Carbon for the oxygen reduction reaction: a defect mechanism

Zhao, Huanyu; Sun, Chenghua; Zhao, Jin; Wang, Da‐Wei; Yan, Xuecheng; Chen, Zhigang; Zhu, Guangshan; Yao, Xiangdong

doi:10.1039/c5ta02229k

Cited by 271 publications

(218 citation statements)

References 23 publications

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“…2a). 48 It was notable that the N-content decreased stepwise with the increase in the calcination temperatures (Fig. 2b).…”

Section: Investigations Of N-orr Activity Relationshipmentioning

confidence: 99%

“…1). First, we introduce the concept of defect electrocatalysis, including how this defect mechanism for ORR was discovered in an earlier work, 48 in which we clearly presented the concept of defect mechanism, exhibited the topological defects (e.g. the combination of carbon rings with pentagon-octagon-pentagon, denoted as D585) as the active sites and developed a methodology to create such defects for ORR.…”

Section: Account Of Recent Work On Defective Carbon Based Materials Fmentioning

confidence: 99%

“…48,49 Researchers from other groups have also started to devote great efforts to prepare carbon-based materials with a large number of intrinsic/induced defects. Almost simultaneously, Xia and co-workers theoretically studied the effect of point-and line-defects in graphene on the catalytic activities using density functional theory (DFT) methods.…”

Section: Orr Activity In Defective Carbonsmentioning

confidence: 99%

“…54 2.3 Defective graphene: defect mechanism for ORR, OER and HER As discussed in Sections 2.1 and 2.2, a defect catalytic mechanism in ORR was proved by both experimental results and theoretical calculations. However, currently a few issues still need to be addressed for understanding the defect catalytic mechanism: (i) the topological defects, such as in PAF/MOFderived carbons, have not been directly observed due to the resulting complex 3D structures obtained after carbonization; 48,49 (ii) according to theoretical correlations of the carbon defect types and electronic structures, carbon defects can be analogously categorized into n-type and p-type, leading to a potential enhancement in electrochemical reductions (e.g. ORR and HER) and oxidation reactions (e.g.…”

Section: Materials Chemistry Frontiers Reviewmentioning

confidence: 99%

“…90 Then, we present controllable strategies in preparing diverse carbon materials with defects. [48][49][50][51][52][53][54][55][56] Importantly, the defective carbon-based materials exhibit excellent ORR activities, which overcomes the common sense of the necessity for heteroatom doping. 49 Besides the carbon defect mechanism for ORR, our group further demonstrated that defects as active sites in carbon (graphene used as an ideal model material for direct instrumental identification purpose) were also functional for other electrochemical reactions, such as OER and HER, which may originate from different types of carbon defects.…”

Section: Account Of Recent Work On Defective Carbon Based Materials Fmentioning

confidence: 99%

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Defect electrocatalytic mechanism: concept, topological structure and perspective

Jia

Chen

Yao

2018

Mater. Chem. Front.

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125

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Carbon-based materials have been attracting intense interest for electrocatalysis due to their various merits, such as abundance, low cost, high conductivity and tunable molecular structures. However, to date, the electrochemical activities of these electrocatalysts are mainly attributed to different active dopants (e.g. N, B, P or S), leading to a common concept that heteroatom doping is essential for carbon-based electrocatalysts. Recently, we presented a new concept where the specific topological defects could activate the oxygen reduction reaction (ORR) and developed a facile method to create such unique defects. Subsequent research has extended this new mechanism to other reactions, such as the hydrogen and oxygen evolution reactions (HER and OER) and confirmed that heteroatom doping is not essential but that these defects can serve as actives sites for electrochemical reactions. This new theory then creates a new research direction in electrocatalysis. In this short review, we summarise the origin and presentation of the defect mechanism concept, the possible topological defect structures that are effective for electrochemical reactions, the formation of desirable defects, the challenges in the synthesis and characterization of typical defects and future research directions on the electrochemical defect mechanism. Carbon-based materials have been attracting intense interest for electrocatalysis due to their various merits, such as abundance, low cost, high conductivity and tunable molecular structures. However, to date, the electrochemical activities of these electrocatalysts are mainly attributed to different active dopants (e.g. N, B, P or S), leading to a common concept that heteroatom doping is essential for carbon-based electrocatalysts. Recently, we presented a new concept where the specific topological defects could activate the oxygen reduction reaction (ORR) and developed a facile method to create such unique defects. Subsequent research has extended this new mechanism to other reactions, such as the hydrogen and oxygen evolution reactions (HER and OER) and confirmed that heteroatom doping is not essential but that these defects can serve as actives sites for electrochemical reactions. This new theory then creates a new research direction in electrocatalysis. In this short review, we summarise the origin and presentation of the defect mechanism concept, the possible topological defect structures that are effective for electrochemical reactions, the formation of desirable defects, the challenges in the synthesis and characterization of typical defects and future research directions on the electrochemical defect mechanism.

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“…2a). 48 It was notable that the N-content decreased stepwise with the increase in the calcination temperatures (Fig. 2b).…”

Section: Investigations Of N-orr Activity Relationshipmentioning

confidence: 99%

Section: Account Of Recent Work On Defective Carbon Based Materials Fmentioning

confidence: 99%

Section: Orr Activity In Defective Carbonsmentioning

confidence: 99%

Section: Materials Chemistry Frontiers Reviewmentioning

confidence: 99%

Section: Account Of Recent Work On Defective Carbon Based Materials Fmentioning

confidence: 99%

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Defect electrocatalytic mechanism: concept, topological structure and perspective

Jia

Chen

Yao

2018

Mater. Chem. Front.

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125

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Environmental Remediation with Electrochemical Technologies

Chen

Rajić

Zhao

et al. 2018

Kirk-Othmer Encyclopedia of Chemical Technology

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Significant concerns continue to be raised over environmental pollution of soils and water resources. Chemical fate and transport coupled with redox manipulation are the primary processes that have been considered for removing contamination and minimizing exposure. Electrochemical processes utilize electron transfer to drive transport of chemicals and redox manipulation for treatment of contaminated media. Electrokinetic remediation relies on the electric field to transport contaminants in low permeability soils toward the electrode vicinity for removal. In water cleanup, both electroreduction and electrooxidation have been used. Electroreduction has been used for dechlorination and defluorination of halogenated calcitrant compounds. Electrooxidation has also gained significant potential for transformation of many legacy and emerging contaminants. For example, organic contaminants could be oxidized directly on anode surface (direct anodic oxidation), by electrochemically generated hydroxyl radicals or by other electrochemically generated oxidants (indirect anodic oxidation). In this article, we present an overview of the state‐of‐the‐art electrochemical processes for treatment of contaminated soil and water. We also describe a perspective for future research directions in the field of electrochemical treatment of contaminated media.

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Metal‐Free Carbon‐Based Nanomaterials: Fuel Cell Applications as Electrocatalysts

Chung

Lin

2022

Functional Nanomaterials

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Carbon for the oxygen reduction reaction: a defect mechanism

Abstract: A new defect mechanism for the ORR was proposed based on the theoretical calculations and our experimental results.

Cited by 271 publications

References 23 publications

Defect electrocatalytic mechanism: concept, topological structure and perspective

Defect electrocatalytic mechanism: concept, topological structure and perspective

Environmental Remediation with Electrochemical Technologies

Metal‐Free Carbon‐Based Nanomaterials: Fuel Cell Applications as Electrocatalysts

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