A Directional Synthesis for Topological Defect in Carbon

Wang, Xin; Jia, Yi; Mao, Xin; Zhang, Longzhou; Liu, Daobin; Li, Song; Yan, Xuecheng; Chen, Jun; Yang, Dongjiang; Zhou, Jizhi; Wang, Kang; Du, Aijun; Yao, Xiangdong

doi:10.1016/j.chempr.2020.05.010

Cited by 138 publications

(142 citation statements)

References 44 publications

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“…These properties can also endow topological aberrant sites with local charge/spin redistribution of the carbon network (Fig. 4 a), leading to the enhanced electrocatalytic activity [ 51 , 90 ]. For example, Yao et al [ 91 ] investigated the ORR performance of pentagon–octagon–pentagon defect based on the monolayer graphene model (G585, Fig.…”

Section: Defect Inducingmentioning

confidence: 99%

“…Among all the topological defects in carbon materials, the unique pentagon defect tends to be more potential for ORR, in terms of the low reaction free energy, narrow band gap, high charge density along with high oxygen-binding ability based on DFT calculations (Fig. 4 i–k) [ 90 , 92 ]. In early 2015, Hu et al synthesized carbon nanocages using magnesium oxide as a template and benzene as the precursor.…”

Section: Defect Inducingmentioning

confidence: 99%

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Defect and Doping Co-Engineered Non-Metal Nanocarbon ORR Electrocatalyst

et al. 2021

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Exploring low-cost and earth-abundant oxygen reduction reaction (ORR) electrocatalyst is essential for fuel cells and metal–air batteries. Among them, non-metal nanocarbon with multiple advantages of low cost, abundance, high conductivity, good durability, and competitive activity has attracted intense interest in recent years. The enhanced ORR activities of the nanocarbons are normally thought to originate from heteroatom (e.g., N, B, P, or S) doping or various induced defects. However, in practice, carbon-based materials usually contain both dopants and defects. In this regard, in terms of the co-engineering of heteroatom doping and defect inducing, we present an overview of recent advances in developing non-metal carbon-based electrocatalysts for the ORR. The characteristics, ORR performance, and the related mechanism of these functionalized nanocarbons by heteroatom doping, defect inducing, and in particular their synergistic promotion effect are emphatically analyzed and discussed. Finally, the current issues and perspectives in developing carbon-based electrocatalysts from both of heteroatom doping and defect engineering are proposed. This review will be beneficial for the rational design and manufacturing of highly efficient carbon-based materials for electrocatalysis.

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Section: Defect Inducingmentioning

confidence: 99%

Section: Defect Inducingmentioning

confidence: 99%

Defect and Doping Co-Engineered Non-Metal Nanocarbon ORR Electrocatalyst

et al. 2021

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“…However, from the test results (Figure 4C, D), it can be seen that the specific N‐doped carbon was not the active center, and the carbon defects generated by the removal of specific N atoms showed more active in electrochemical reactions, whose activity was closely related to the defect type. Therefore, this work not only provides guidance for the design of carbon‐based catalysts by controlling defect synthesis, but also clarifies the real active sites in metal‐free catalysis [30] …”

Section: Defect Chemistrymentioning

confidence: 79%

Defect Chemistry on Electrode Materials for Electrochemical Energy Storage and Conversion

Zhang

Long

et al. 2020

ChemNanoMat

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Efficient and sustainable clean energy technology is an urgent need to solve energy crisis and alleviate environmental pollution. Reasonable design of electrode materials can effectively improve the performance of electrochemical energy storage and conversion devices. As an effective method to control the properties of electrode materials, defects have recently received extensive attention. Herein, in this review, we will systematically summarize the application of defect chemistry on electrode materials for electrochemical energy storage and conversion. Firstly, we mainly describe the research content of defect chemistry from three aspects, including defect construction, the dynamic evolution and regulation of defects. Based on those understanding, the applications of defect chemistry in fuel cells, metal‐ion batteries and carbon/nitrogen fixation are discussed, respectively. Finally, the existing challenges and future development prospects of defect chemistry are proposed. Overall, we hope this review could help readers to better understand and apply defect chemistry on electrode materials.

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“…Theoretically, the electrondonating capability of electrocatalysts determines the interfacial electronic transfer with oxygen intermediates, with an extensive effect on the oxygen reduction. 17,59 Generally, a catalyst with a small work function is more apt to undergo four proton-electron coupled steps, because electrons are effortless to escape from the catalyst surface. 32 According to the Ultraviolet Photoelectron Spectroscopy (UPS) spectra (Supplementary Figs.…”

Section: Resultsmentioning

confidence: 99%

Identify the impact of the covalent-bonded carbon matrix to FeN4 sites for acidic oxygen reduction

Xiang

2021

Preprint

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Atomically dispersed Fe and N co-doped carbon (Fe–N–C) catalysts exhibited superior acid oxygen reduction reaction (ORR) activities and recently been considered as the most promising alternatives to the benchmark Pt-based catalysts for proton exchange membrane fuel cells. The atomic configuration between Fe, N and C is one of the key factors to affect ORR activity. However, the traditional synthetic methods that rely on pyrolysis of the mixtures of Fe, N and C precursors often result in the plurality of local environment for the FeNx site. Unveiling the effect of covalent-bonded carbon matrix to FeNx sites towards ORR activity is important but still a great challenge due to inevitable connection of diverse N as well as random defects during the pyrolysis process. Here, we report a proof-of-concept study on the evaluation of covalent-bonded carbon environment connected to FeN4 sites on their catalytic activity via pyrolysis-free approach. Basing on the closed π conjugated phthalocyanine-based intrinsic covalent organic polymers (COPs) with well-designed structures, we directly synthesized a series of atomically dispersed Fe-N-C catalysts with various pure carbon environment without any N doping directly connected to the same FeN4 sites. Experiments coupled with density functional theory demonstrate that the catalytic activities appear a volcano plot with the increase of degree of delocalized π electrons from the carbon matrix. The delocalized π electrons changed anti-bonding d-state energy level of the single FeN4 moieties, hence tailored the adsorption between active centers and oxygen intermediates and altered the rate-determining step of oxygen reduction reaction.

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A Directional Synthesis for Topological Defect in Carbon

Cited by 138 publications

References 44 publications

Defect and Doping Co-Engineered Non-Metal Nanocarbon ORR Electrocatalyst

Defect and Doping Co-Engineered Non-Metal Nanocarbon ORR Electrocatalyst

Defect Chemistry on Electrode Materials for Electrochemical Energy Storage and Conversion

Identify the impact of the covalent-bonded carbon matrix to FeN4 sites for acidic oxygen reduction

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