-tetracetic acid (DOTA), the widest explored chelator in nuclear medicine, and the nonfunctionalized backbone 1,4,7,10-tetrazacyclododecane (cyclen) were considered as well to shed light on the role of the sulfanyl arms in the metal coordination. To this purpose, a comprehensive experimental and theoretical study encompassing aqueous coordination chemistry investigations through potentiometry, nuclear magnetic resonance (NMR) spectroscopy, X-ray crystallography, and density functional theory (DFT) calculations, as well as concentration- and temperature-dependent [197m/gHg]Hg2+ radiolabeling and in vitro stability assays in human serum was conducted. The obtained results reveal that the investigated chelators rapidly complex Hg2+ in aqueous media, forming extremely thermodynamically stable 1:1 metal-to-ligand complexes with superior stabilities compared to those of DOTA or cyclen. These complexes exhibited 6- to 8-fold coordination environments, with donors statically bound to the metal center, as evidenced by the presence of 1H-199Hg spin-spin coupling via NMR. A similar octacoordinated environment was also found for DOTA in both solution and solid state, but in this case, multiple slowly exchanging conformers were detected at ambient temperature. The sulfur-rich ligands quantitatively incorporate cyclotron-produced [197m/gHg]Hg2+ under relatively mild reaction conditions (pH = 7 and T = 50 °C), with the resulting radioactive complexes exhibiting decent stability in human serum (up to 75% after 24 h). By developing viable chelators and understanding the impact of structural modifications, our research addresses the scarcity of suitable chelating agents for 197m/gHg, offering promise for its future in vivo application as a theranostic Auger-emitter radiometal.

Nuclear charge radii of germanium isotopes around N = 40

Collinear laser spectroscopy measurements were performed on 68−74Ge isotopes (Z=32) at ISOLDE-CERN, by probing the 4s24p2P13→4s24p5sP1o3 atomic transition (269 nm) of germanium. Nuclear charge radii are determined via the measured isotope shifts, revealing a larger local variation than the neighboring isotopic chains. Nuclear density functional theory with the Fayans functionals Fy(Δr,HFB) and Fy(IVP), and the SV-min Skyrme describes the experimental data for the differential charge radii δ〈r2〉 and charge radii Rc within the theoretical uncertainties. The observed large variation in the charge radii of germanium isotopes is better accounted for by theoretical models incorporating ground state quadrupole correlations. This suggests that the polarization effects due to pairing and deformation contribute to the observed large odd-even staggering in the charge radii of the Ge isotopic chain.

Zirconium-Based Metal-Organic Frameworks with Free Hydroxy Groups for Enhanced Perfluorooctanoic Acid Uptake in Water.

Perfluorooctanoic acid (PFOA) is a highly recalcitrant organic pollutant, and its bioaccumulation severely endangers human health. While various methods are developed for PFOA removal, the targeted design of adsorbents with high efficiency and reusability remains largely unexplored. Here the rational design and synthesis of two novel zirconium-based metal‒organic frameworks (MOFs) bearing free ortho-hydroxy sites, namely noninterpenetrated PCN-1001 and twofold interpenetrated PCN-1002,are presented. Single crystal analysis of the pure ligand reveals that intramolecular hydrogen bonding plays a pivotal role in directing the formation of MOFs with free hydroxy groups. Furthermore, the transformation from PCN-1001 to PCN-1002 is realized. Compared to PCN-1001, PCN-1002 displays higher chemical stability due to interpenetration, thereby demonstrating an exceptional PFOA adsorption capacity of up to 632mgg-1 (1.53mmolg-1), which is comparable to the reported record values. Moreover, PCN-1002 shows rapid kinetics, high selectivity, and long-life cycles in PFOA removal tests. Solid-state nuclear magnetic resonance results and density functional theory calculations reveal that multiple hydrogen bonds between the free ortho-hydroxy sites and PFOA, along with Lewis acid-base interaction, work collaboratively to enhance PFOA adsorption.

A novel red-to-near-infrared AIE fluorescent probe for detection of Hg2+ with large Stokes shift in plant and living cells

Due to the highly toxic nature of mercury ions to living organisms, accurately detecting Hg2+ in water samples and biological systems is of great significance. In this study, we designed and synthesized a novel red-to-near-infrared Aggregation-Induced Emission (AIE) fluorescent probe (named as DS) based Fluorene derivatives on specifically for Hg2+ detection. Probe DS can visually identify Hg2+ through an red-to-near-infrared fluorescence enhancement change, characterized by a large Stokes shift (130 nm) and AIE feature. This probe offers a fast response, high selectivity and sensitivity. The Hg2+-induced deprotection reaction of the thioketal mechanism was thoroughly investigated using nuclear magnetic resonance spectroscopy (NMR), mass spectrometry (MS) and density functional theory (DFT) calculation. Additionly, dynamic light scattering (DLS) results indicated that the aggregation states changes of the molecular play a crucial role in the AIE fluorescence response of probe DS toward Hg2+. The red-to-near-infrared response with AIE feature not only avoids the interference of auto-fluorescence signals in complex environments, but also reduces the fluorescence quenching caused by probe molecular aggregation. This makes probe DS highly suitable for high-quality imaging detection of Hg2+ in aqueous environments. Furthermore, probe DS demonstrates the capability for visual fluorescence detection of Hg2+ concentrations in water sample, plant roots and living cells.

Ion Dynamics at the Intermediate Charging State of the Sodium Vanadium Fluorophosphate Cathode.

Na super ionic conductor (NASICON)-type polyanionic vanadium fluorophosphate Na3V2O2(PO4)2F (NVOPF) is a promising cathode material for high-energy sodium-ion batteries. The dynamic diffusion and exchange of sodium ions in the lattice of NVOPF are crucial for its electrochemical performance. However, standard characterizations are mostly focused on the as-synthesized material without cycling, which is different from the actual battery operation conditions. In this work, we investigated the hopping processes of sodium in NVOPF at the intermediate charging state with 23Na solid-state nuclear magnetic resonance (ssNMR) and density functional theory (DFT) calculations. Our experimental characterizations revealed six distinct sodium coordination sites in the intermediate structure and determined the exchange rates among these sites at variable temperatures. The theoretical calculations showed that these dynamic processes correspond to different ion transport pathways in the crystalline lattice. Our combined experimental and theoretical study uncovered the underlying mechanisms of the ion transport in cycled NVOPF and these understandings may help the optimization of cathode materials for sodium-ion batteries.

Pillarurilarenes: Glycoluril-Expanded Pillararenes.

Glycoluril-expanded pillararenes composed of glycoluril and dialkoxybenzene units, namely, pillarurilarenes (PURA), were synthesized through a fragment coupling macrocyclization strategy. Partial replacement of dialkoxybenzene with glycoluril endows PURA with polarized equatorial methine protons for derivatization or CH-anion binding. Crystal structures of pillar[2]uril[4]arene and pillar[1]uril[4]arene containing two glycoluril units and one glycoluril unit, respectively, indicated the inward orientation of the glycoluril unit, as also suggested by 1H nuclear magnetic resonance and density functional theory calculation. This work lays a good foundation for expanding pillararenes using non-aromatic rings.

Excess properties and intermolecular interactions of 2-methoxyethanol + ethylenediamine binary system: Density, viscosity, spectral analyses, computational chemistry, and CO2 absorption property

To examine the fundamental physicochemical properties as well as intermolecular interactions for the 2-methoxyethanol (EGME) (1) + ethylenediamine (EDA) (2) binary system, this work systemically measured the density (ρ) and viscosity (η) values of the binary system with various mole ratios at P = 100.5 kPa and T = (298.15–318.15) K with the growth gap of 5 K. The as-measured values of the pure substances were compared with literature data. Multiple semi-empirical formulas were used to fit ρ and η values, and the absolute average deviations (AAD%) were calculated. After that, the excess molar volume (VmE), partial molar volume (V¯), apparent molar volume (Vφ), viscosity deviation (Δη), excess activation of Gibbs free energy (ΔG∗E), and several thermodynamic properties of the binary system were systemically analyzed. According to analysis results, it has been proven that the interaction exists between EGME and EDA molecules. And then, excess properties were fitted to the Redlich-Kister equation using multi-parametric nonlinear regression analyses, and standard deviations (σ) were calculated. In addition, based on various characterization methods including Raman, ultraviolet (UV), and nuclear magnetic resonance hydrogen (1H NMR) spectral analyses and density functional theory (DFT) calculation results, it is demonstrated that there is intermolecular hydrogen bonds in EGME (1) + EDA (2) binary system as the form of –OH⋯NH2–, which was consistent with the existence forms of intermolecular hydrogen bonds in different alcohol-amine systems from references. Finally, CO2 absorption capacity by pure EDA, pure EGME, and the EGME (1) + EDA (2) binary system were severally determined.

Quantum simulation approach to implementing nuclear density functional theory via imaginary time evolution

The quantum imaginary time evolution (QITE) algorithm is a direct implementation of the classical imaginary time evolution algorithm on quantum computer. We implement the QITE algorithm for the case of nuclear Hartree-Fock equations in a formalism equivalent to nuclear density functional theory. We demonstrate the algorithm in the case of the helium-4 nucleus with a simplified effective interaction of the Skyrme kind and demonstrate that the QITE, as implemented on simulated quantum computer, gives identical results to the classical algorithm. Published by the American Physical Society 2024

Dual channel chemosensor for successive detection of environmentally toxic Pd2+ and CN− ions and its application to cancer cell imaging

BackgroundDetecting and neutralizing Pd2+ ions are a significant challenge due to their cytotoxicity, even at low concentrations. To address this issue, various chemosensors have been designed for advanced detection systems, offering simplicity and the potential to differentiate signals from different analytes. Nonetheless, these chemosensors often suffer from limited emission response and complex synthesis procedures. As a result, the tracking and quantification of residual palladium in biological systems and environments remain challenging tasks, with only a few chemosensing probes available for commercial use. ResultsIn this paper, a straightforward approach for the selective detection of Pd2+ ions is proposed, which involves the design, synthesis, and utilization of a propargylated naphthalene-derived probe (E)-N'-((2-(prop-2-yn-1-yloxy)naphthalen-1-yl)methylene)benzohydrazide (NHP). The NHP probe exhibits sensitive dual-channel colorimetry and fluorescence Pd2+ detection over other tested metal ions. The detection process is performed through a catalytic depropargylation reaction, followed by an excited state intramolecular proton transfer (ESIPT) process, the detection limit is as low as 11.58 × 10−7 M under mild conditions. Interestingly, the resultant chemodosimeter adduct (E)-N'-((2-hydroxynaphthalen-1-yl)methylene)benzohydrazide (NHH) was employed for the consecutive detection of CN− ions, exhibiting an impressive detection limit of 31.79 × 10−8 M. Validation of both detection processes was achieved through 1H nuclear magnetic resonance and density functional theory calculations. For real-time applications of the NHP and NHH probes, smartphone-assisted detection, and intracellular detection of Pd2+ and CN− ions within HeLa cells were studied. SignificanceThis research presents a novel naphthalene derivative for visually detecting environmentally toxic Pd2+ and CN− ions. The synthesized probe selectively binds to Pd2+, forming a chemodosimeter. It successfully detects CN− ions through colorimetry and fluorimetry, offering a low detection limit and quick response. Notably, it's the first naphthalene-based small molecule to serve as a dual probe for toxic analytes - palladium and cyanide. Moreover, it effectively detects Pd2+ and CN− intracellularly in cancer cells.

Synthesis, anticancer, anti‐inflammatory, antimicrobial activities, molecular docking, and Density functional theory studies of nanometal (IV) glycoconjugates

Oxovanadium (IV) and diphenyltin (IV) complexes were synthesized on the nanoscale based on the Schiff base (H2L) derived from salicylaldehyde and d‐glucosamine. The complexes were formed with a molar ratio of 1:1 and 1:2 (metal: dligand) relative to oxovanadium (IV) and diphenyltin (IV), respectively. Fourier‐transform infrared spectroscopy, 1H and 13C nuclear magnetic resonance, mass fragmentations, electronic transitions, thermogravimetric analysis, and density functional theory were employed to validate the structure of synthesized compounds. The results demonstrated that the ligand (H2L) was successfully attached to oxovanadium (IV) and diphenyltin (IV) as di‐anionic and mono‐anionic ligands, respectively. The size of the complexes was investigated using the transmission scanning microscope. The work presents a prospective concept for the drug design of the targeted anticancer through the glucose moiety. All compounds revealed remarkable anticancer activities against the colorectal (HCT‐116) cell line, recording IC50 values 4.94, 21.73, and 62.5 μg/ml for VO (II)(L), free H2L, and Sn (ph)2(HL)2, respectively. The IC50 value of VO (II)(L) complex was increased after the quercetin inhibitor. Therefore, the sugar‐conjugated compound can be recognized by the glucose recognition binding site of GLUT and their cell‐killing effect depends highly on the GLUT inhibitor, quercetin. The potential GLUT transportability of the compounds was investigated through a molecular docking study. The anti‐migration activity was investigated for VO (II)(L) complex. The free ligand observed the best antimicrobial results. The antibacterial stimulation was investigated and represented different interaction types with the selected ribosyl transferase enzyme.

Density, viscosity, excess properties, and intermolecular interaction of propylene glycol methyl ether + 1,2-propylenediamine binary system

In this work, the systematic measurements of physicochemical properties, viz., density (ρ) and viscosity (η) values of propylene glycol methyl ether (PGME) + 1,2-propylenediamine (1,2-PDA) binary system, including pure substances, over the entire mole fraction range at the temperatures of T/K = (298.15 to 318.15) under atmospheric pressure of P = 100.5 kPa. The fundamental data were used to calculate several excess properties, including excess molar volume (VmE), viscosity deviation (Δη), and excess activation Gibbs free energy (ΔG∗E). Meanwhile, the work further investigated the values of thermal expansion coefficient (αp), partial molar volume (V¯) and apparent molar volume (Vφ), thereby offering a comprehensive understanding on non-ideal behavior of the binary system. Furthermore, the variations in ρ values with various molar ratios and temperatures were evaluated through Jouyban-Acree model and nonlinear least squares method. Simultaneously, Grunberg-Nissan model, Eyring-Margules model, Heric model, and McAllister model, were used to fit the dependence of η values on the molar ratio. Arrhenius equation was employed to fit the temperature dependency of η values. In addition, Redlich-Kister (R-K) equation was utilized to fit the VmE, Δη, and ΔG∗E values of binary system. Based on spectral analyses of Raman, ultra-violet (UV), and 1H Nuclear Magnetic Resonance (NMR) and density functional theory (DFT) calculation, the intermolecular hydrogen bond (IHB) of PGME with 1,2-PDA was discussed in depth.

Diphosphine-Protected IrAu12 Superatom with Open Site(s): Synthesis and Programmed Stepwise Assembly.

One or two phenylacetylide (PA) ligand(s) were successfully removed from the IrAu12 superatomic core of [IrAu12(dppe)5(PA)2]+ (dppe=1,2-bis(diphenylphosphino)ethane) by reaction with controlled amounts of tetrafluoroboric acid. Optical and nuclear magnetic resonance spectroscopies and density functional theory calculations revealed the formation of open Au site(s) on the IrAu12 core of [IrAu12(dppe)5(PA)1]2+ and [IrAu12(dppe)5]3+ with the remaining structure intact. Isocyanide was efficiently trapped at the open electrophilic site on [IrAu12(dppe)5(PA)1]2+, whereas a dimer or trimer of the IrAu12 superatoms was formed using diisocyanide as a linker. These results open the door to designed assembly of chemically modified metal superatoms.

Diphosphine‐Protected IrAu12 Superatom with Open Site(s): Synthesis and Programmed Stepwise Assembly

AbstractOne or two phenylacetylide (PA) ligand(s) were successfully removed from the IrAu12 superatomic core of [IrAu12(dppe)5(PA)2]+ (dppe=1,2‐bis(diphenylphosphino)ethane) by reaction with controlled amounts of tetrafluoroboric acid. Optical and nuclear magnetic resonance spectroscopies and density functional theory calculations revealed the formation of open Au site(s) on the IrAu12 core of [IrAu12(dppe)5(PA)1]2+ and [IrAu12(dppe)5]3+ with the remaining structure intact. Isocyanide was efficiently trapped at the open electrophilic site on [IrAu12(dppe)5(PA)1]2+, whereas a dimer or trimer of the IrAu12 superatoms was formed using diisocyanide as a linker. These results open the door to designed assembly of chemically modified metal superatoms.

In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations

Detoxicating materials of chemical warfare agents (CWAs) and their simulants play a critical role in reducing pollution contamination and environmental renovation. In this work, we present a simple strategy to prepare a core–shell structure Fe3O4/UiO-66-NH2/ILs@mSiO2 using hydrogen bonding association and electrostatic forces. We performed disinfection studies on dimethyl 4-nitrophenyl phosphate (DMNP) and 2-chloroethyl ethyl sulfide (2-CEES). The synergistic effects of catalytic activations for CWAs, which reduce the electron transport distance and lower the reaction energy barrier, lead to an increase in hydrolysis and Fenton-like reactions efficiency. Eliminationing tests of DMNP and 2-CEES showed that the half-lives of the degradation reactions were 128.36 and 1.12 min, respectively, and the degradation efficiency did not decrease significantly after 4 cycles. This new type of structure could be magnetically separated within 60 s to facilitate material recovery and reuse. Moreover, the presence of a mesoporous silica shell made the catalyst particles to become biocompatible and environmentally friendly. The degradation pathways of the intermediates were revealed based on nuclear magnetic resonance spectroscopy (NMR), gaschromatography-mass spectrometry (GC–MS) and density functional theory (DFT) calculations. The effective combination of catalysts provided a facile strategy for developing multi-effect synergistic catalysts for the elimination of CWAs and other pollutants.