Sulfur doped graphene as a promising metal-free electrocatalyst for oxygen reduction reaction: a DFT-D study

Lu, Zhansheng; Li, Shuo; Liu, Chuang; He, Chaozheng; Yang, Xinwei; Ma, Dongwei; Xu, Guoliang; Yang, Zhou

doi:10.1039/c7ra00632b

Cited by 58 publications

(35 citation statements)

References 42 publications

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“…First-principles calculations within the density functional theory (DFT) methods were carried out in the Vienna ab initio simulation package (VASP). [36][37][38] The PBE methods have been employed to investigate the structural stability and electronic properties, and the HSE hybrid functional methods have been used to check the band gaps of all the cases employed here to overcome the problem of band gap underestimation in PBE functional. 39,40 The projector augmented wave (PAW) method is used to describe the electron-ion interaction, and the valence electrons of 4s 2 4p 2 for Sn and 3s 2 3p 4 for S atoms have been adopted in the calculations.…”

Section: Methodsmentioning

confidence: 99%

Coupling effects of strain on structural transformation and bandgap engineering in SnS monolayer

Zhang

Shang

et al. 2017

RSC Adv.

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Section: Methodsmentioning

confidence: 99%

Coupling effects of strain on structural transformation and bandgap engineering in SnS monolayer

Zhang

Shang

et al. 2017

RSC Adv.

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“…[271,338] Moreover, the abundant states near the Fermi level may indicate the high activity of the catalysts. [339] For instance, Lu et al [340] investigated the sulfurdoped graphene for ORR by the DOS analysis. As shown in Figure 9a, the emerged peaks in the DOS profile mainly come from the sulfur dopant and its neighboring C atom, indicating that the enhanced activity stemmed from Sdoping.…”

Section: Density Of Statesmentioning

confidence: 99%

“…[377] By comparing the barrier heights for different reaction pathways, one can find the mechanism of the electrocatalytic reaction. [378][379][380][381] Taking the formation of *O and *OH on S-doped graphene as example (Figure 9g), [340] DFT calculations have shown that the first step is the co-adsorption of *O 2 and *H. Subsequently, the *H moieties approached *O 2 to form the metastable state of *OOH on the S site. Afterward, the adsorbed *OOH is dissociated into co-adsorption of *O + *OH species and they move to a proper site to form the most stable configuration.…”

Section: Transition State Theory (Tst)mentioning

confidence: 99%

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Density Functional Theory for Electrocatalysis

Liao

Xia

et al. 2021

Energy & Environ Materials

161

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With the increase in energy demand and worldwide natural environment crises, it is imperative to develop green and sustainable energy systems to produce clean fuels and chemicals, which can replace fossil fuels and reduce carbon dioxide emissions. [1][2][3] A promising strategy is to develop advanced electrochemical technologies that can convert some common molecules (e.g., water, carbon dioxide, and nitrogen) into high-value chemical products (e.g., hydrogen, hydrocarbons, oxygenates, ammonia, and carbonates). [4][5][6][7] The important energy-related electrocatalytic reactions, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), nitrogen reduction reaction (NRR), carbon dioxide reduction reaction (CO 2 RR), are the key conversion routes. In the complex processes for the electrocatalytic reactions, an efficient, highly selective, and stable electrocatalyst plays a pivotal role in speeding up the reaction kinetics and decreasing the overpotential, [5,8,9] which can enhance the sustainable energy conversion efficiency. Over the past few decades, tremendous progresses have been made in the establishment of electrocatalysts preparation and fundamental catalytic mechanisms. [6,7,[9][10][11][12][13][14][15][16][17][18] Nevertheless, those breakthroughs still stay at the stage of experimental synthesis and lack of indepth understanding of fundamental principles of the active site on the catalyst surface and catalytic reactions mechanisms, which seriously limits the development of efficient catalysts. Researchers are full of enthusiasm about preparation of advanced catalysts with ideal properties, expecting to establish the composition-structure-function relationships. Density functional theory (DFT) calculations are based on quantum mechanics, which can calculate the electronic structure of the whole catalytic system. It is probably the most powerful computational approach to investigate the structure-activity relationships of electrocatalysts at atomic level. With the rapid advances of computer technology, DFT calculations have created tremendous opportunities in shedding light on the electrocatalytic mechanisms and predicting promising catalysts. [19,20] Identification of the active sites and understanding of the reaction mechanisms are the two key aspects for the study of electrocatalytic reactions. [21] For the former, the experimental approach for identifying active sites is indirect by prepared specified catalysts and establishing definite correlations between catalytic performances and controllable factors. [22,23] Actually, many intermediate states of electrocatalytic

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“…Technically, precious Pt-based nanomaterials are the commercial electrocatalysts for the oxygen reduction reaction (ORR), which reports 36-56% of the cost of the PEMFCs [188]. Various heteroatomdoped carbon materials [189], sulfur-doped graphene (SG) [190], phosphorous-doped graphite layers [191], iodine-doped graphene [192] and edge-halogenated (Cl, Br, or I) graphene nanoplatelets [193] and mesoporous nitrogen-doped carbons prepared from ionic liquids and nucleobases for productive metal-free oxygen reductions [194] are investigated. An article published by Iqbal et al [195] outlines graphene-based materials for fuel cell technology applications such as electrodes additives, bipolar plates and proton conducting electrolyte membrane.…”

Section: Go/rgo As Electrocatalystmentioning

confidence: 99%

Recent advances in the catalytic applications of GO/rGO for green organic synthesis

Sachdeva

2020

Green Processing and Synthesis

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Graphene is considered a promising catalyst candidate due to its 2D nature, single-atom thickness, zero bandgap and very high surface to volume ratio. Further, graphene oxide (GO) has been used as a catalytic support material for metal/metal oxide nanoparticles due to its tunable electrical properties. In addition, its high chemical stability and ultrahigh thermal conductivity may possibly promote high loading of catalytically active sites. This review article focuses on the recent progress in the catalytic applications of GO especially (i) as catalytic-support material (GO/reduced graphene oxide supported metal/metal oxide nanohybrids) for the green synthesis of biologically relevant molecules, (ii) for metal-free catalysis and (iii) for electrocatalysis, with special focus on graphene contribution to catalytic efficiency. The critical overview and future perspectives are also discussed.

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Sulfur doped graphene as a promising metal-free electrocatalyst for oxygen reduction reaction: a DFT-D study

Abstract: As an efficient metal-free catalyst, graphene doped with heteroatoms is highly active in promoting electrochemical oxygen reduction reaction (ORR).

Cited by 58 publications

References 42 publications

Coupling effects of strain on structural transformation and bandgap engineering in SnS monolayer

Coupling effects of strain on structural transformation and bandgap engineering in SnS monolayer

Density Functional Theory for Electrocatalysis

Recent advances in the catalytic applications of GO/rGO for green organic synthesis

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