Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

Environmental Science & Technology, Год журнала: 2023, Номер 58(4), С. 2112 - 2122

Опубликована: Дек. 26, 2023

Development of electrode materials exhibiting exceptional phosphate removal performance represents a promising strategy to mitigate eutrophication and meet ever-stricter stringent emission standards. Herein, we precisely designed novel LaCeOx heterostructure-decorated hierarchical carbon composite (L8C2PC) for high-efficiency electrosorption. This approach establishes an internal electric field within the heterostructure, where electrons transfer from Ce atoms neighboring La through superexchange interactions in La–O–Ce coordination units. The modulatory heterostructure endows positive shift d band sites increase electron density at Fermi level, promoting stronger orbital overlap binding interactions. introduction oxygen vacancies during situ nucleation process reduces kinetic barrier phosphate-ion migration supplies additional active centers. Moreover, framework ensures electrical double-layer capacitance storage interconnected ion channels. Such synergistically multiple centers grant L8C2PC with record As expected, demonstrates highest capability among reported saturation capacity 401.31 mg P g–1 dynamic 91.83 1.2 V. electrochemical system also performs well dephosphorization natural water samples low concentration that enable effluent first-class discharge standard China (0.5 L–1). study advances efficient techniques new level offers deep understanding regulates metal orbitals densities engineering.

Язык: Английский

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Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 22, 2024

Abstract The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites intensive consumption still severely restrict decontamination performance. While nanoconfinement SACs allows drastically enhanced reaction kinetics, detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment reactants, pathway shift is also an important cause for reactivity enhancement nanoconfined SACs. electronic structure cobalt site altered confining it within nanopores mesostructured silica particles, which triggers a fundamental transition singlet oxygen electron transfer 4-chlorophenol oxidation. changed accelerated interfacial mass render system up 34.7-fold higher degradation rate raised peroxymonosulfate utilization efficiency (from 61.8% 96.6%) relative unconfined control. It demonstrates superior other electron-rich phenolic compounds, good environment robustness, high stability treating real lake water. Our findings deepen knowledge catalysis may inspire innovations in low-carbon purification technologies heterogeneous applications.

Язык: Английский

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Molecular level removal of antibiotic resistant bacteria and genes: A review of interfacial chemical in advanced oxidation processes

Water Research, Год журнала: 2024, Номер 254, С. 121373 - 121373

Опубликована: Фев. 23, 2024

Язык: Английский

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Revealing the Role of Binary Distortion in PMS Activation over Spinel toward Efficient New Pollutants Removal

Advanced Functional Materials, Год журнала: 2024, Номер 34(25)

Опубликована: Фев. 16, 2024

Abstract Improving peroxymonosulfate (PMS) activation efficiency to enhance simultaneous generation of radicals and non‐radicals is essential for removing new pollutants (NPs) in complex waters. However, achieving this with standard lattice‐structured heterogeneous catalysts remains challenging due inefficient electron transfer. Here, CuCo 2 O 4 properties are successfully tuned by controlling lattice distortion, enabling PMS oxidation reduction. Unlike the slow rate transfer metal structures, highly active binary distortion alters structure distribution, exposes more Cu Co sites, lowers adsorption barriers, realizes synergistic production SO •− /•OH), 1 . The k‐value ciprofloxacin as high 17.83 min −1 M , 29.42 times higher than that non‐binary distortion. Additionally, developed intermittent reactor consistently maintains a removal above 95% over five cycles actual wastewater treatment scenarios. This work provides avenue water bodies.

Язык: Английский

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Electronic Metal‐Support Interactions Boost *OOH Intermediate Generation in Cu/In₂Se₃ for Electrochemical H₂O₂ Production

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Апрель 3, 2024

Abstract Two‐electron oxygen reduction reaction (2e − ORR) is a promising method for the synthesis of hydrogen peroxide (H 2 O ). However, high energy barriers generation key *OOH intermediates hinder process 2e ORR. Herein, we prepared copper‐supported indium selenide catalyst (Cu/In Se 3 ) to enhance selectivity and yield ORR by employing an electronic metal–support interactions (EMSIs) strategy. EMSIs‐induced charge rearrangement between metallic Cu In conducive intermediate generation, promoting H production. Theoretical investigations reveal that inclusion significantly lowers barrier impedes 4e pathway, thus favoring formation . The concentration produced Cu/In ~2 times than , shows applications in antibiotic degradation. This research presents valuable approach future utilization EMSIs

Язык: Английский

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Generating 1O2 and CoIV=O through efficient peroxymonosulfate activation by ZnCo2O4 nanosheets for pollutant control

Nano Research, Год журнала: 2024, Номер 17(9), С. 8025 - 8035

Опубликована: Июль 25, 2024

Язык: Английский

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Oxidative Polymerization in Water Treatment: Chemical Fundamentals and Future Perspectives

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 6, 2025

For several decades, the methodology of complete destruction organic pollutants via oxidation, i.e., mineralization, has been rooted in real water treatment applications. Nevertheless, this industrially accepted protocol is far from sustainable because excessive input chemicals and/or energy as well unregulated carbon emission. Recently, there have emerging studies on removal a completely different pathway, polymerization, meaning that target undergo oxidative polymerization reactions to generate polymeric products. These collectively shown compared conventional mineralization pathway allows more efficient pollutants, largely reduced chemicals, and suppressed In review, we aim provide comprehensive examination fundamentals process, current state-of-the-art strategies for regulation both kinetic thermodynamic perspectives, resource recovery formed end, limitations process pollutant are discussed, with perspectives future studies. Hopefully, review could not only critical insight advancement polymerization-oriented technologies greener manner but also stimulate paradigm innovations low-carbon treatment.

Язык: Английский

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O‐Bridged Co‐Cu Dual‐Atom Catalyst Synergistically Triggers Interfacial Proton‐Coupled Electron Transfer: A New Approach to Sustainable Decontamination

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 28, 2025

Abstract Heteroatom‐bridged dual‐atom catalysts (DACs), featuring more flexible active sites and intermetallic interaction, provide an opportunity for sustainable environmental remediation. Herein, innovative oxygen‐bridged Co‐Cu DAC supported on nano‐alumina (CoOCu‐DAC) is fabricated using a straightforward two‐step process. The as‐prepared catalyst significantly enhances both decontamination kinetics peroxymonosulfate (PMS) utilization efficiency by 1–3 orders of magnitude toward monoethanolamine (MEA, p K = 9.5) compared to Co single‐atom (Co‐SAC) bulk metal catalysts, largely outperforms previously reported systems. In‐situ ATR‐FTIR theoretical investigations reveal that the secondary introduction Cu plays multiple important roles: it activates lattice oxygen trigger key proton transfer (PT) MEAH + via nucleophilic attack at interface subsequently favors deprotonated MEA as efficient electron donor accelerate (ET) enhancing orbital overlaps co‐activation O 2 PMS. Such stepwise proton‐coupled (PCET)‐enhanced catalytic pathway mediated CoOCu‐DAC fundamentally different from common route identified in Co‐SAC‐involved Fenton‐like system. established binary QSAR further substantiates universality PCET‐enhanced strategy versatile nitrogen‐containing organic compounds. This study offers new perspective water other related areas catalysis based rationalized design multifunctional atomic level.

Язык: Английский

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The mechanism differences between sulfadiazine degradation and antibiotic resistant bacteria inactivation by iron-based graphitic biochar and peroxydisulfate system

Journal of Hazardous Materials, Год журнала: 2024, Номер 475, С. 134907 - 134907

Опубликована: Июнь 13, 2024

Язык: Английский

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Manipulating the Spin State of Spinel Octahedral Sites via a π–π Type Orbital Coupling to Boost Water Oxidation

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(37)

Опубликована: Июнь 24, 2024

Spin state is often regarded as the crucial valve to release reactivity of energy-related catalysts, yet it also challenging precisely manipulate, especially for active center ions occupied at specific geometric sites. Herein, a π-π type orbital coupling 3d (Co)-2p (O)-4f (Ce) was employed regulate spin octahedral cobalt sites (Co

Язык: Английский

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