Probing the active sites of site-specific nitrogen doping in metal-free graphdiyne for electrochemical oxygen reduction reactions

Chen, Xingzhu; Ong, Wee‐Jun; Kong, Zhongxin; Zhao, Xiujian; Li, Neng

doi:10.1016/j.scib.2019.10.016

Cited by 52 publications

(26 citation statements)

References 72 publications

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“…To optimize the chemisorption energies and molecular bond energies, we employed the generalized gradient approximation (GGA) in the form of revised Perdew-Burke-Ernzerhof (revPBE) functional for the exchange-correlation potential [56]. We used the DFT-D3 method to describe the van der Waals interactions [57,58]. The k-points were sampled using the 2 Â 2 Â 1 and 4 Â 4 Â 1 Monkhorst-Pack mesh for ion relaxation and electronic structure calculations respectively [59].…”

Section: Methodsmentioning

confidence: 99%

Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Chen

Ong

Zhao

et al. 2021

Journal of Energy Chemistry

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Section: Methodsmentioning

confidence: 99%

Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Chen

Ong

Zhao

et al. 2021

Journal of Energy Chemistry

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“…To date, N-doped graphite carbon material including activated carbon, carbon nanotubes and graphene [72,[101][102][103] have demonstrated to be the effective ORR catalysts. In this respect, the ORR process of N-atom-doped GDY on the cathode of a fuel cell was also discussed in many studies [104][105][106][107][108][109][110][111]. The ORR mechanism of N-doped GDY was investigated by using the first principles calculations.…”

Section: Nonmetallic-atom-doped Gdy Electrocatalystsmentioning

confidence: 99%

“…The kinetically most favorable and efficient four-electron reaction pathway (O 2 → OOH → O + H 2 O → OH → H 2 O) was adopted [104]. The site-specific N doping of GDY including grap-N, sp-N (I) and sp-N (II)-doped GDY (Figure 8a) was systematically investigated as ORR electrocatalysts via DFT [108]. The adjacent sp-C atoms are activated as centers of ORR electrocatalytic process because the charge redistribution is caused by the doping of N atoms.…”

Section: Nonmetallic-atom-doped Gdy Electrocatalystsmentioning

confidence: 99%

“…Of particular interest, the sp-N (II) doping provides the most significant ORR performance improvement by increasing the onset potential to 0.76 V, which is even comparable to that of noble metal Pt (1 1 1) catalyst (0.78 V) [96]. discussed in many studies [104][105][106][107][108][109][110][111]. The ORR mechanism of N-doped GDY was investigated by using the first principles calculations.…”

Section: Nonmetallic-atom-doped Gdy Electrocatalystsmentioning

confidence: 99%

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Atomic-Level Functionalized Graphdiyne for Electrocatalysis Applications

et al. 2020

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Graphdiyne (GDY) is a two-dimensional (2D) electron-rich full-carbon planar material composed of sp2- and sp-hybridized carbon atoms, which features highly conjugated structures, uniformly distributed pores, tunable electronic characteristics and high specific surface areas. The synthesis strategy of GDY by facile coupling reactions under mild conditions provides more convenience for the functional modification of GDY and offers opportunities for realizing the special preparation of GDY according to the desired structure and unique properties. These structural characteristics and excellent physical and chemical properties of GDY have attracted increasing attention in the field of electrocatalysis. Herein, the research progress in the synthesis of atomic-level functionalized GDYs and their electrocatalytic applications are summarized. Special attention was paid to the research progress of metal-atom-anchored and nonmetallic-atom-doped GDYs for applications in the oxygen reduction reaction (ORR), the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) catalytic processes. In addition, several potential development prospects and challenges of these 2D highly conjugated electron-rich full-carbon materials in the field of electrocatalysis are presented.

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“…To date most of the very few theoretical studies in this regard span only around Gdy. [51][52][53] The electrocatalytic activities and reaction mechanism of non-metal doped Gys/Gdy still remains largely unexplored for ORR in alkaline medium. In alkaline medium, the reaction occurs via completely different intermediate formations compared to acidic medium and the mechanisms are hardly been investigated for the large group of Gys and Gdy to date.…”

Section: Introductionmentioning

confidence: 99%

Mechanism of Oxygen Reduction Reaction in Alkaline Medium on Nitrogen‐Doped Graphyne and Graphdiyne Families: A First Principles Study

2022

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Using extensive first principles protocols, a systematic investigation is performed to probe the oxygen reduction reaction (ORR) mechanism on nitrogen (N) doped graphynes (Gys, e. g. αGy, βGy, γGy and 6,6,12Gy) and graphdiyne (Gdy) in alkaline medium. We considered both associative and dissociative pathways, as well as two distinct intermediate forks for each of them depending on the first protonation site(s). Following the dissociative approach, the activation energy to form an O 2 dissociated configuration is found as a function of the distances migrated by the O atoms over the catalyst surface and the amount of charge transferred from the C atoms linked to N. N doped αGy and 6,6,12Gy emerged as the best electrocatalyst comparing both pathways having lowest overpotentials of 0.88 and 0.82 V, respectively. The rate-limiting steps for the two different intermediate routes are observed to be dependent on the first protonation site(s) and related to the desorption of the OH radical from the sp hybridized C atom site(s) linked to N. Hence, the OH adsorption energy is identified as a descriptor for the efficiency of the ORR for the considered systems. The stabilities of the ORR intermediates are further elaborated in terms of pH and electrode potential.

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Probing the active sites of site-specific nitrogen doping in metal-free graphdiyne for electrochemical oxygen reduction reactions

Cited by 52 publications

References 72 publications

Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Atomic-Level Functionalized Graphdiyne for Electrocatalysis Applications

Mechanism of Oxygen Reduction Reaction in Alkaline Medium on Nitrogen‐Doped Graphyne and Graphdiyne Families: A First Principles Study

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