Integrating single-cobalt-site and electric field of boron nitride in dechlorination electrocatalysts by bioinspired design

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Jan. 12, 2021

The construction of enzyme-inspired artificial catalysts with enzyme-like active sites and microenvironment remains a great challenge. Herein, we report single-atomic-site Co catalyst supported by carbon doped boron nitride (BCN) locally polarized B-N bonds (Co SAs/BCN) to simulate the reductive dehalogenases. Density functional theory analysis suggests that BCN supports, featured ionic characteristics, provide additional electric field effect compared graphitic or N-doped (CN), which could facilitate adsorption organochlorides. Consistent theoretical results, SAs/BCN delivers high activity nearly complete dechlorination (~98%) at potential -0.9 V versus Ag/AgCl for chloramphenicol (CAP), showing rate constant (k) contributed unit mass metal (k/ratio) is 4 19 times more than those SAs/CN state-of-the-art Pd/C catalyst, respectively. We show single atoms coupled host exhibit stability selectivity in CAP suppress competing hydrogen evolution reaction, endowing as candidate sustainable conversion organic chloride.

Language: Английский

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Recent progress in cathodic reduction-enabled organic electrosynthesis: Trends, challenges, and opportunities

eScience, Journal Year: 2022, Volume and Issue: 2(3), P. 243 - 277

Published: April 23, 2022

Compared with general redox chemistry, electrochemistry using the electron as a potent, controllable, yet traceless alternative to chemical oxidants/reductants usually offers more sustainable options for achieving selective organic synthesis. With its environmentally benign features gradually being uncovered and studied, electrosynthesis is currently undergoing revival becoming rapidly growing area within synthetic community. Among electrochemical transformations, anodically enabled ones have been far extensively exploited than those driven by cathodic reduction, although both approaches are conceptually attractive. To stimulate development of cathodically reactions, this review summarizes recently developed reductive electrosynthetic protocols, discussing highlighting reaction features, substrate scopes, applications, plausible mechanisms reveal recent trends in area. Herein, reduction-enabled preparative transformations categorized into four types: reduction (1) unsaturated hydrocarbons, (2) heteroatom-containing carbon-based systems, (3) saturated C-hetero or C–C polar/strained bonds, (4) hetero-hetero linkages. Apart from net electroreductive few examples photo-electrosynthesis well paired electrolysis also introduced, which offer opportunities overcome certain limitations improve versatility. The electrochemically driven, transition metal-catalyzed cross-couplings that comprehensively discussed several other reviews not included here.

Language: Английский

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Atomic Hydrogen in Electrocatalytic Systems: Generation, Identification, and Environmental Applications

Water Research, Journal Year: 2022, Volume and Issue: 223, P. 118994 - 118994

Published: Aug. 18, 2022

Language: Английский

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Evaluation of the concentration and contribution of superoxide radical for micropollutant abatement during ozonation

Water Research, Journal Year: 2021, Volume and Issue: 194, P. 116927 - 116927

Published: Feb. 15, 2021

Language: Английский

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Electrocatalytic hydro-dehalogenation of halogenated organic pollutants from wastewater: A critical review

Water Research, Journal Year: 2023, Volume and Issue: 234, P. 119810 - 119810

Published: March 1, 2023

Language: Английский

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Migration and remediation of typical contaminants in soil and groundwater: A state of art review

Land Degradation and Development, Journal Year: 2024, Volume and Issue: 35(8), P. 2700 - 2715

Published: April 3, 2024

Abstract Soil and groundwater contamination has always been a global concern. Contaminants are migrated transformed in the soil environments, which turn pose potential environmental risks to humans. This paper describes four typical contaminants, including heavy metals, polycyclic aromatic hydrocarbons, microplastics, perfluorinated polyfluoroalkyl substances. Based on systematic summary of sources, hazards, migration behaviors these various existing remediation methods analyzed, advantages disadvantages different discussed. Finally, future research prospects described, significance study contaminant subsurface environment is emphasized. can help provide theoretical technical support for removal further improve rate actual sites.

Language: Английский

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Critical Review of Pd-Catalyzed Reduction Process for Treatment of Waterborne Pollutants

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 7, 2024

Catalyzed reduction processes have been recognized as important and supplementary technologies for water treatment, with the specific aims of resource recovery, enhancement bio/chemical-treatability persistent organic pollutants, safe handling oxygenate ions. Palladium (Pd) has widely used a catalyst/electrocatalyst in these processes. However, due to limited reserves high cost Pd, it is essential gain better understanding Pd-catalyzed decontamination process design affordable sustainable Pd catalysts. This review provides systematic summary recent advances reductive designing Pd-based nanocatalysts treatment water-borne special focus on interactions transformation mechanisms pollutant molecules catalysts at atomic scale. The discussion begins by examining adsorption pollutants onto sites from thermodynamic viewpoint. followed an explanation molecular-level reaction mechanism, demonstrating how electron-donors participate pollutants. Next, influence reactive site structure catalytic performance explored. Additionally, facilitating oxidation briefly discussed. longevity catalysts, crucial factor determining their practicality, also examined. Finally, we argue increased attention mechanism study, well precise construction under batch synthesis conditions, use catalysts/electrocatalysts concentrated facilitate recovery.

Language: Английский

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Ether-Based High-Voltage Lithium Metal Batteries: The Road to Commercialization

ACS Nano, Journal Year: 2024, Volume and Issue: 18(16), P. 10726 - 10737

Published: April 11, 2024

Ether-based high-voltage lithium metal batteries (HV-LMBs) are drawing growing interest due to their high compatibility with the Li anode. However, commercialization of ether-based HV-LMBs still faces many challenges, including short cycle life, limited safety, and complex failure mechanisms. In this Review, we discuss recent progress achieved in electrolytes for propose a systematic design principle electrolyte based on three important parameters: electrochemical performance, industrial scalability. Finally, summarize challenges commercial application suggest roadmap future development.

Language: Английский

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Electrochemical Reduction of Perfluorooctanoic Acid (PFOA): An Experimental and Theoretical Approach

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(15), P. 10687 - 10698

Published: April 5, 2024

Perfluorooctanoic acid (PFOA) is an artificial chemical of global concern due to its high environmental persistence and potential human health risk. Electrochemical methods are promising technologies for water treatment because they efficient, cheap, scalable. The electrochemical reduction PFOA one the current methodologies. This process leads defluorination carbon chain hydrogenated products. Here, we describe a mechanistic study in gold electrodes. By using linear sweep voltammetry (LSV), E0′ −1.80 V vs Ag/AgCl was estimated. Using scan rate diagnosis, determined electron-transfer coefficient (αexp) 0.37, corresponding concerted mechanism. strong adsorption into surface confirmed by Langmuir-like isotherm absence (KA = 1.89 × 1012 cm3 mol–1) presence negative 3.94 107 mol–1, at −1.40 Ag/AgCl). Based on Marcus–Hush's theory, calculations show solvent reorganization energy (λ0) 0.9 eV, suggesting large electrostatic repulsion between perfluorinated water. estimated free transition state electron transfer (ΔG‡ 2.42 eV) suggests that it thermodynamically reaction-limiting step. 19F – 1H NMR, UV–vis, mass spectrometry studies confirm displacement fluorine atoms hydrogen. Density functional theory (DFT) also support mechanism reductive PFOA, agreement with experimental values.

Language: Английский

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Phosphate-Functionalized CeO₂ Nanosheets for Efficient Catalytic Oxidation of Dichloromethane

Environmental Science & Technology, Journal Year: 2018, Volume and Issue: 52(22), P. 13430 - 13437

Published: Oct. 29, 2018

Tuning the nature and profile of acidic basic sites on surface redox-active metal oxide nanostructures is a promising approach to constructing efficient catalysts for oxidative removal chlorinated volatile organic compounds (CVOCs). Herein, using dichloromethane (DCM) oxidation as model reaction, we report that phosphate (PO x) Brønsted acid can be incorporated onto CeO2 nanosheet (NS) via an organophosphate-mediated route, which effectively enhance CeO2's catalytic performance by promoting chlorine poisoning species. From systematic study correlation between PO x composition, structure (acid sites), properties, find also function decrease amount medium-strong (O2-), reducing formation byproduct monochloromethane (MCM) leading desirable product, HCl. At optimized P/Ce ratio (0.2), x-CeO2 NSs perform stable DCM conversion 65-70% over 10 h at 250 °C 95% 300 °C, superior both pristine other phosphate-modified NSs. Our work clearly identifies critical role functionalized CVOCs oxidation, guiding future advanced catalyst design environmental remediation.

Language: Английский

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