Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H<sub>2</sub>O<sub>2</sub>

Chang, Jia‐Nan; Li, Qi; Shi, Jingwen; Zhang, Mi; Zhang, Lei; Li, Shan; Chen, Yifa; Li, Shun-Li; Lan, Ya‐Qian

doi:10.1002/ange.202218868

“…The ring potential was fixed at 1.2 V versus a reversible hydrogen electrode (RHE) to collect the produced H 2 O 2 . All potentials measured against the SCE were converted to the RHE scale using Eqn (5). The selectivity of H 2 O 2 can be calculated based on Eqn (6) 14 :…”

Section: Characterizationmentioning

confidence: 99%

“…3,4 The production of H 2 O 2 has increased in recent years, reaching 6.5 million tons by 2022. 5 At present, the main production method of H 2 O 2 is the anthraquinone process. 6,7 However, this method necessitates costly catalysts and time-consuming reactant extraction steps.…”

Section: Introductionmentioning

confidence: 99%

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Hydrogen peroxide electrosynthesis with nickel foam electrodes: influence mechanism of surface oxidation

Zhao,

Ding,

Zhu

et al. 2023

J of Chemical Tech & Biotech

0

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BACKGROUNDNickel foam (NF) is widely used as battery electrode matrix and electrochemical process cathode. However, the surface of NF is prone to oxidation, which may affect its ability to reduce oxygen and produce H2O2, but the influence mechanism is still unclear. In this paper, surface oxidation of the NF was regulated by pickling and drying pretreatment, and the surface oxides were characterized by X‐ray photoelectron spectroscopy (XPS) and energy dispersive X‐ray spectrometry (EDS). The NF was used as the substrate, graphite powder as the catalyst, and PTFE as the binder to prepare graphite‐coated NF composite electrodes. The effect of NF surface oxidation on their ability to generate H2O2 was investigated.RESULTSThe results demonstrated that after pickling and drying, the NF surface generated a large amount of NiO, which increased the charge transfer resistance of the NF by 20.3%, and accelerated further reduction decomposition of H2O2. The rotating ring‐disk electrode (RRDE) tests further confirmed that NiO can reduce the two‐electron oxygen reaction selectivity, which was detrimental to H2O2 electrosynthesis. The graphite‐coated NF composite electrode with pristine NF as the substrate can produce 869.1 mg L−1 of H2O2 and maintain relatively good reusability.CONCLUSIONOverall, the surface oxidation of NF is not conducive to H2O2 electrosynthesis, and it is necessary to prevent oxidation during electrode preparation. This study provides a valuable reference for the preparation of NF electrodes and can promote the further study of in situ H2O2 electrosynthesis. © 2023 Society of Chemical Industry (SCI).

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12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis

Wang,

Jin,

Li

et al. 2024

Angewandte Chemie

0

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Developing high connectivity (>8) three‐dimensional (3D) covalent organic frameworks (COFs) towards new topologies and functions remains a great challenge owing to the difficulty in getting high connectivity organic building blocks. This however represents the most important step towards promoting the diversity of COFs due to the still limited dynamic covalent bonds available for constructing COFs at this stage. Herein, highly connected phthalocyanine‐based (Pc‐based) 3D COFs MPc‐THHI‐COFs (M = H2, Ni) were afforded from the reaction between 2,3,9,10,16,17,23,24‐octacarboxyphthalocyanine M(TAPc) (M = H2, Ni) and 5,5',5'',5''',5'''',5'''''‐(triphenylene‐2,3,6,7,10,11‐hexayl)hexa(isophthalohydrazide) (THHI) with 12 connecting sites. Powder X‐ray diffraction analysis together with theoretical simulations and transmission electron microscopy reveals their crystalline nature with an unprecedented non‐interpenetrated shp topology. Experimental and theoretical investigations disclose the broadened visible light absorption range and narrow optical band gap of MPc‐THHI‐COFs. This in combination with their 3D nanochannels endows them with efficient photocatalysis performance for H2O2 generation from O2 and H2O via 2e− oxygen reduction reaction and 2e− water oxidation reaction under visible‐light irradiation (λ > 400 nm). This work provides valuable result for the development of high connectivity functional COFs towards diverse application potentials.

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12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis

Wang,

Jin,

Li

et al. 2024

Angew Chem Int Ed

4

0

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Developing high connectivity (>8) three‐dimensional (3D) covalent organic frameworks (COFs) towards new topologies and functions remains a great challenge owing to the difficulty in getting high connectivity organic building blocks. This however represents the most important step towards promoting the diversity of COFs due to the still limited dynamic covalent bonds available for constructing COFs at this stage. Herein, highly connected phthalocyanine‐based (Pc‐based) 3D COFs MPc‐THHI‐COFs (M = H2, Ni) were afforded from the reaction between 2,3,9,10,16,17,23,24‐octacarboxyphthalocyanine M(TAPc) (M = H2, Ni) and 5,5',5'',5''',5'''',5'''''‐(triphenylene‐2,3,6,7,10,11‐hexayl)hexa(isophthalohydrazide) (THHI) with 12 connecting sites. Powder X‐ray diffraction analysis together with theoretical simulations and transmission electron microscopy reveals their crystalline nature with an unprecedented non‐interpenetrated shp topology. Experimental and theoretical investigations disclose the broadened visible light absorption range and narrow optical band gap of MPc‐THHI‐COFs. This in combination with their 3D nanochannels endows them with efficient photocatalysis performance for H2O2 generation from O2 and H2O via 2e− oxygen reduction reaction and 2e− water oxidation reaction under visible‐light irradiation (λ > 400 nm). This work provides valuable result for the development of high connectivity functional COFs towards diverse application potentials.

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Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H₂O₂

Cited by 4 publications

References 67 publications

Hydrogen peroxide electrosynthesis with nickel foam electrodes: influence mechanism of surface oxidation

Hydrogen peroxide electrosynthesis with nickel foam electrodes: influence mechanism of surface oxidation

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis

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Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H2O2

Cited by 4 publications

References 67 publications

Hydrogen peroxide electrosynthesis with nickel foam electrodes: influence mechanism of surface oxidation

Hydrogen peroxide electrosynthesis with nickel foam electrodes: influence mechanism of surface oxidation

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H2O2 Synthesis

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H2O2 Synthesis

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Product

Resources

About

Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H₂O₂

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis

12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H₂O₂ Synthesis