Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study

Lin, Yangming; Wu, Kuang‐Hsu; Lü, Qing; Gu, Qingqing; Zhang, Liyun; Zhang, Bingsen; Plodinec, Milivoj; Schlögl, Robert; Heumann, Saskia

doi:10.1021/jacs.8b07627

Cited by 56 publications

(44 citation statements)

References 48 publications

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“…After careful deconvolution with the same standard rules, four distinct regions were identified. To easily distinguish them, we labelled them O I (531.35 ± 0.05 eV, C=O related groups) 46,47 , O II (532.8 eV, C-O-C or COOH) 46,47 , O III (534.0 eV, C-O(H)) 46 , and O IV (535.6 eV, physically adsorbed H 2 O and O 2 ) 41,42 . Because the different groups overlap, it was difficult to determine the contents of the groups by O 1s alone.…”

Section: Photon Energy (Ev)mentioning

confidence: 99%

Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

et al. 2020

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The one-step electrochemical synthesis of H 2 O 2 is an on-site method that reduces dependence on the energy-intensive anthraquinone process. Oxidized carbon materials have proven to be promising catalysts due to their low cost and facile synthetic procedures. However, the nature of the active sites is still controversial, and direct experimental evidence is presently lacking. Here, we activate a carbon material with dangling edge sites and then decorate them with targeted functional groups. We show that quinone-enriched samples exhibit high selectivity and activity with a H 2 O 2 yield ratio of up to 97.8 % at 0.75 V vs. RHE. Using density functional theory calculations, we identify the activity trends of different possible quinone functional groups in the edge and basal plane of the carbon nanostructure and determine the most active motif. Our findings provide guidelines for designing carbon-based catalysts, which have simultaneous high selectivity and activity for H 2 O 2 synthesis.

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Section: Photon Energy (Ev)mentioning

confidence: 99%

Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

et al. 2020

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“…These redox peak positions of PQ and PYT monomers were in accordance with the aforementioned CV results for 2KT-Tp COF and 4KT-Tp COF (Figure 4a), indicating a similar electron transfer process during the charge-discharge cycles. According to the previous studies on the orthoquinone derivatives and corresponding polymers [46][47][48][49] combined with the electrochemical behaviors of PQ and PYT monomers, the possible redox mechanisms of 2KT-Tp COF and 4KT-Tp COF are summarized in Supporting Information Figure S33.…”

Section: Supercapacitor Performancementioning

confidence: 99%

Skeleton Engineering of Isostructural 2D Covalent Organic Frameworks: Orthoquinone Redox-Active Sites Enhanced Energy Storage

Liu

et al. 2021

CCS Chem

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The integration of redox-active sites into the skeleton of open-framework materials is an efficient strategy toward high-performance organic electrodes for energy storage devices. In this work, stepwise introduction of ketone (KT) groups to the skeletons of isostructural two-dimensional (2D) covalent organic frameworks (COFs) was realized by the condensation of 2,4,6-triformylphloroglucinol (Tp, as nodes) with a series of ditopic diamines, which contained none, one, two, and four KT moieties in each linker units, respectively. The precise control of the redox functionalities at the molecular level, combined with regular built-in channels in these KT-Tp COFs endowed them with superior capacitances and excellent rate capabilities for energy storage. In particular, 2KT-Tp COF and 4KT-Tp COF electrodes exhibited high capacitances of 256 and 583 F g −1 at a discharge rate of 0.2 A g −1 , respectively, which outperformed most reported COF-based electrodes. More importantly, exceptional long-term cyclabilities (> 92% capacitance retention) were achieved even after 20,000 cycles at a high current density of 5 A g −1 for these KT-Tp COFs. Our results demonstrated that orthoquinone moieties rendered enhanced performance than the redox COFs with isolated carbonyl groups.

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“…This technique features a collection ring electrode in a mass transport controlled system, offering detection and discrimination of reaction products in only a few seconds [16–17] . Recent progress has appreciated the use of RRDE in the gas‐evolving water oxidation reaction, [18–19] whereas only very limited success is witnessed in the CO 2 RR [10,20] . The key challenges reside at the real‐time product discrimination, signal interference and product collection efficiency, which are immediate issues from using a Pt ring electrode, although some plausible solutions to the problems are left undiscussed.…”

Section: Introductionmentioning

confidence: 99%

Real‐Time Carbon Monoxide Detection using a Rotating Gold Ring Electrode: A Feasibility Study

Zhang

Lin

et al. 2020

ChemElectroChem

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Dedication to the late of Professor Dang Sheng Su and for his contribution in nanocarbons for electrocatalysis Rotating ring-disc electrodes (RRDEs) offer a powerful electroanalytical method for studying electrochemical reactions with continuous real-time feedback capabilities. However, its use in the electrochemical CO 2 reduction reaction (CO 2 RR) sees very limited success despite the method being a sensible choice. Here, we assess the use of commercial polycrystalline Pt and Au ring electrodes for the selective detection of CO in a nearneutral NaHCO 3 electrolyte (pH = 7.5) and their suitability for real-time monitoring during the CO 2 RR. Our results show that the commercial Pt ring electrode, as a highly sensitive detector, cannot discriminate among most of C 1 reduction products such as H 2 , CO, formate, formaldehyde and methanol, whereas the Au ring electrode can satisfy many criteria for real-time CO detection but the poor sensitivity of the polycrystalline electrode prohibits the practical use for quantitative purpose. A set of design principles for the Au-based ring electrode is put forward in order to endow RRDEs the capability of rapid realtime detection of CO in CO 2 electroreduction.

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Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study

Cited by 56 publications

References 48 publications

Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

Skeleton Engineering of Isostructural 2D Covalent Organic Frameworks: Orthoquinone Redox-Active Sites Enhanced Energy Storage

Real‐Time Carbon Monoxide Detection using a Rotating Gold Ring Electrode: A Feasibility Study

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