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. 2022 Jul 8;12(31):19955-19964.
doi: 10.1039/d2ra00898j. eCollection 2022 Jul 6.

Density functional theory analysis for H2S adsorption on pyridinic N- and oxidized N-doped graphenes

Takaya Fujisaki  1 , Kei Ikeda  2 , Aleksandar Tsekov Staykov  3 , Hendrik Setiawan  4 , Yusuke Shiratori  5
Affiliations

Density functional theory analysis for H2S adsorption on pyridinic N- and oxidized N-doped graphenes

Takaya Fujisaki et al. RSC Adv. .

Abstract

Biomass discharged from primary industries can be converted into methane by fermentation. This methane is used for generating electricity with solid oxide fuel cells (SOFCs). This methane fermentation provides H2S, which reduces the efficiency of SOFCs even at a level as low as a few parts per million. It has been experimentally reported that a nitrogen (N)-doped graphene-based material known as pyridinic N removes H2S via an oxidation reaction compared with another graphene-based material known as oxidized N. To understand this experimental result, we investigated H2S adsorption on pyridinic N and oxidized N by a density functional theory analysis and further examined the activation barrier of dissociation reactions. We found that the adsorption of H2S on pyridinic N is more stable than that on oxidized N. In addition, the H2S dissociation reaction occurs only on pyridinic N.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. Material and energy circulation model using biomass.
Fig. 2
Fig. 2. Top and side views of the geometry optimized structure of H2S on (a) pyridinic N and (b) oxidized N.
Fig. 3
Fig. 3. Adsorption energy (Eads) and interaction energy (Eint) between H2S and pyridinic N/oxidized N. The deformation energies of pyridinic N (Edef_pyridinic N), oxidized N (Edef_oxidized N), and H2S are also shown.
Fig. 4
Fig. 4. Adsorption energy (Eads) and interaction energy (Eint) between H2S and pyridinic N/oxidized N. The deformation energies of pyridinic N (Edef_pyridinic N), oxidized N (Edef_oxidized N), and H2S are also shown.
Fig. 5
Fig. 5. (a) Electron mapping for H2S on pyridinic N, including density of states of (b) H–N and (c) S–N electrons. (d) Electron mapping of H2S on oxidized N, and (e) density of states of H–O.
Fig. 6
Fig. 6. Walsh diagram of H2S. Black and white lobes show positive and negative wave functions, respectively.
Fig. 7
Fig. 7. H2S dissociated as HS− and H+ on pyridinic N under (a) holding electrical neutrality, and (b) one electron added condition.
Fig. 8
Fig. 8. Activation barrier of the H2S dissociation reaction on pyridinic N under the conditions of holding electrical neutrality and adding one electron.
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