Single-atom catalysis in advanced oxidation processes for environmental remediation

Chemical Society Reviews, Год журнала: 2021, Номер 50(8), С. 5281 - 5322

Опубликована: Янв. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Язык: Английский

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Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts

Chemical Society Reviews, Год журнала: 2021, Номер 50(13), С. 7745 - 7778

Опубликована: Янв. 1, 2021

Bifunctional oxygen reduction and evolution constitute the core processes for sustainable energy storage. The advances on noble-metal-free bifunctional electrocatalysts are reviewed.

Язык: Английский

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Operando Cooperated Catalytic Mechanism of Atomically Dispersed Cu−N₄ and Zn−N₄ for Promoting Oxygen Reduction Reaction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(25), С. 14005 - 14012

Опубликована: Март 31, 2021

Abstract Dual‐metal single‐atom catalysts exhibit superior performance for oxygen reduction reaction (ORR), however, the synergistic catalytic mechanism is not deeply understood. Herein, we report a dual‐metal catalyst consisted of Cu−N 4 and Zn−N on N‐doped carbon support (Cu/Zn−NC). It exhibits high‐efficiency ORR activity with an E onset 0.98 V 1/2 0.83 V, excellent stability (no degradation after 10 000 cycles), surpassing state‐of‐the‐art Pt/C great mass Pt‐free single atom catalysts. Operando XANES demonstrates that as active center experiences change from atomic dispersion to cluster cooperation during process, then turns state again reaction. DFT calculation further indicates adjustment effect Zn d‐orbital electron distribution Cu could benefit stretch cleavage O‐O center, speeding up process rate determining step OOH*.

Язык: Английский

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Single-atom catalysts for photocatalytic energy conversion

Joule, Год журнала: 2022, Номер 6(1), С. 92 - 133

Опубликована: Янв. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Язык: Английский

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Atomically Dispersed Co₂–N₆ and Fe–N₄ Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media

Advanced Materials, Год журнала: 2021, Номер 33(49)

Опубликована: Окт. 8, 2021

Abstract Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based for oxygen reduction reaction (ORR). Regulating the local configuration of atomic is key catalyst performance enhancement. Different from previously reported single‐atom or dual‐atom configurations, a new type ternary‐atom catalyst, which consists atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co 2 –N 6 Fe–N 4 structures) that coanchored on highly graphitized carbon supports developed. This unique ORR outperforms with only in both alkaline acid conditions. Density functional theory calculations clearly unravels synergistic effect sites, can induce higher filling degree Fe–d orbitals favors binding capability *OH intermediates (the rate determining step). may be alternative Pt drive cathodic zinc–air batteries.

Язык: Английский

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Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2954 - 3009

Опубликована: Янв. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Язык: Английский

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Activation of peroxymonosulfate via mediated electron transfer mechanism on single-atom Fe catalyst for effective organic pollutants removal

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 299, С. 120714 - 120714

Опубликована: Сен. 14, 2021

Язык: Английский

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Novel Cd0.5Zn0.5S/Bi2MoO6 S-scheme heterojunction for boosting the photodegradation of antibiotic enrofloxacin: Degradation pathway, mechanism and toxicity assessment

Separation and Purification Technology, Год журнала: 2022, Номер 304, С. 122401 - 122401

Опубликована: Окт. 17, 2022

Язык: Английский

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Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

Chemical Reviews, Год журнала: 2021, Номер 121(21), С. 13620 - 13697

Опубликована: Окт. 13, 2021

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which heterogenized on inert supports such as graphene, porous carbon, and oxides. Their thermal stability, electronic properties, catalytic activities can be controlled via interactions between the center neighboring heteroatoms nitrogen, oxygen, sulfur. Due to atomic dispersion amount required for catalysis decreased, thus offering new possibilities control selectivity a given transformation well improve catalyst turnover frequencies numbers. This review aims comprehensively summarize synthesis Fe-SACs with focus anchoring single atoms (SA) carbon/graphene supports. The characterization these advanced materials using various spectroscopic techniques their applications in diverse research areas described. When applicable, mechanistic investigations conducted understand specific behavior Fe-SACs-based highlighted, including use theoretical models.

Язык: Английский

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Hierarchical trimetallic Co-Ni-Fe oxides derived from core-shell structured metal-organic frameworks for highly efficient oxygen evolution reaction

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 287, С. 119953 - 119953

Опубликована: Фев. 6, 2021

Metal-organic frameworks (MOFs) have recently emerged as promising precursors to construct efficient non-noble metal electrocatalyst for oxygen evolution reaction (OER). Herein, a Co-Ni-Fe spinel oxide-carbonitrides hybrids (CoNiFeOx-NC) with hierarchical structure was synthesized from Fe-MIL-101-NH2 through unique ion-exchange based strategy. The ion exchange of both Ni and Co ions induced hierarchically structured 2-D ternary MOF shell layer encapsulated 3-D octahedral crystals core. This prevents the collapse during air calcination process affords highly porous large surface area. Additionally, combination in oxides derived core-shell provides favorable electronic environment adsorption OER intermediates, which further verified by XPS characterizations DFT calculations. study revealed Ni-Co coordinated Oh sites MFe2O4 reverse structures main active sites, tuned binding strength species catalyst electron transfer Fe→Co→Ni, thereby lowered energy barriers OER. As result, rationally designed CoNiFeOx-NC manifests superior performance low overpotential 265 mV at 50 mA cm−2 decent Tafel slope 64.1 dec-1. strategy may serve versatile platform rational design synthesis multi-metallic electrocatalysts.

Язык: Английский

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