Identification of the Highly Active Co–N₄ Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(32), С. 14505 - 14516

Опубликована: Авг. 3, 2022

Electrosynthesis of hydrogen peroxide (H

Язык: Английский

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Dual-doping NiMoO4 with multi-channel structure enable urea-assisted energy-saving H2 production at large current density in alkaline seawater

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 320, С. 121977 - 121977

Опубликована: Сен. 13, 2022

Язык: Английский

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Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

Nature Catalysis, Год журнала: 2023, Номер 6(3), С. 234 - 243

Опубликована: Март 13, 2023

Язык: Английский

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Tuning Two‐Electron Oxygen‐Reduction Pathways for H₂O₂ Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts

Advanced Materials, Год журнала: 2022, Номер 34(23)

Опубликована: Фев. 8, 2022

Abstract The hydrogen peroxide (H 2 O ) generation via the electrochemical oxygen reduction reaction (ORR) under ambient conditions is emerging as an alternative and green strategy to traditional energy‐intensive anthraquinone process unsafe direct synthesis using H . It enables on‐site decentralized production air renewable electricity for various applications. Currently, atomically dispersed single metal site catalysts have emerged most promising platinum group (PGM)‐free electrocatalysts ORR. Further tuning their central sites, coordination environments, local structures can be highly active selective 2e − Herein, recent methodologies achievements on developing are summarized. Combined with theoretical computation advanced characterization, a structure–property correlation guide rational catalyst design favorable ORR aimed provide. Due oxidative nature of derived free radicals, stability effective solutions improve tolerance emphasized. Transferring intrinsic properties electrode performance viable applications always remains grand challenge. key metrics knowledge during electrolyzer development are, therefore, highlighted.

Язык: Английский

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Carbon nitride based materials: more than just a support for single-atom catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 4878 - 4932

Опубликована: Янв. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Язык: Английский

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An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(30), С. 16584 - 16596

Опубликована: Июль 24, 2023

In this work, we have fabricated an aryl amino-substituted graphitic carbon nitride (g-C3N4) catalyst with atomically dispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new exhibited excellent reactivity, obtaining up to 2230 μM H2O2 in 7 h alkaline water and 1800 seawater under identical conditions. More importantly, the was quickly recovered for subsequent reuse without appreciable loss performance. Interestingly, unlike usual two-electron oxygen reduction reaction pathway, generation through a less common oxidation (WOR) process which both direct indirect WOR processes occurred; namely, photoinduced h+ oxidized H2O via one-step 2e- WOR, first hydroxide (OH-) ion generate hydroxy radical (•OH), formed indirectly by combination two •OH. We characterized material, at catalytic sites, atomic level using electron paramagnetic resonance, X-ray absorption near edge structure, extended fine high-resolution transmission microscopy, photoelectron spectroscopy, magic-angle spinning solid-state NMR multiscale molecular modeling, combining classical reactive dynamics simulations quantum chemistry calculations.

Язык: Английский

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Highly Efficient Hydroxyl Radicals Production Boosted by the Atomically Dispersed Fe and Co Sites for Heterogeneous Electro-Fenton Oxidation

Environmental Science & Technology, Год журнала: 2023, Номер 57(7), С. 2907 - 2917

Опубликована: Фев. 7, 2023

The heterogeneous electro-Fenton (hetero-e-Fenton)-coupled electrocatalytic oxygen reduction reaction (ORR) is regarded as a promising strategy for ·OH production by simultaneously driving two-electron ORR toward H2O2 and stepped activating the as-generated to ·OH. However, high-efficiency electrogeneration of remains challengeable, it difficult synchronously obtain efficient catalysis both steps above on one catalytic site. In this work, we propose dual-atomic-site catalyst (CoFe DAC) cooperatively catalyze electrogeneration, where atomically dispersed Co sites are assigned enhance O2 intermediates Fe responsible activation CoFe DAC delivers higher rate 2.4 mmol L-1 min-1 gcat-1 than single-site Co-NC (0.8 gcat-1) Fe-NC (1.0 gcat-1). Significantly, hetero-e-Fenton process demonstrated be more energy-efficient actual coking wastewater treatment with an energy consumption 19.0 kWh kg-1 COD-1 other electrochemical technologies that reported values 29.7∼68.0 kW h COD-1. This study shows attractive advantages efficiency sustainability which should have fresh inspiration development new-generation technology.

Язык: Английский

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Structure-controlled graphene electrocatalysts for high-performance H₂O₂ production

Energy & Environmental Science, Год журнала: 2022, Номер 15(7), С. 2858 - 2866

Опубликована: Янв. 1, 2022

A structure-mechanism-performance relationship of metal-free carbon catalysts for outstanding H 2 O production activity and selectivity in alkaline media.

Язык: Английский

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Versatile Photoelectrocatalysis Strategy Raising Up the Green Production of Hydrogen Peroxide

Advanced Energy Materials, Год журнала: 2023, Номер 13(14)

Опубликована: Март 1, 2023

Abstract H 2 O plays an irreplaceable role in many aspects of human society, such as paper bleaching, medical disinfection, wastewater treatment, organic synthesis, hydrometallurgy and the electronic industry. However, unsustainability current industrial production process traditional anthraquinone has a serious conflict with green sustainable development. The photo/electrocatalytic from renewable energy advantages being more economical, low‐carbon green, line requirements economy. These catalytic methods have played demonstrative development small molecules, contributing to fundamental understanding general catalysis providing scientific perspective for future new cycles. In this review, authors aim integrate reaction mechanism photocatalytic electrocatalytic production, summarize application recent years, assess modern technologies promoted research, including flux equipment coproduction, etc. This review intends provide clear logic profile directions calls researchers insights into field.

Язык: Английский

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Strategies for Sustainable Production of Hydrogen Peroxide via Oxygen Reduction Reaction: From Catalyst Design to Device Setup

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Май 9, 2023

Abstract An environmentally benign, sustainable, and cost-effective supply of H 2 O as a rapidly expanding consumption raw material is highly desired for chemical industries, medical treatment, household disinfection. The electrocatalytic production route via electrochemical oxygen reduction reaction (ORR) offers sustainable avenue the on-site from O. most crucial innovative part such technology lies in availability suitable electrocatalysts that promote two-electron (2e – ) ORR. In recent years, tremendous progress has been achieved designing efficient, robust, catalyst materials, including noble metals their alloys, metal-free carbon-based single-atom catalysts, molecular catalysts. Meanwhile, cell designs have significantly advanced applications at industrial level. This review summarizes fundamental basics advances 2e -ORR, design, mechanistic explorations, theoretical computations, experimental evaluations, designs. Perspectives on addressing remaining challenges are also presented with an emphasis large-scale synthesis route.

Язык: Английский

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