Synergistic effect of doped nitrogen and oxygen-containing functional groups on electrochemical synthesis of hydrogen peroxide

Bao, Zhikang; Zhao, Jinyan; Zhang, Shijie; Ding, Lei; Peng, Xiaoge; Wang, Guoliang; Zhao, Zijiang; Zhong, Xing; Yao, Zihao; Wang, Jianguo

doi:10.1039/d1ta09915a

Cited by 45 publications

(25 citation statements)

References 47 publications

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“…(H) Stability testing of 30% Ag‐TCNQ/rGO assembled GDE for 10 h at 0.267 V (vs. RHE), and the inset shows LSV before and after testing. (I) H 2 O 2 yield rate comparison of as‐prepared catalysts with reported ones (References 30–41)…”

Section: Resultsmentioning

confidence: 99%

Dynamic gas‐diffusion electrodes for oxygen electroreduction to hydrogen peroxide

Xia

Huang

et al. 2023

AIChE Journal

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Flow‐type electrolytic cell is a viable system for many electrochemical processes, in which gas‐diffusion electrode (GDE) plays a vital role in providing optimal reacting interfaces for improved performances. Different from traditional GDEs with fixed porosity, here we propose a new type of GDE that features flexible diffusion channels. Particularly, the GDE has been assembled by pairing PTFE substrate with Ag‐TCNQ/graphene hydrogels that can be further manipulated through capillary compression. With dynamic adjustment, the average pore size inside GDE ranges from 1750 to 125 nm, and the packing density varies from 56.81 to 446.07 mg cm−3. As a consequence, the as‐assembled flow‐type electrolytic cell can display excellent performances, with a yield rate of 5572 mmol gcat−1 h−1 and Faradic efficiency of 86.4% at 0.267 V (vs. RHE). In addition, a photovoltaic (PV)‐driven flow‐electrolytic system has been assembled that achieves a record solar‐to‐hydrogen peroxide efficiency of 14.8%.

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Section: Resultsmentioning

confidence: 99%

Dynamic gas‐diffusion electrodes for oxygen electroreduction to hydrogen peroxide

Xia

Huang

et al. 2023

AIChE Journal

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“…284.5, 285.2, and 288.5 eV, which can be assigned to three carbon species, including C=C, C=N/C−N, and C-O, respectively (Figure S8). 32 In addition, the high-resolution O 1s spectra are deconvoluted into three peaks, corresponding to C=O (531.0 eV), C−O−C/O=C−O (532.4eV), and C−OH (533.7 eV); 33 and their contents are on a similar level (Table S2 and Figure S9). The presence of different N species was also con rmed using N K-edge X-ray absorption near edge structure (XANES) spectra.…”

Section: Resultsmentioning

confidence: 99%

“…0.6 V vs. reversible hydrogen electrode (RHE), which is absent in the Ar-saturated electrolyte, indicating the capability of the material for catalyzing ORR. 33 Subsequently, linear sweep voltammetry (LSV) was conducted on a rotating ring-disc electrode to further assess the 2e − -ORR performance of the materials. As shown in the corresponding LSV curves of the materials (Figure 3b), P-NMG-10 has the largest ring current and the smallest disk current, indicating that it is more inclined to the 2e − -ORR pathway.…”

Section: Resultsmentioning

confidence: 99%

Kinetically Facilitating Two-electron Oxygen Reduction by the Synergy of Multiple Pyrrolic Nitrogen Sites for Ultra-high-yield Electrochemical Hydrogen Peroxide Production

Wei

Liu

et al. 2022

Preprint

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Electrocatalytic hydrogen peroxide (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 high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. Addressing this, we herein report a synergy of multiple pyrrolic N sites located on a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e−-ORR catalysis. The coordination of pyrrolic N sites effectively modulates the adsorption configuration of the *OOH species and reduces the reaction barrier for 2e−-ORR, thus providing a kinetically favorable pathway for H2O2 production, as demonstrated by a combined explicit solution model and slow-growth approach investigation. Consequently, a record-high H2O2 yield of up to 30 mol g−1 h−1 has been achieved on this material, together with a satisfactory Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L−1. This strategy of manipulating the adsorption configuration of reactants by the synergy of multiple non-metal active sites thus provides a highly efficient and durable metal-free electrocatalyst for 2e−-ORR with high practical feasibility.

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“…Hydrogen peroxide (H 2 O 2 ) is regarded as one of the most significant chemical compounds [ 1 , 2 , 3 ]. It is serves as both a desirable energy carrier and a green oxidant and disinfectant.…”

Section: Introductionmentioning

confidence: 99%

Promotion of the Efficient Electrocatalytic Production of H2O2 by N,O- Co-Doped Porous Carbon

Sun

Huo

et al. 2023

Nanomaterials

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H2O2 generation via an electrochemical two-electron oxygen reduction (2e− ORR) is a potential candidate to replace the industrial anthraquinone process. In this study, porous carbon catalysts co-doped by nitrogen and oxygen are successfully synthesized by the pyrolysis and oxidation of a ZIF-67 precursor. The catalyst exhibits a selectivity of ~83.1% for 2e− ORR, with the electron-transferring number approaching 2.33, and generation rate of 2909.79 mmol g−1 h−1 at 0.36 V (vs. RHE) in KOH solution (0.1 M). The results prove that graphitic N and –COOH functional groups act as the catalytic centers for this reaction, and the two functional groups work together to greatly enhance the performance of 2e− ORR. In addition, the introduction of the –COOH functional group increases the hydrophilicity and the zeta potential of the carbon materials, which also promotes the 2e− ORR. The study provides a new understanding of the production of H2O2 by electrocatalytic oxygen reduction with MOF-derived carbon catalysts.

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Synergistic effect of doped nitrogen and oxygen-containing functional groups on electrochemical synthesis of hydrogen peroxide

Abstract: Electrocatalytic production of hydrogen peroxide (H2O2) by 2e- oxygen reduction (ORR) is a clean on-site method. Although doped carbon materials have been widely used in hydrogen peroxide research, few studies...

Cited by 45 publications

References 47 publications

Dynamic gas‐diffusion electrodes for oxygen electroreduction to hydrogen peroxide

Dynamic gas‐diffusion electrodes for oxygen electroreduction to hydrogen peroxide

Kinetically Facilitating Two-electron Oxygen Reduction by the Synergy of Multiple Pyrrolic Nitrogen Sites for Ultra-high-yield Electrochemical Hydrogen Peroxide Production

Promotion of the Efficient Electrocatalytic Production of H2O2 by N,O- Co-Doped Porous Carbon

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