An abnormal size effect enables ampere-level O<sub>2</sub>electroreduction to hydrogen peroxide in neutral electrolytes

Ding, Shan; Xia, Baokai; Li, Ming; Lou, Fengqian; Chi, Cheng; Gao, Taotao; Kang, Yang; Jiang, Lili; Nie, Zhihao; Zhang, Yuxiang; Guan, Hua; Duan, Jingjing; Chen, Sheng

doi:10.1039/d3ee00509g

“…The mechanism of 4e – -ORR is as follows: The mechanism of 2e – -ORR is as follows: For the ORR, both pathways have the same reactive intermediate of *OOH (Figure d). , The adsorption strength of *OOH on the catalyst surface and the breaking of the O–O bond in OOH had a significant effect on the final reaction pathway. The smaller Δ G *OOH (the adsorption energy of *OOH species) value implies a stronger adsorption of *OOH, which can lead to a shortening of the O–O bond in *OOH, prompting a 4e – reaction to occur to produce H 2 O.…”

Section: Oxygen Reduction Reaction Synthesis Of H2o2mentioning

confidence: 99%

Perspectives on Carbon-Based Catalysts for the Two-Electron Oxygen Reduction Reaction for Electrochemical Synthesis of Hydrogen Peroxide: A Minireview

Peng,

Tan,

Liu

et al. 2023

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Hydrogen peroxide (H2O2) is an extremely important chemical used in a range of industry and healthcare fields, including disinfection, bleaching, and water treatment. Electrocatalytic H2O2 production via the two-electron oxygen reduction reaction (2e–-ORR) is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with a high H2O2 yield, selectivity, and durability is still challenging because the synthesis of catalysts with precise atomic level structures is very difficult. This paper reviews the research and progress on the preparation of H2O2 by 2e–-ORR from carbon-based materials in recent years, aiming to help design low-cost and high-performance 2e–-ORR catalysts.

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“…[9] Besides, the majority of the agents for stabilizing H 2 O 2 products are near neutral. [10] However, the neutral electrolytes usually have low concentrations of ions, resulting in high ohmic loss and insufficient binding towards OOH* associated with slow ORR kinetics. [8,11] Owing to these, it is highly challenging for the concentrated neutral H 2 O 2 electrosynthesis at large current densities.…”

Section: Introductionmentioning

confidence: 99%

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

Song,

Chi,

Dong

et al. 2024

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The electrosynthesis of hydrogen peroxide (H2O2) via two‐electron (2e‐) oxygen (O2) reduction reaction (ORR) has great potential to replace the traditional energy‐intensive anthraquinone process, but the design of low‐cost and highly active and selective catalysts is greatly challenging for the long‐term H2O2 production under industrial relevant current density, especially under neutral electrolytes. To address this issue, this work constructed a carboxylated hexagonal boron nitride/graphene (h‐BN/G) heterojunction on the commercial activated carbon through the coupling of B, N co‐doping with surface oxygen groups functionalization. The champion catalyst exhibited a high 2e‐ ORR selectivity (>95%), production rate (up to 13.4 mol g‐1 h‐1), and Faradaic efficiency (FE, >95%). The long‐term H2O2 production under the high current density of 100 mA cm‐2 caused the cumulative concentration as high as 2.1 wt.%. The combination of in‐situ Raman spectra and theoretical calculation indicated that the carboxylated h‐BN/G configuration promotes the adsorption of O2 and the stabilization of the key intermediates (OOH* and HOOH*), allowing a low energy barrier for the rate‐determining step of HOOH* release from the active site, and thus improving the 2e‐ ORR performance. The fast dye degradation by using this electrochemical synthesized H2O2 further illustrated the promising practical application.

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“…[9] Besides, the majority of the agents for stabilizing H 2 O 2 products are near neutral. [10] However, the neutral electrolytes usually have low concentrations of ions, resulting in high ohmic loss and insufficient binding towards OOH* associated with slow ORR kinetics. [8,11] Owing to these, it is highly challenging for the concentrated neutral H 2 O 2 electrosynthesis at large current densities.…”

Section: Introductionmentioning

confidence: 99%

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

Song,

Chi,

Dong

et al. 2024

Angewandte Chemie

0

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The electrosynthesis of hydrogen peroxide (H2O2) via two‐electron (2e‐) oxygen (O2) reduction reaction (ORR) has great potential to replace the traditional energy‐intensive anthraquinone process, but the design of low‐cost and highly active and selective catalysts is greatly challenging for the long‐term H2O2 production under industrial relevant current density, especially under neutral electrolytes. To address this issue, this work constructed a carboxylated hexagonal boron nitride/graphene (h‐BN/G) heterojunction on the commercial activated carbon through the coupling of B, N co‐doping with surface oxygen groups functionalization. The champion catalyst exhibited a high 2e‐ ORR selectivity (>95%), production rate (up to 13.4 mol g‐1 h‐1), and Faradaic efficiency (FE, >95%). The long‐term H2O2 production under the high current density of 100 mA cm‐2 caused the cumulative concentration as high as 2.1 wt.%. The combination of in‐situ Raman spectra and theoretical calculation indicated that the carboxylated h‐BN/G configuration promotes the adsorption of O2 and the stabilization of the key intermediates (OOH* and HOOH*), allowing a low energy barrier for the rate‐determining step of HOOH* release from the active site, and thus improving the 2e‐ ORR performance. The fast dye degradation by using this electrochemical synthesized H2O2 further illustrated the promising practical application.

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An abnormal size effect enables ampere-level O₂electroreduction to hydrogen peroxide in neutral electrolytes

Abstract: The principle of size effect has been noticed a century ago, which has nowadays been widely used to express the activity enhancement of a catalyst as a result of size...

Cited by 29 publications

References 46 publications

Perspectives on Carbon-Based Catalysts for the Two-Electron Oxygen Reduction Reaction for Electrochemical Synthesis of Hydrogen Peroxide: A Minireview

Perspectives on Carbon-Based Catalysts for the Two-Electron Oxygen Reduction Reaction for Electrochemical Synthesis of Hydrogen Peroxide: A Minireview

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

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An abnormal size effect enables ampere-level O2electroreduction to hydrogen peroxide in neutral electrolytes

Abstract: The principle of size effect has been noticed a century ago, which has nowadays been widely used to express the activity enhancement of a catalyst as a result of size...

Cited by 29 publications

References 46 publications

Perspectives on Carbon-Based Catalysts for the Two-Electron Oxygen Reduction Reaction for Electrochemical Synthesis of Hydrogen Peroxide: A Minireview

Perspectives on Carbon-Based Catalysts for the Two-Electron Oxygen Reduction Reaction for Electrochemical Synthesis of Hydrogen Peroxide: A Minireview

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

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An abnormal size effect enables ampere-level O₂electroreduction to hydrogen peroxide in neutral electrolytes