Selective H2O2 electrosynthesis by O-doped and transition-metal-O-doped carbon cathodes via O2 electroreduction: A critical review

Zhou, Wei; Xie, Liang; Gao, Jihui; Nazari, Roya; Zhao, Haiqian; Meng, Xiaoxiao; Sun, Fei; Zhao, Guangbo; Ma, Jun

doi:10.1016/j.cej.2020.128368

Cited by 140 publications

(64 citation statements)

References 81 publications

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Section: Resultssupporting

confidence: 60%

“…This is further supported by the substantially lower selectivity of N-CNH, which has a high content of pyridinic-N and graphitic N that are likely the active sites toward the 4e − product. 60 While it has been established that tuning the O content is an effective design strategy, 61 our results suggest that incorporating the N dopant, particularly pyrrolic-N, on top of the O-dopant will distinctively further enhance the selectivity of carbon-based catalysts toward the 2e − ORR. Among all catalysts, O-CNH demonstrates the earliest onset potential due to its high defect density and a good selectivity for the 2e − product due to the presence of pyrrolic N. Thus, the catalyst stability and scalability for the electrochemical H 2 O 2 production from O 2 were further examined.…”

Section: ■ Results and Discussionmentioning

confidence: 73%

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Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

Chakthranont

Nitrathorn

Thongratkaew

et al. 2021

ACS Appl. Energy Mater.

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Electroreduction of O2 is a promising method for decentralized H2O2 production. Due to their high selectivity, low cost, and highly tunable properties, O- and N-doped carbon catalysts are appealing for this process. However, the relative effects of O and N dopants on the catalytic performances of carbon are not well understood. In this work, we present highly active and selective 2e– O2 reduction catalysts based on doped carbon nanohorns (CNH) synthesized by the gas-injected arc-in-water (GI-AIW) method. The effects of O and N dopants incorporated during the synthesis and the post-treatment are investigated. We discovered that the selectivity of CNH may be more sensitive to changes in N dopant than to changes in O dopant. Our doped CNH catalyst exhibits an early onset potential of 0.85 V vs RHE, >80% selectivity, and excellent stability even after 5,000 cycles and 12 h of flow electrolysis. Our gas diffusion device can generate H2O2 at a practical concentration of 56 mM per hour, corresponding to a production rate of 0.74 mol h–1 gcat –1. These results suggest that regulating both O and N dopants is an effective design strategy for an efficient carbon catalyst, which is essential in the electrosynthesis of H2O2 from O2.

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Section: Resultssupporting

confidence: 60%

Section: ■ Results and Discussionmentioning

confidence: 73%

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

Chakthranont

Nitrathorn

Thongratkaew

et al. 2021

ACS Appl. Energy Mater.

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“…The introduction of oxygen-containing functional group enables the carbon materials to achieve upper conductivity and electroactivity, as well as hydrophilicity which may accelerate the transportation of oxygen to the surface of electrocatalyst in liquid phase. [25,26] Besides, carbonyl, quinone, carboxyl, and ester groups were regarded as surface active sites for improving the electrochemical performance in Zhou's experiment, [27] and carboxyl (COOH), ether bond (COC) have been proved to be the active sites of the two-electron ORR pathway in Lu's study [28] with density functional calculation. B atoms, usually combined with nitrogen to fabricate h-BN domains, can weaken the bond between oxygen and carbon substrates and boost the protonation of OOH*, increasing the H 2 O 2 selectivity up to 85% in graphene with defects removed.…”

Section: Heteroatomic Doping and N-doped Carbon Electrocatalystsmentioning

confidence: 99%

“…At present, ORR reaction mechanisms promoted by N doping materials mainly focus on the following three aspects: 1) Dipole-Dipole Interaction (Figure 3A). It was found that the carbon atoms adjacent to nitrogen could display higher positive charge density, stronger electron affinity, and better catalytic activity; [19][20][21][22][23][24][25][26][27][28][29][30][31][32] 2) Nitrogen Hydrogenation (Figure 3B). Briega [33] found more than half of the nitrogen atoms would undergo a hydrogenation process (Equation ( 7)) at a particular initial potential, leading to the destabilization of adjacent carbon atoms.…”

Section: Heteroatomic Doping and N-doped Carbon Electrocatalystsmentioning

confidence: 99%

H₂O₂ Electrogeneration from O₂ Electroreduction by N‐Doped Carbon Materials: A Mini‐Review on Preparation Methods, Selectivity of N Sites, and Prospects

Ding

Zhou

Gao

et al. 2021

Adv Materials Inter

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promising and environmentally friendly oxidant in advanced oxidation processes (AOPs). Besides, hydrogen peroxide received great attention in fuel cell as well, in which hydrogen still plays an important role. But the low volumetric energy density makes the storage of hydrogen a difficult issue. H 2 O 2 possesses a high energy density and oxidation potential [13] in full pH range (E 0 = 1.763 V at pH = 0, E 0 = 0.878 V at pH 14), [1] which enables it an ideal energy carrier alternative. [11] With a compounded increase of 6%, [14] the annual production of H 2 O 2 had reached 5.5 million tons in 2015. [1] At present, three main categories were conducted to produce H 2 O 2 : direct H 2 O 2 synthesis from H 2 and O 2 , [15] anthraquinone oxidation process (AO-process), [12] and oxygen electroreduction. [16][17] More than 95% of H 2 O 2 were synthesized by AO-process, involving hydrogenation and oxidation of the anthraquinone molecule over Ni or Pd catalysts in organic solvents. [14] However, AO-process is facing some challenges: 1) Low sustainability. The combustible and explosive substances used in AO-process, such as heavy aromatics, trioctyl phosphate, are not environmentally friendly, which brings a negative influence on the sustainability of the AO-process; 2) Transportation insecurity. The high concentration of H 2 O 2 has the potential to explode when flammable materials exist, which brings safety problems to transportation; 3) Exorbitant additional cost. Ahead of being transported, H 2 O 2 has to be concentrated up to 70 wt% with impurity separation [18] and requires acid promoter stabilizer, [14] causing the increase of extra cost. All these make AO-process not the best choice for low cost and distributed H 2 O 2 production.Comparatively, two-electron oxygen reduction reaction (ORR) provides an economic, efficient, and nonhazardous alternative process, achieving the in situ H 2 O 2 production under mild conditions. [1] Furthermore, ORR process could be coupled with renewable energy sources [18] and fuel cell, [19] recovering the energy released ( f 0 ∆G , 120 KJ mol −1 ). [20,21] For instance, solar energy can be directly used as an energy source to produce H 2 O 2 through photoelectric catalysis. [22] In brief, H 2 O 2 production via two-electron oxygen electro-reduction has emerged as a promising candidate to address the demand for distributed energy.Hydrogen peroxide (H 2 O 2 ) is one of the 100 most paramount chemicals in the world, which has been widely used in industrial synthesis, pulp and bleaching, semiconductor cleaning, medical sterilizing, environmental treatments, and energy storage. Among various H 2 O 2 production methods, anthraquinone process has intrinsic drawbacks such as energy-intensive and environmental pollution while 2-electron oxygen reduction reaction (ORR) provides an economic, efficient, and nonhazardous alternative process to realize the in situ production of H 2 O 2 instead. Recently, heteroatom-doped carbon electrocatalysts, especially the nitrogen-doped ones, receive special a...

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“…H2O2 [52] 。Garcia-Rodriguez 等 [53] [52] 。氧基官能团(-COOH、-C=O、-OH、C-O-C 等) 作为 O2 电化学还原活性位点已被频繁报道 [56] 。有研究发现，具有亲水性的氧基官能团(-COOH、-COH、 -COO-、R-OH、>C=O)，易于接触电极表面产生溶解 O2 [57] 。同时，氧基官能团浓度和 H2O2 产量之间存在明显线性相关性 [58,59] 。Lu 等 [60]…”

Section: Figureunclassified

Research progress of carbon-based materials for electro-Fenton degradation of pollutants

Shen¹,

Yang²,

Zhu³

et al. 2021

Sci. Sin.-Chim

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Electro-Fenton process is one of the simple and effective methods for the treatment of organic pollutants in water. Carbon-based material serves as a robust cathode for in-situ formation of H2O2 via the two-electron O2 reduction reaction. With the help of Electro-Fenton catalysts, the generated H2O2 decomposed into strong oxidizing hydroxyl radicals for efficient mineralization of organic pollutants. Based on the analysis of the main Electro-Fenton processes on carbon-based materials, this review systematically summarizes the modification of various carbon-based electrode in an attempt to enhance O2 mass transfer and Fenton reaction. Moreover, the practical application and economic cost of carbon-based electrode in Electro-Fenton degradation of organic pollutants are described. The current development trend of carbon-based electrode materials and foreseeable future research direction in the field of Electro-Fenton pollution control are pointed out at the end.

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Selective H2O2 electrosynthesis by O-doped and transition-metal-O-doped carbon cathodes via O2 electroreduction: A critical review

Cited by 140 publications

References 81 publications

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

H₂O₂ Electrogeneration from O₂ Electroreduction by N‐Doped Carbon Materials: A Mini‐Review on Preparation Methods, Selectivity of N Sites, and Prospects

Research progress of carbon-based materials for electro-Fenton degradation of pollutants

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Selective H2O2 electrosynthesis by O-doped and transition-metal-O-doped carbon cathodes via O2 electroreduction: A critical review

Cited by 140 publications

References 81 publications

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H2O2 from O2 Reduction

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H2O2 from O2 Reduction

H2O2 Electrogeneration from O2 Electroreduction by N‐Doped Carbon Materials: A Mini‐Review on Preparation Methods, Selectivity of N Sites, and Prospects

Research progress of carbon-based materials for electro-Fenton degradation of pollutants

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Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

Rational Design of Metal-free Doped Carbon Nanohorn Catalysts for Efficient Electrosynthesis of H₂O₂ from O₂ Reduction

H₂O₂ Electrogeneration from O₂ Electroreduction by N‐Doped Carbon Materials: A Mini‐Review on Preparation Methods, Selectivity of N Sites, and Prospects