Fluorographdiyne: A Metal‐Free Catalyst for Applications in Water Reduction and Oxidation

Xing, Changrui; Xue, Yurui; Huang, Bolong; Yu, Hongwei; Hui, Lan; Fang, Yan; Liu, Yuxin; Zhao, Yingjie; Li, Zhibo; Li, Yuliang

doi:10.1002/ange.201905729

Cited by 37 publications

(18 citation statements)

References 57 publications

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“…As shown in Figure 4D, the newly‐developed metal‐free COOH‐3.9‐MWNTs exhibited outstanding OER performance in acidic conditions, outperformed most noble metal (e.g., Ir‐ and Ru)‐based catalysts. To the best of our knowledge, they represent the best metal‐free electrocatalysts for the acidic OER 21–25,31–36 . The methodology developed in this work could also be applied for the design and development of new carbon catalysts for OER and many other reactions.…”

Section: Resultsmentioning

confidence: 97%

“…Herein, we report a facile hydrothermal acid oxidation of CNTs to produce carboxyl‐enriched multiple‐walled carbon nanotubes (COOH‐MWNTs), which exhibited unprecedented OER performance in acidic conditions with a low overpotential of 265 mV at a current density of 10 mA cm –2 and a small Tafel slope of 82 mV dec –1 —better OER performance than that of any metal‐free electrocatalysts in acidic conditions reported to date 20–25 and comparable to those of the RuO 2 and IrO 2 benchmark catalysts. Our experimental observations combined with the theoretical calculations revealed a novel OER mechanism for the carboxyl‐enriched MWNTs catalysts, in which the carboxyl group lowers the energy barrier for water splitting via the formation and hydrolysis of a lactone.…”

Section: Introductionmentioning

confidence: 99%

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Carboxylated carbon nanotubes with high electrocatalytic activity for oxygen evolution in acidic conditions

Zhang

Dai

et al. 2021

InfoMat

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Since most electrocatalysts for oxygen evolution reaction (OER), except for precious metal oxides RuO2 and IrO2, are unstable in harsh acidic solutions, it is highly desirable to develop high‐performance OER electrocatalysts for acidic media, though it is still a big challenge. Herein, we report a simple strategy to produce carboxyl‐enriched multiwalled carbon nanotubes (COOH‐MWNTs) that exhibit stable and high electrocatalytic activities for OER in acidic solutions, showing an overpotential at a current density of 10 mA cm–2 and a Tafel slope as low as of 265 mV and 82 mV dec–1, respectively. As far as we are aware, these results represent the best OER performance for metal‐free electrocatalysts, even comparable to those of RuO2 and IrO2. We have further revealed the catalytic mechanism, which involves one electron lose from the COOH‐MWNTs catalyst at the beginning of the OER process to trigger H2O molecule oxidation by forming peralcohol, followed by the recapture of one electron from water molecule to oxidize water and to recover the initial state for the COOH‐MWNTs catalyst. The unravel of this new OER mechanism is important as it provides new insights into the crucial role of organic functional groups in electrocatalytic processes. Also, the mechanistic understanding can be used to guide the design and development of novel metal‐free catalysts for acidic OER electrocatalysis and beyond.

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Section: Resultsmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

Carboxylated carbon nanotubes with high electrocatalytic activity for oxygen evolution in acidic conditions

Zhang

Dai

et al. 2021

InfoMat

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“…The fluoro-GDY nanostructures on a carbon cloth (p-F-GDY/CC) network exhibited good performance as bifunctional catalysts for both HER and OER, as well as overall water splitting (OWS) under both acidic and alkaline conditions (Figure 7). 37 In the HER process, p-F-GDY/CC exhibited low onset overpotentials of 82 and 92 mV (versus the reversible hydrogen electrode) to achieve 10 mA cm −2 in both alkaline and acidic conditions, comparable to the metal-based catalysts. Extremely long stability over 8500 cycles in 1.0 M KOH verified the dramatic stability of F-GDY during the HER process.…”

Section: Heteroatom Dopingmentioning

confidence: 99%

“…(a) Schematic structure of F-GDY, (b) photograph of the p-F-GDY/CC material, (c) polarization curves of the catalysts for HER in 1.0 M KOH, (d) long-term stability tests of the p-F-GDY/CC in 1.0 M KOH during the HER process. Reproduced with permission from ref . Copyright 2019 Wiley-VCH.…”

Section: Application On Electrochemical Catalysismentioning

confidence: 99%

Fundament and Application of Graphdiyne in Electrochemical Energy

et al. 2020

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Conspectus The artificial synthesis of graphdiyne (GDY) in 2010 successfully fills the blank of low temperature preparation of all-carbon allotropes. GDY is an emerging two-dimensional (2D) planar carbon material composed of benzene rings moieties (sp2 carbon atoms), butadiyne (sp carbon atoms) linkers, and well dispersed electron-rich cavities, forming a large π-conjunction structure. GDY has attracted increasing attention in many fields. GDY is the first carbon material with both 2D fast transfer channels for electrons and 3D channels for ions. The 2D electron-rich all-carbon nature endows GDY with considerable conductivity and tunable electronic properties, and the in-plane cavities give it intrinsic selectivity and accessibility for electrochemically active metal ions. In addition, its easy preparation under mild conditions well complements the disadvantages of the traditional sp2-hybridized carbon materials (carbon nanotubes, graphene, and graphite) in the highly efficient synthesis and processing for potential electrochemical applications. As an all-carbon material, the unique advantages of GDY in both structure and preparation match well the urgent demands in key materials for solving many challenging problems in recent electrochemical areas and beyond. During the last decade since the first preparation of GDY, it has already achieved much enlightening and creative progress in both fundamental scientific research and forward-looking applications. This Account is intended not to summarize all this progress in preparation and applications but to outline some newly reported interesting phenomena in both high-quality preparation and electrochemical applications. This Account mainly discusses the recent progress in electrochemical applications: (i) constructing new concepts and new functions in electrochemical interfaces for realizing highly active electrochemical catalysts in the fields of water splitting and oxygen reduction reaction and (ii) building a highly stable conductive network and electrochemical interface for reversible energy storage. In the field of electrochemical catalysis, based on current studies of structural advantages and superior performance, atomic catalysis with metal atoms anchored in GDY is encouraging, owing to the desirable immobilizing capability of electron-rich dialkyne cavities toward metal atoms and corresponding electron transfer. For high-energy batteries, the in situ growth of the all-carbon GDY on the various battery electrodes shows great promise for solving key practical problems (safety, long lifespan, high power), which are ascribed to weak interfacial stability. In addition, the perspective application of GDY to broader interfacial modifications is described, bringing new choices for solving the interfacial challenges in various energy storage devices.

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“…In the further study of GDY, it is found that due to the unique preparation process of GDY, the bottom-up synthesis method can be adopted for doping various heteroatoms into GDY qualitatively and quantitatively, which is conducive to improve the electrochemical behavior of GDY. To date, a variety of elements and groups have been successfully doped into GDY including H, Cl, F, N, CH 3 , NH, etc., − and greatly changed the electrochemical performance of GDY. Both the heteroatoms substituting the carbon atoms in the benzene ring and the impurity groups replacing the acetylene chain make the morphological characteristics of GDY change from a combination of benzene rings and triangular apertures into a nanosheet consisting of benzene rings and hexagonal apertures.…”

Section: Introductionmentioning

confidence: 99%

Enabling Enhanced Lithium Ion Storage Performance of Graphdiyne by Doping with Group-15 Elements: A First-Principles Study

Huang

2021

ACS Omega

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As a typical two-dimensional material possessing sp and sp 2 hybrid orbitals, graphdiyne (GDY) and its derivatives have been proposed as an attractive candidate for high-performance lithium ion batteries (LIBs). In this work, an advanced GDY LIB electrode is designed by doping with group-15 elements. With the aid of first-principles simulations, the geometric properties, electronic structures, theoretical storage capacities, open-circuit voltages, and diffusion path of Li atoms on doped GDY are comprehensively investigated. Specifically, 14 different adsorption sites are proposed, most of which are situated out of plane of the carbon network, resulting from the out of plane Pz orbitals of conduction band minimum and valence band maximum. Among the five doped GDY, phosphorusdoped graphdiyne (P-GDY) exhibits prominent lithium ion storage behavior, i.e., the maximum theoretical capacity is 1949 mA•h• g −1 , which is ∼2.6 times higher than that of GDY. Moreover, calculation results in terms of the in-plane migration of lithium ion on P-GDY indicate that Li atoms prefer to diffuse across the carbon network (with a moderate barrier of 0.46 eV) rather than directly through the middle of the hexagonal aperture (with a higher barrier of 1.78 eV). Thus, this approach provides novel insights into the Li ion storage properties of group-15 element-doped GDY from the prospect of theoretical calculations, which would be useful to guide the future design of high-capacity GDY anodes for LIBs.

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Fluorographdiyne: A Metal‐Free Catalyst for Applications in Water Reduction and Oxidation

Cited by 37 publications

References 57 publications

Carboxylated carbon nanotubes with high electrocatalytic activity for oxygen evolution in acidic conditions

Carboxylated carbon nanotubes with high electrocatalytic activity for oxygen evolution in acidic conditions

Fundament and Application of Graphdiyne in Electrochemical Energy

Enabling Enhanced Lithium Ion Storage Performance of Graphdiyne by Doping with Group-15 Elements: A First-Principles Study

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