Electrochemical oxygen reduction for H<sub>2</sub>O<sub>2</sub> production: catalysts, pH effects and mechanisms

Pang, Yongyu; Xie, Huan; Sun, Yuan; Titirici, Maria‐Magdalena; Chai, Guoliang

doi:10.1039/d0ta09122g

Cited by 128 publications

(73 citation statements)

References 98 publications

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“…[9] In neutral or acidic solution, the performance of M-N-C is still insufficient with high overpotential or low selectivity. [10] Atomically dispersed CoNC is a promising material for H 2 O 2 selective electrosynthesis via a two-electron oxygen reduction reaction. However, the performance of typical CoNC materials with routine CoN 4 active center is insufficient and needs to be improved further.…”

mentioning

confidence: 99%

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Shen

Qiu

Liu

et al. 2022

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An attractive alternative route for direct on-site production of H 2 O 2 is through two-electron oxygen reduction reaction (ORR). [3] For safe and eco-friendly electrosynthesis of H 2 O 2 , efficient catalysts are vital. [4] Benefiting from the desirable features of atomically isolated metal center, the end-on type of adsorption of O 2 on single-atom catalysts (SACs), reduce the possibility of OO bond splitting; thereby facilitating the selective production of H 2 O 2 production. [5] By maximizing the atom utilization efficiency, the SACs of metal-nitrogen doped carbon (M-N-C) with tunable geometry and electronic structures are considered as promising candidates for ORR. [6] Till now, various M-N-C materials (M = Co, Ni, Mo, etc.) [7] have been explored for efficient H 2 O 2 production in alkaline solution. However, H 2 O 2 is intrinsically unstable in an alkaline solution due to the decomposition catalyzed by OH − . [8] To suppress the decomposition of H 2 O 2 , an extra inhibitor is necessary. [9] In neutral or acidic solution, the performance of M-N-C is still insufficient with high overpotential or low selectivity. [10] Atomically dispersed CoNC is a promising material for H 2 O 2 selective electrosynthesis via a two-electron oxygen reduction reaction. However, the performance of typical CoNC materials with routine CoN 4 active center is insufficient and needs to be improved further. This can be done by finetuning its atomic coordination configuration. Here, a single-atom electrocatalyst (Co/NC) is reported that comprises a specifically penta-coordinated CoNC configuration (OCoN 2 C 2 ) with Co center coordinated by two nitrogen atoms, two carbon atoms, and one oxygen atom. Using a combination of theoretical predictions and experiments, it is confirmed that the unique atomic structure slightly increases the charge state of the cobalt center. This optimizes the adsorption energy towards *OOH intermediate, and therefore favors the two-electron ORR relevant for H 2 O 2 electrosynthesis. In neutral solution, the as-synthesized Co/NC exhibits a selectivity of over 90% over a potential ranging from 0.36 to 0.8 V, with a turnover frequency value of 11.48 s −1 ; thus outperforming the state-of-the-art carbon-based catalysts.

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confidence: 99%

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Shen

Qiu

Liu

et al. 2022

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“…There are multiple factors that control a catalysts preference for HO 2 − desorption vs. OH − desorption for the selectivity determining step. These include the structure of the active site and its environment that can influence its catalyst – oxygen binding strength [23–24] . While we cannot exclude factors such as differing amounts of defects and undercoordinated sites within our set of MON catalysts, a principle factor that may lead do their varying FEs is the identity of the ligand bound to the layers of Ni−O polyhedra.…”

Section: Resultsmentioning

confidence: 99%

“…These include the structure of the active site ChemElectroChem and its environment that can influence its catalyst -oxygen binding strength. [23][24] While we cannot exclude factors such as differing amounts of defects and undercoordinated sites within our set of MON catalysts, a principle factor that may lead do their varying FEs is the identity of the ligand bound to the layers of NiÀ O polyhedra. The different ligands have different degrees of electron donating/withdrawing character, which affects the electronic structure of the active sites (open Ni sites).…”

Section: Chemelectrochemmentioning

confidence: 99%

Linker‐Modulated Peroxide Electrosynthesis Using Metal‐Organic Nanosheets**

Kuruvinashetti

Kornienko

2022

ChemElectroChem

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The electrochemical synthesis of hydrogen peroxide (H 2 O 2 ), a widely used oxidant, is emerging as a green alternative to the conventional anthraquinone method. In this work, Ni-based metal-organic nanosheet (NiÀ MON) catalysts constructed using a variety of linkers were studied as oxygen reduction catalysts. Using a host of analytical techniques, we reveal how modulating the terephthalic acid linker with hydroxy, amine, and fluorine groups impacts the resulting physical and electronic structure of the Ni catalytic sites. These changes further impact the catalysts' Faradaic Efficiency for H 2 O 2 , with the NiÀ AmineÀ MON reaching near 100 % FE at minimal overpotential for the 2e À H 2 O 2 pathway in alkaline electrolyte. Finally, we translate the NiÀ AmineÀ MON catalyst to a gasdiffusion reaction geometry and demonstrate a H 2 O 2 partial current density of 200 mA/cm 2 while maintaining 85 % Faradaic efficiency. In all, this study puts forth a simple route to catalyst modulation for highly effective H 2 O 2 electrosynthesis.

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“…In general, electrolyte pH has a considerable impact on 2e − ORR for H 2 O 2 production. [20] Here comes a question, whether electrolyte pH will influence the performance of the ZAB/ UV system or not. To disclose this enigma, the initial pH of the dye wastewater was adjusted by sulfuric acid (H 2 SO 4 ) or sodium hydroxide (NaOH), and we subsequently studied the corresponding degradation behaviors of the dye.…”

Section: Application Of Zab/uv System For Water Purificationmentioning

confidence: 99%

On‐Site Production of Dilute H₂O₂ with Zinc–Air Battery

Huang

et al. 2021

Adv Materials Technologies

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Hydrogen peroxide (H2O2) is extensively applied in environmental remediation, disinfection, bleaching, and so on. Two‐electron oxygen reduction reaction for synthesizing H2O2 is the most promising alternative to the traditional energy‐intensive anthraquinone process. Existing strategies for electrocatalytic synthesis of H2O2 generally proceed well in alkaline electrolytes. But environmental application demands the reaction to take place in a broad pH range, especially in acidic medium. Here a zinc‐air battery technology is developed for on‐site production of H2O2 in alkaline, neutral, and acidic conditions. A key component of the battery is the tubular cathode fabricated by partially oxidized carbon nanotubes self‐assembled on the substrate of nickel foam. The battery exhibits an unusual 2e− discharge property and achieves an appreciable H2O2 accumulation (215.1 µmol, 497 ppm, 162.5 mg L−1 h−1) in acidic solution within 3 h, which is among the highest value ever been reported through electrosynthesis. Excitingly, the battery coupled with UV light demonstrates a promising application in water purification, which enables rapid degradation of model pollutants and actual pollutants ranging from municipal sewage to dye and pesticide wastewaters. Furthermore, this water treatment technology can be self‐powered, as the battery in the system generates the power that is available to drive UV lights.

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Electrochemical oxygen reduction for H₂O₂ production: catalysts, pH effects and mechanisms

Abstract: Electrochemical oxygen reduction offers an efficient and environmental-friendly route for hydrogen peroxide (H2O2) generation. This electrochemical process can produces H2O2 on-site under ambient conditions. High selectivity and activity two-electron oxygen...

Cited by 128 publications

References 98 publications

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Linker‐Modulated Peroxide Electrosynthesis Using Metal‐Organic Nanosheets**

On‐Site Production of Dilute H₂O₂ with Zinc–Air Battery

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Electrochemical oxygen reduction for H2O2 production: catalysts, pH effects and mechanisms

Abstract: Electrochemical oxygen reduction offers an efficient and environmental-friendly route for hydrogen peroxide (H2O2) generation. This electrochemical process can produces H2O2 on-site under ambient conditions. High selectivity and activity two-electron oxygen...

Cited by 128 publications

References 98 publications

Boosting Oxygen Reduction for High‐Efficiency H2O2 Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Boosting Oxygen Reduction for High‐Efficiency H2O2 Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Linker‐Modulated Peroxide Electrosynthesis Using Metal‐Organic Nanosheets**

On‐Site Production of Dilute H2O2 with Zinc–Air Battery

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Product

Resources

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Electrochemical oxygen reduction for H₂O₂ production: catalysts, pH effects and mechanisms

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

Boosting Oxygen Reduction for High‐Efficiency H₂O₂ Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts

On‐Site Production of Dilute H₂O₂ with Zinc–Air Battery