Ultra-dense carbon defects as highly active sites for oxygen reduction catalysis

Wu, Qilong; Jia, Yi; Liu, Qian; Guo, Qi; Yan, Xuecheng; Zhao, Jiong‐Peng; Liu, Fuchen; Du, Aijun; Yao, Xiangdong

doi:10.1016/j.chempr.2022.06.013

Cited by 98 publications

(73 citation statements)

References 50 publications

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“…Nowadays, a series of well-known carbon-based electrocatalysts have been fabricated through the combinations of various modification methods and substrate materials, such as heteroatom doped graphene, defective graphene, Mxene, heteroatom doped carbon nanotubes/ribbons and modified carbon dots. [57][58][59][60][61][62][63][64][65] However, the design of state-of-the-art electrocatalysts still relies on inefficient trial-and-error approaches, and the catalytic mechanism is still controversial and difficult to reveal only through experimental research. DFT calculations are thus utilized to address two issues: 1) predicting catalytic performance and guiding the synthesis of electrocatalysts.…”

Section: Theoretical Guidance In Catalyst Design and Mechanism Studymentioning

confidence: 99%

DFT-Assisted Low-Dimensional Carbon-based Electrocatalysts Design and Mechanism Study: A Review

Yan¹,

Han²,

Xu³

et al. 2022

Preprint

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Low-dimensional carbon-based (LDC) materials have attracted extensive research attentions in electrocatalysis because of their unique advantages such as structural diversity, low cost, and chemical tolerance. They have been widely used in a broad range of electrochemical reactions to relief environmental pollution and energy crisis. Typical examples include hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO2RR), and nitrogen reduction reaction (NRR). Traditional “trial and error” strategies seriously slowed down the rational design of electrocatalysts for these important applications. Recent studies show that the combination of density functional theory (DFT) calculations and experimental research is capable of accurately predicting the structures of electrocatalysts, thus could reveal the catalytic mechanisms. Herein, current well-recognized collaboration methods of theory and practice are reviewed. The history of modern DFT, commonly used calculation methods, and basic functionals are briefly summarized. Special attention is paid to descriptors that are widely accepted as a bridge links the structure and activity, and the breakthroughs for high-volume accurate prediction of electrocatalysts. Importantly, correlating multiple descriptors are used to systematically describe the complicated interfacial electrocatalytic processes of LDC catalysts. In addition, machine learning and high-throughput simulations are crucial in assisting the discovery of new multiple descriptors and reaction mechanisms. This review will guide the further development of LDC electrocatalysts for extended applications from the aspect of DFT computations.

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Section: Theoretical Guidance In Catalyst Design and Mechanism Studymentioning

confidence: 99%

DFT-Assisted Low-Dimensional Carbon-based Electrocatalysts Design and Mechanism Study: A Review

Yan¹,

Han²,

Xu³

et al. 2022

Preprint

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show abstract

“…Excessive defect concentration will destroy the C-C sp 2 conjugated structure and make the conductivity worse, thereby impairing the cycling stability of the battery and the activity of electrochemistry. 40 Recently, great progress has been made with regard to carbon defect engineering for energy storage and conversion, while revealing the active origin and precisely customizing defects in the carbon matrix currently remain a challenge. An in-depth understanding of the role of carbon defects in electrochemical redox reactions is crucial, which can guide the rational design of high-performance carbon defect sites.…”

Section: Introductionmentioning

confidence: 99%

“…Excessive defect concentration will destroy the C–C sp 2 conjugated structure and make the conductivity worse, thereby impairing the cycling stability of the battery and the activity of electrochemistry. 40…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2023

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“…Defect engineering of carbon materials has been widely investigated for electrocatalytic reactions and/or energy storage. − The foreign-doping defects (e.g., heteroatoms and functional groups) not only serve as the active sites but also endow the carbon materials with some novel functions such as high activity and good surface wettability. − For example, Alshareef and Zhao proposed that oxygen-bearing functional groups possessed a reversible pseudocapacitive behavior by reacting with H + and Zn 2+ to enhance the energy storage ability of porous carbon for aqueous Zn-ion capacitors. Lu revealed that nitrogen-bearing functional groups could generate pseudocapacitance by reducing the energy barrier of C–O–Zn bonding.…”

Section: Introductionmentioning

confidence: 99%

Revealing the Self-Doping Defects in Carbon Materials for the Compact Capacitive Energy Storage of Zn-Ion Capacitors

Yuan

Wang

Shang

et al. 2023

ACS Appl. Mater. Interfaces

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Zn-ion capacitors are attracting great attention owing to the abundant and relatively stable Zn anodes but are impeded by the low capacitance of porous carbon cathodes with insufficient energy storage sites. Herein, using ball-milled graphene with different defect densities as the models, we reveal that the selfdoping defects of carbon show a capacitive energy storage behavior with robust charge-transfer kinetics, providing a capacitance contribution of ca. 90 F g −1 per unit of defect density (A D /A G value from Raman spectra) in both aqueous and organic electrolytes. Furthermore, a simple NaCl-assisted ball-milling method is developed to prepare novel graphene blocks (BSG) with abundant self-doping defect density, enriched pores, balanced electric conductivity, and high compact density (0.83 g cm −3 ). The optimized ion and electron transfer paths promote efficient utilization of the self-doping defects in BSG, contributing to improved gravimetric and volumetric capacitance (224 F g −1 /186 F cm −3 at 0.5 A g −1 ) and remarkable rate performance (52.2% capacitance retention at 20 A g −1 ). The defect engineering strategy may open up a new avenue to improve the capacitive performance of dense carbons for Zn-ion capacitors.

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Ultra-dense carbon defects as highly active sites for oxygen reduction catalysis

Cited by 98 publications

References 50 publications

DFT-Assisted Low-Dimensional Carbon-based Electrocatalysts Design and Mechanism Study: A Review

DFT-Assisted Low-Dimensional Carbon-based Electrocatalysts Design and Mechanism Study: A Review

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

Revealing the Self-Doping Defects in Carbon Materials for the Compact Capacitive Energy Storage of Zn-Ion Capacitors

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