Defect engineering in carbon materials for electrochemical energy storage and catalytic conversion

Zhao, Zhiqiang; Chen, Huan; Zhang, Wanyu; Yi, Shan; Chen, Hongli; Su, Zhe; Niu, Bo; Zhang, Yayun; Long, Donghui

doi:10.1039/d2ma01009g

Cited by 22 publications

(17 citation statements)

References 284 publications

(519 reference statements)

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“…Despite the fact that charge and geometric structure regulation of the metal active site could enhance the catalytic activity of SMACs, few studies have focused on the effect of structural elements other than metal sites on catalytic activity. Defects are one of the structural elements which largely affect the catalytic properties of nanomaterials [19] . The rich defect structure can effectively increase the exposure of metal sites and activate the redox activity of the sites by changing the charge and energy distribution [20] .…”

Section: Catalysis Regulation Of Smacsmentioning

confidence: 99%

Designing Efficient Single Metal Atom Biocatalysts at the Atomic Structure Level

Liu,

Zhao,

Zhao

2024

Angewandte Chemie

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Various nanomaterials as biocatalysts could be custom‐designed and modified to precisely match the specific microenvironment of diseases, showing a promise in achieving effective therapy outcome. Compared to conventional biocatalysts, single metal atom catalysts (SMACs) with the maximized atom utilization through well‐defined structures offer enhanced catalytic activity and selectivity and enable the exploration of catalytic activity and the examination of structure‐mechanism interactions. There is still a gap in the comprehensive overview encompassing the interplay among the structure, catalytic mechanism, and biomedical applications of SMACs. Therefore, it is crucial to deeply investigate the role of SMACs in biocatalysis from the atomic structure level and to elucidate their potential mechanisms in biocatalytic processes. In this mini‐review, we summarize catalysis regulation methods of SMACs at the atomic structure level, focusing on the optimization of catalytic active sites, coordination environment, and active site‐support interactions, and discuss biocatalytic mechanisms for biomedical applications.

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Section: Catalysis Regulation Of Smacsmentioning

confidence: 99%

Designing Efficient Single Metal Atom Biocatalysts at the Atomic Structure Level

Liu,

Zhao,

Zhao

2024

Angewandte Chemie

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“…[27,28] However, excessive defects may influence the Fermi level and electronic structure, raising the material's electrical conductivity, which is beneficial for improving the overall electrochemical performance of the electrode. [29,30] As illustrated in the HR-TEM pattern in Figure 1f-h, the margins of the crystalline fringes are discontinuous, which might result in a significant number of defects. The lattice interplanar distance is precisely determined using digital microscopy software (Figure 1i).…”

Section: Synthesis Of Mof-derived 𝜶-/𝜸-Mns@co X S Y @N S─c -Electrodesmentioning

confidence: 99%

Electronic Structure Engineered Heteroatom Doped All Transition Metal Sulfide Carbon Confined Heterostructure for Extrinsic Pseudocapacitor

Patil

Moon

Roy

et al. 2023

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Ultra‐high energy density battery‐type materials are promising candidates for supercapacitors (SCs); however, slow ion kinetics and significant volume expansion remain major barriers to their practical applications. To address these issues, hierarchical lattice distorted α‐/γ‐MnS@CoxSy core‐shell heterostructure constrained in the sulphur (S), nitrogen (N) co‐doped carbon (C) metal‐organic frameworks (MOFs) derived nanosheets (α‐/γ‐MnS@CoxSy@N, SC) have been developed. The coordination bonding among CoxSy, and α‐/γ‐MnS nanoparticles at the interfaces and the π–π stacking interactions developed across α‐/γ‐MnS@CoxSy and N, SC restrict volume expansion during cycling. Furthermore, the porous lattice distorted heteroatom‐enriched nanosheets contain a sufficient number of active sites to allow for efficient electron transportation. Density functional theory (DFT) confirms the significant change in electronic states caused by heteroatom doping and the formation of core‐shell structures, which provide more accessible species with excellent interlayer and interparticle conductivity, resulting in increased electrical conductivity. . The α‐/γ‐MnS@CoxSy@N, SC electrode exhibits an excellent specific capacity of 277 mA hg−1 and cycling stability over 23 600 cycles. A quasi‐solid‐state flexible extrinsic pseudocapacitor (QFEPs) assembled using layer‐by‐layer deposited multi‐walled carbon nanotube/Ti3C2TX nanocomposite negative electrode. QFEPs deliver specific energy of 64.8 Wh kg−1 (1.62 mWh cm−3) at a power of 933 W kg−1 and 92% capacitance retention over 5000 cycles.

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“…Edge defects, such as zigzag and armchair edges (Figure 1a), have high spin and charge density due to the configuration of carbon atoms. [23] The local charge redistribution is thought to saturate the edge sites with electrons, hence, providing sites for better charge transfer. [27] Carbon vacancies refer to an absence of one (vacancy) or multiple (hole) carbon atoms in the matrix (Figure 1b), and therefore act in a similar way to edge defects due to the carbon edges formed around the carbon vacancy or hole.…”

Section: Defect Classifications and Their Functionalitymentioning

confidence: 99%

“…Defects in carbon-based materials can be categorised as either intrinsic or non-intrinsic (also referred to as doping defects). [23,24] Intrinsic defects include those induced within the carbon lattice, such as lattice distortions, carbon vacancies, and edge defects (such as zigzag and armchair edges). Doping defects refer to those formed because of heteroatom or metal doping, and can result in heteroatom-carbon bonds, heteroatom vacancies (similar to a carbon vacancy defect), and changes in the carbon matrix.…”

Section: Defect Classifications and Their Functionalitymentioning

confidence: 99%

“…The pathways for synthesising HC can take multiple approaches. The topdown approach inherits the already established microstructures 23 Na MAS NMR of HCs carbonised at different temperatures and after discharging to 5 mV; (e) Schematic illustration of sodium storage where no metallic sodium is detectable (i) and clustering in closed pores (ii). Reprinted with permission from ref., [88] used under Creative Commons CC-BY licence.…”

Section: The Choice Of the Precursor -Artificial Or Biomass Derivedmentioning

confidence: 99%

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Defective Carbon for Next‐Generation Stationary Energy Storage Systems: Sodium‐Ion and Vanadium Flow Batteries

McArdle,

Bauer,

Granieri

et al. 2023

ChemElectroChem

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This review examines the role of defective carbon‐based electrodes in sodium‐ion and vanadium flow batteries. Methods for introducing defects into carbon structures are explored and their effectiveness in improving electrode performance is demonstrated. In sodium‐based systems, research focuses primarily on various precursor materials and heteroatom doping to optimise hard carbon electrodes. Defect engineering increases interlayer spacing, porosity, and changes the surface chemistry, which improves sodium intercalation and reversible capacities. Heteroatom functionalisation and surface modification affect solid electrolyte interface formation and coulombic efficiencies. For flow batteries, post‐fabrication electrode enhancement methods produce defects to improve electrode kinetics, although these methods often introduce oxygen functional groups as well, making isolation of defect effects difficult. Continued research efforts are key to developing carbon‐based electrodes that can meet the unique challenges of future battery systems.

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Defect engineering in carbon materials for electrochemical energy storage and catalytic conversion

Abstract: Carbon, featured by its distinct physical, chemical, and electronic properties, has been considered a significant functional material for electrochemical energy storage and conversion systems. Significant improvements in the geometry, electron...

Cited by 22 publications

References 284 publications

Designing Efficient Single Metal Atom Biocatalysts at the Atomic Structure Level

Designing Efficient Single Metal Atom Biocatalysts at the Atomic Structure Level

Electronic Structure Engineered Heteroatom Doped All Transition Metal Sulfide Carbon Confined Heterostructure for Extrinsic Pseudocapacitor

Defective Carbon for Next‐Generation Stationary Energy Storage Systems: Sodium‐Ion and Vanadium Flow Batteries

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