Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Янв. 12, 2023

Direct hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain be challenging, partially due insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches identify transition-metal single-site catalysts for using *OOH binding energy as descriptor. The predictions are then used guidance synthesize desired cobalt O-modified Co-(pyrrolic N)4 configuration that can achieve current densities up 300 mA cm-2 96-100% Faradaic efficiencies H2O2 at record rate of 11,527 mmol h-1 gcat-1. Here, show feasibility versatility metal design various commercial carbon phthalocyanine starting materials high applicability acidic, neutral alkaline electrolytes.

Язык: Английский

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CoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Авг. 8, 2023

The two-electron oxygen reduction reaction in acid is highly attractive to produce H2O2, a commodity chemical vital various industry and household scenarios, which still hindered by the sluggish kinetics. Herein, both density function theory calculation in-situ characterization demonstrate that dual-atom CoIn catalyst, O-affinitive In atom triggers favorable stable adsorption of hydroxyl, effectively optimizes OOH on neighboring Co. As result, Co atoms shifts pathway for efficient H2O2 production acid. partial current reaches 1.92 mA cm-2 at 0.65 V rotating ring-disk electrode test, while rate as high 9.68 mol g-1 h-1 three-phase flow cell. Additionally, CoIn-N-C presents excellent stability during long-term operation, verifying practicability catalyst. This work provides inspiring insights into rational design active catalysts other catalytic systems.

Язык: Английский

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Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

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

Опубликована: Окт. 13, 2023

Abstract Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design synthesis SACs with versatile local configurations significantly accelerated development efficient sustainable electrocatalysts for a wide range electrochemical applications. As an emergent coordination avenue, intentionally breaking planar symmetry by adding ligands axial direction metal single atoms offers novel approach tuning both geometric structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline burgeoning research topic axially coordinated provide comprehensive summary recent advances synthetic strategies Besides, challenges outlooks field also been emphasized. present review provides in-depth understanding SACs, which could bring new perspectives solutions fine regulation structures catering high-performing electrocatalysis.

Язык: Английский

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Enhancing H₂O₂ Electrosynthesis at Industrial-Relevant Current in Acidic Media on Diatomic Cobalt Sites

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(13), С. 9434 - 9443

Опубликована: Март 20, 2024

Electrocatalytic synthesis of hydrogen peroxide (H2O2) in acidic media is an efficient and eco-friendly approach to produce inherently stable H2O2, but limited by the lack selective catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction efficiently H2O2 at 50–400 mA cm–2 acid. Electrode kinetics study shows >95% selectivity on sites. In flow cell device, record-high production rate 11.72 mol gcat–1 h–1 exceptional long-term stability (100 h) are realized high situ spectroscopic studies theoretical calculations reveal that introducing second metal into coordination sphere site can optimize binding strength key intermediates due downshifted d-band center cobalt. We also demonstrate feasibility processing municipal plastic wastes through decentralized production.

Язык: Английский

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Tailoring the Atomic‐Local Environment of Carbon Nanotube Tips for Selective H₂O₂ Electrosynthesis at High Current Densities

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Авг. 3, 2023

The atomic-local environment of catalytically active sites plays an important role in tuning the activity carbon-based metal-free electrocatalysts (C-MFECs). However, rational regulation is always impeded by synthetic limitations and insufficient understanding formation mechanism catalytic sites. Herein, possible cleavage carbon nanotubes (CNTs) through crossing points during ball-milling proposed, resulting abundant CNT tips that are more susceptible to be modified heteroatoms, achieving precise modulation atomic at tips. obtained CNTs with N,S-rich (N,S-TCNTs) exhibit a wide potential window 0.59 V along H2 O2 selectivity for over 90.0%. Even using air as source, flow cell system N,S-TCNTs catalyst attains high productivity up 30.37 mol gcat.-1 h-1 @350 mA cm-2 , superior most reported C-MFECs. From practical point view, solid electrolyzer based on further employed realize in-situ continuous generation pure solution (up 4.35 mmol @300 ; 300 h). functionalized hold great promise applications, even beyond generation.

Язык: Английский

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Single atom catalysts for use in the selective production of hydrogen peroxide via two-electron oxygen reduction reaction: Mechanism, activity, and structure optimization

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 337, С. 122987 - 122987

Опубликована: Июнь 12, 2023

Язык: Английский

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Single‐atom catalyst application in distributed renewable energy conversion and storage

SusMat, Год журнала: 2023, Номер 3(2), С. 160 - 179

Опубликована: Март 2, 2023

Abstract In recent years, owing to the depletion of fossil energy and aggravation environmental pollution, conversion storage distributed renewable (such as solar energy, wind tidal energy) based on electrochemical technology have attracted extensive attention. Electrocatalytic processes with high efficiency selectivity play a key role in clean storage. With nearly 100% atomic utilization rate unique catalytic activity, single‐atom catalysts (SACs) been rapidly developed widely used field this review, we first introduce characteristics SACs. Then, focus application SACs conversion, including water electrolysis reaction, nitrogen reduction nitrate oxygen carbon dioxide reaction. terms storage, supercapacitors Li–S batteries. Further, enumerate some methods for synthesis metal loading or large scale. Finally, main challenges opportunities emerging future are discussed prospected.

Язык: Английский

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Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production

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

Опубликована: Янв. 2, 2024

Abstract Direct electrosynthesis of hydrogen peroxide (H 2 O ) via the two-electron oxygen reduction reaction presents a burgeoning alternative to conventional energy-intensive anthraquinone process for on-site applications. Nevertheless, its adoption is currently hindered by inferior H selectivity and diminished yield induced consecutive or Fenton reactions. Herein, guided theoretical calculations, we endeavor overcome this challenge activating main-group Pb single-atom catalyst local micro-environment engineering strategy employing sulfur super-coordinated structure. The catalyst, synthesized using carbon dot-assisted pyrolysis technique, displays an industrial current density reaching 400 mA cm −2 elevated accumulated concentrations (1358 mM) with remarkable Faradaic efficiencies. Both experimental results simulations elucidate that S super-coordination directs fraction electrons from sites coordinated atoms, consequently optimizing *OOH binding energy augmenting 2e − activity. This work unveils novel avenues mitigating production-depletion in through rational design catalysts.

Язык: Английский

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Understanding Advanced Transition Metal‐Based Two Electron Oxygen Reduction Electrocatalysts from the Perspective of Phase Engineering

Advanced Materials, Год журнала: 2024, Номер 36(25)

Опубликована: Март 8, 2024

Abstract Non‐noble transition metal (TM)‐based compounds have recently become a focal point of extensive research interest as electrocatalysts for the two electron oxygen reduction (2e − ORR) process. To efficiently drive this reaction, these TM‐based must bear unique physiochemical properties, which are strongly dependent on their phase structures. Consequently, adopting engineering strategies toward structure has emerged cutting‐edge scientific pursuit, crucial achieving high activity, selectivity, and stability in electrocatalytic This comprehensive review addresses intricate field applied to non‐noble 2e ORR. First, connotation fundamental concepts related kinetics thermodynamics succinctly elucidated. Subsequently, focus shifts detailed discussion various approaches, including elemental doping, defect creation, heterostructure construction, coordination tuning, crystalline design, polymorphic transformation boost or revive ORR performance (selectivity, stability) catalysts, accompanied by an insightful exploration phase‐performance correlation. Finally, proposes fresh perspectives current challenges opportunities burgeoning field, together with several critical directions future development electrocatalysts.

Язык: Английский

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General Design Concept of High‐Performance Single‐Atom‐Site Catalysts for H₂O₂ Electrosynthesis

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 5, 2024

Hydrogen peroxide (H

Язык: Английский

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