Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon

Chang, Qiaowan; Zhang, Pu; Mostaghimi, Amir Hassan Bagherzadeh; Zhao, Xinbing; Denny, Steven R.; Lee, Ji Hoon; Gao, Hongpeng; Zhang, Ying; Xin, Huolin L.; Siahrostami, Samira; Chen, Jingguang G.; Chen, Zheng

doi:10.1038/s41467-020-15843-3

Cited by 245 publications

(167 citation statements)

References 44 publications

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“…reported a Pd δ + –OCNT electrocatalyst with nearly 100% selectivity toward H 2 O 2 electrochemical production and a high mass activity (1.946 A mg −1 at 0.45 V) in acidic electrolyte ( Figure a). [ 20 ] The X‐ray absorption fine structure characterization and DFT calculations demonstrate that the synergistic interaction between partially oxidized Pd clusters and oxygen‐functionalized CNT substrate is crucial for the high 2e − ORR catalytic activity. Various other Pd/C catalysts displayed highly selectivity toward H 2 O 2 production.…”

Section: Electrocatalysts and Factors Influencing 2e− Orr Activity/selectivitymentioning

confidence: 99%

Recent Progress of Electrochemical Production of Hydrogen Peroxide by Two‐Electron Oxygen Reduction Reaction

et al. 2021

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Shifting electrochemical oxygen reduction reaction (ORR) via two‐electron pathway becomes increasingly crucial as an alternative/green method for hydrogen peroxide (H2O2) generation. Here, the development of 2e− ORR catalysts in recent years is reviewed, in aspects of reaction mechanism exploration, types of high‐performance catalysts, factors to influence catalytic performance, and potential applications of 2e− ORR. Based on the previous theoretical and experimental studies, the underlying 2e− ORR catalytic mechanism is firstly unveiled, in aspect of reaction pathway, thermodynamic free energy diagram, limiting potential, and volcano plots. Then, various types of efficient catalysts for producing H2O2 via 2e− ORR pathway are summarized. Additionally, the catalytic active sites and factors to influence catalysts’ performance, such as electronic structure, carbon defect, functional groups (O, N, B, S, F etc.), synergistic effect, and others (pH, pore structure, steric hindrance effect, etc.) are discussed. The H2O2 electrogeneration via 2e− ORR also has various potential applications in wastewater treatment, disinfection, organics degradation, and energy storage. Finally, potential future directions and prospects in 2e− ORR catalysts for electrochemically producing H2O2 are examined. These insights may help develop highly active/selective 2e− ORR catalysts and shape the potential application of this electrochemical H2O2 producing method.

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Section: Electrocatalysts and Factors Influencing 2e− Orr Activity/selectivitymentioning

confidence: 99%

Recent Progress of Electrochemical Production of Hydrogen Peroxide by Two‐Electron Oxygen Reduction Reaction

et al. 2021

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“…The possible impacts of these trace amount of O dopants on our samples' ORR performances were successfully excluded in our later discussions. Defects in carbon materials is another factor that we need to take into consideration when we analyze the origin of H 2 O 2 selectivity in B-C 17,25 . Raman spectroscopy was utilized to examine whether the doping process increases or decreases the concentration of defects in the CB support.…”

Section: Catalysts Preparation and Characterizationsmentioning

confidence: 99%

“…As O 2 molecules can also be fully reduced to H 2 O via a 4e − transfer process [12][13][14] , which is the preferred pathway in fuel cell applications, developing highly selective and active 2e − -ORR catalysts is the prerequisite of this sustainable synthetic route. Metal-based catalysts including noble metals and their alloys have been demonstrated to be selective for H 2 O 2 [15][16][17][18][19][20] . However, the cost and scarcity of noble metal elements make it difficult for future large-scale deployments.…”

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confidence: 99%

Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates

et al. 2021

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Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm−2) while maintaining high H2O2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H2O2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H2O2 solutions with high selectivity (up to 95%) and high H2O2 partial currents (up to ~400 mA cm−2), illustrating the catalyst’s great potential for practical applications in the future.

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“…H 2 O 2 is one of the very few chemicals that attract research interest in both energy and environmental contexts [1–7] . It has been widely used for pulp and textile bleaching, as a first‐aid disinfectant, in advanced oxidation processes (AOPs) for wastewater treatment, hydrometallurgy, and the electronics industry [8] .…”

Section: Introductionmentioning

confidence: 99%

Electrochemical and Photoelectrochemical Water Oxidation for Hydrogen Peroxide Production

et al. 2021

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Hydrogen peroxide (H2O2), as a green fuel and oxidant, has drawn increasing attention in the energy and environmental research. Compared with the traditional anthraquinone process, the electrochemical (EC) and photoelectrochemical (PEC) syntheses of H2O2 are cost‐effective and environmentally friendly. In order to construct membraneless EC/PEC devices for the full H2O2 synthesis, anodic H2O2 production by water oxidation, which is less developed than cathodic H2O2 generation, is highly desirable. Here, we review recent developments for the EC/PEC H2O2 production by water oxidation, including fundamental aspects, benchmarking activity evaluation, material/catalyst selection, and strategies for increasing selectivity, efficiency, and accumulation. Furthermore, we discuss the challenges and outlook of water oxidation for H2O2 production, especially device‐level development, accumulation and stability, and industrial applications. Our review is intended to stimulate studies further improving EC/PEC H2O2 production.

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Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon

Cited by 245 publications

References 44 publications

Recent Progress of Electrochemical Production of Hydrogen Peroxide by Two‐Electron Oxygen Reduction Reaction

Recent Progress of Electrochemical Production of Hydrogen Peroxide by Two‐Electron Oxygen Reduction Reaction

Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates

Electrochemical and Photoelectrochemical Water Oxidation for Hydrogen Peroxide Production

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