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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Rational Fabrication of Low‐Coordinate Single‐Atom Ni Electrocatalysts by MOFs for Highly Selective CO₂ Reduction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(14), С. 7607 - 7611

Опубликована: Янв. 15, 2021

Abstract Single‐atom catalysts (SACs) have attracted tremendous interests due to their ultrahigh activity and selectivity. However, the rational control over coordination microenvironment of SACs remains a grand challenge. Herein, post‐synthetic metal substitution (PSMS) strategy has been developed fabricate single‐atom Ni with different N numbers (denoted Ni‐N x ‐C) on pre‐designed N‐doped carbon derived from metal‐organic frameworks. When served for CO 2 electroreduction, obtained 3 ‐C catalyst achieves Faradaic efficiency (FE) up 95.6 %, much superior that 4 ‐C. Theoretical calculations reveal lower number in can significantly enhance COOH* formation, thereby accelerating reduction. In addition, shows excellent performance Zn–CO battery FE stability. This work opens new general avenue modulation (MEM) utilization.

Язык: Английский

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Non-Bonding Interaction of Neighboring Fe and Ni Single-Atom Pairs on MOF-Derived N-Doped Carbon for Enhanced CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(46), С. 19417 - 19424

Опубликована: Ноя. 15, 2021

Single-atom catalysts (SACs), featuring high atom utilization, have captured widespread interests in diverse applications. However, the single-atom sites SACs are generally recognized as independent units and interplay of adjacent is largely overlooked. Herein, by direct pyrolysis MOFs assembled with Fe Ni-doped ZnO nanoparticles, a novel Fe1-Ni1-N-C catalyst, neighboring Ni pairs decorated on nitrogen-doped carbon support, has been precisely constructed. Thanks to synergism pairs, presents significantly boosted performances for electrocatalytic reduction CO2, far surpassing Fe1-N-C Ni1-N-C separate or single atoms. Additionally, also exhibits superior performance excellent CO selectivity durability Zn-CO2 battery. Theoretical simulations reveal that, Fe1-Ni1-N-C, atoms can be highly activated via non-bonding interaction, facilitating formation COOH* intermediate thereby accelerating overall CO2 reduction. This work supplies general strategy construct containing multiple metal species reveals vital importance communitive effect between toward improved catalysis.

Язык: Английский

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Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Июль 2, 2021

While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities stability both CO

Язык: Английский

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Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Advanced Energy Materials, Год журнала: 2020, Номер 11(3)

Опубликована: Ноя. 30, 2020

Abstract Future renewable energy supplies and a sustainable environment rely on many important catalytic processes. Single‐atom catalysts (SACs) are attractive because of their maximum atom utilization efficiency, tunable electronic structures, outstanding performance. Of particular note, transition‐metal SACs exhibit excellent activity selectivity for the oxygen reduction reaction (ORR)—an half in fuel cells metal–air batteries as well portable hydrogen peroxide (H 2 O ) production. Although considerable efforts have been made synthesis ORR, regulation coordination environments thus structures still pose big challenge. In this review, strategies manipulating classified into three categories, including center metal atoms, manipulation surrounding connecting to atom, modification geometric configuration support. Finally, some issues regarding future development ORR raised possible solutions proposed.

Язык: Английский

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Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(31), С. 12220 - 12229

Опубликована: Июль 29, 2021

Well-organized photosensitive units and catalytic sites in proximity are crucial for improving charge separation efficiency boosting photocatalysis. Herein, a general facile strategy the construction of high-loading (>4 wt %) single-atom catalysts (SACs) with tunable coordination microenvironment has been developed on basis metal-organic frameworks (MOFs). The neighboring -O/OHx groups from Zr6-oxo cluster MOFs provide lone-pair electrons balance to immobilize extraneous single metal atoms. well-accessible atomically dispersed possess close (i.e., linkers), which greatly accelerates transfer thereby promotes redox reaction. environment representative Ni significantly modulates electronic state proton activation barrier toward hydrogen production. As result, optimized Ni1-S/MOF unique Ni(I) presents excellent photocatalytic H2 production activity, up 270 fold pristine MOF far surpassing other Ni1-X/MOF counterparts. This work unambiguously demonstrates great advantage fabrication high-content SACs variable microenvironments that linkers, facilitating electron promoting

Язык: Английский

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Novel lignin-based single atom catalysts as peroxymonosulfate activator for pollutants degradation: Role of single cobalt and electron transfer pathway

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 286, С. 119910 - 119910

Опубликована: Янв. 21, 2021

Язык: Английский

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Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Сен. 10, 2022

Electrocatalytic urea synthesis emerged as the promising alternative of Haber-Bosch process and industrial synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe-Ni pairs can significantly improve efficiency electrochemical synthesis. Compared isolated single-atom catalysts, act efficient sites for coordinated adsorption activation multiple reactants, enhancing crucial C-N coupling thermodynamically kinetically. The performance up to an order magnitude higher than those electrocatalysts, high yield rate 20.2 mmol h-1 g-1 corresponding Faradaic 17.8% has been successfully achieved. A total about 100% formation value-added urea, CO, NH3 was realized. This work presents insight into synergistic catalysis towards sustainable via identifying tailoring atomic site configurations.

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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Anion-exchange membrane water electrolyzers and fuel cells

Chemical Society Reviews, Год журнала: 2022, Номер 51(23), С. 9620 - 9693

Опубликована: Янв. 1, 2022

The key components, working management, and operating techniques of anion-exchange membrane water electrolyzers fuel cells are reviewed for the first time.

Язык: Английский

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