Oxygen reduction to hydrogen peroxide on oxidized nanocarbon: Identification and quantification of active sites

Lu, Xingyu; Wang, Dan; Wu, Kuang‐Hsu; Guo, Xiaoling; Qi, Wei

doi:10.1016/j.jcis.2020.04.030

Cited by 94 publications

(47 citation statements)

References 62 publications

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“…DFT calculations illustrated theoretical overpotentials as well as the rate‐limiting steps on typical oxygen functional groups, of which COC groups on the basal plane showed the highest activity. A similar correlation between oxygen concentration and H 2 O 2 selectivity was also confirmed by Lu et al [ 39 ] and Xia et al [ 5 ] Aside from oxidizing methods, reducing methods could be another choice to introduce certain types of oxygen‐containing groups. Kim et al found that both few‐layered mild reduced graphene oxide (F‐mrGO) and annealed F‐mrGO showed high selectivity to H 2 O 2 , the active sites of which were assigned to basal planes and ring ether groups at the edges, respectively, with the aid of in situ Raman, near‐edge X‐ray absorption fine structure (NEXAFS), and other spectroscopic methods ( Figure ).…”

Section: Synthetic Approaches Of Metal‐free Two‐electron Orr Electrocatalystssupporting

confidence: 74%

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

Wang

James

Tour

2021

Adv Energy and Sustain Res

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Hydrogen peroxide (H 2 O 2 ), as an environmentally friendly and highly efficient oxidation reagent, is now widely and increasingly used in many areas. The traditional anthraquinone synthesis process, however, is energy and capital intensive with low efficiency. Electrochemically reducing oxygen (O 2 ) to H 2 O 2 with metal-free catalysts is considered a promising alternative. This work describes the two-electron oxygen reduction process from both thermodynamic and kinetic aspects and summarizes the designing rules for effective H 2 O 2 formation catalysts. This includes tuning the binding energy of the intermediate species, the concentration of dissociation active sites, and adjusting the dielectric constant of solvents. These principles are successfully applied to the design of various metal-free catalysts by proper structure engineering and heteroatom doping, which shows both high activity and efficiency. Furthermore, pH and temperature effects are presented with a view toward reaction optimization. An outlook of future challenges is also discussed.

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Section: Synthetic Approaches Of Metal‐free Two‐electron Orr Electrocatalystssupporting

confidence: 74%

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

Wang

James

Tour

2021

Adv Energy and Sustain Res

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“…The catalytic oxidation current of CP is tested at almost zero in the full range of potential, suggesting that the Ni species are active sites for highly efficient electrooxidation of HMF rather than carbon. In addition, the catalytic oxidation current onset potential of Ni(NS)/CP (1.33 V RHE ) is the lowest among all of the Ni catalysts (Figure 3 a), which indicates its highest electrocatalytic activity in the viewpoint of thermodynamics [31] …”

Section: Resultsmentioning

confidence: 98%

Highly Efficient Electro‐reforming of 5‐Hydroxymethylfurfural on Vertically Oriented Nickel Nanosheet/Carbon Hybrid Catalysts: Structure–Function Relationships

Zhang

et al. 2021

Angew Chem Int Ed

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132

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Ni‐promoted electrocatalytic biomass reforming has shown promising prospect in enabling high value‐added product synthesis. Here, we developed a novel hybrid catalyst with Ni nanosheet forests anchored on carbon paper. The hybrid catalyst exhibits high efficiency in electrooxidation of HMF to FDCA coupling with H2 production in high purity. The Ni nanosheets have small crystal grain sizes with abundant edges, which is able to deliver an efficient HMF oxidation to FDCA (selectivity >99 %) at low potential of 1.36 VRHE with high stability. The post‐reaction structure analysis reveals the Ni nanosheets would transfer electrons to carbon and readily turn into NiOx and Ni(OH)x during the reaction. DFT results suggest high valence Ni species would facilitate the chemical adsorption (activation) of HMF revealing the reaction pathway. This work emphasizes the importance of the precise control of Ni activity via atomic structure engineering.

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“…It was also reported that the 500 °C calcined‐ CB in air for 45 min exhibited a higher activity than the CBs calcined for 5, 15, 30 and 60 min. The specific H 2 O 2 production rate is around 5.93 mol m geo −2 h −1 with a battery power density of 360 Wm geo −2 , [66] and the C−O−C and −C were revealed to be the origin of the high activity towards H 2 O 2 production.…”

Section: Two‐electron Orr Over Carbon Nanomaterialsmentioning

confidence: 99%

Design Strategies of Non‐Noble Metal‐Based Electrocatalysts for Two‐Electron Oxygen Reduction to Hydrogen Peroxide

Zhao

Yuan

2021

ChemSusChem

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Hydrogen peroxide (H2O2) is a highly value‐added and environmentally friendly chemical with various applications. The production of H2O2 by electrocatalytic 2e− oxygen reduction reaction (ORR) has drawn considerable research attention, with a view to replacing the currently established anthraquinone process. Electrocatalysts with low cost, high activity, high selectivity, and superior stability are in high demand to realize precise control over electrochemical H2O2 synthesis by 2e− ORR and the feasible commercialization of this system. This Review introduces a comprehensive overview of non‐noble metal‐based catalysts for electrochemical oxygen reduction to afford H2O2, providing an insight into catalyst design and corresponding reaction mechanisms. It starts with an in‐depth discussion on the origins of 2e−/4e− selectivity towards ORR for catalysts. Recent advances in design strategies for non‐noble metal‐based catalysts, including carbon nanomaterials and transition metal‐based materials, for electrochemical oxygen reduction to H2O2 are then discussed, with an emphasis on the effects of electronic structure, nanostructure, and surface properties on catalytic performance. Finally, future challenges and opportunities are proposed for the further development of H2O2 electrogeneration through 2e− ORR, from the standpoints of mechanistic studies and practical application.

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Oxygen reduction to hydrogen peroxide on oxidized nanocarbon: Identification and quantification of active sites

Cited by 94 publications

References 62 publications

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

Highly Efficient Electro‐reforming of 5‐Hydroxymethylfurfural on Vertically Oriented Nickel Nanosheet/Carbon Hybrid Catalysts: Structure–Function Relationships

Design Strategies of Non‐Noble Metal‐Based Electrocatalysts for Two‐Electron Oxygen Reduction to Hydrogen Peroxide

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