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Theoretical insight into mercury species adsorption on graphene-based Pt single-atom catalysts.

ABSTRACT: Mercury emission from coal-fired flue gases is environmentally crucial. Revealing the interaction between mercury (Hg) and functional materials is significant to controlling emission. We conducted an investigation into the adsorption mechanism of mercury species onto graphene-based Platinum (Pt) single-atom catalysts (SACs). Single-atom Pt is the active center for Hg species chemisorption, with an adsorption energy range of 0.555-3.792 eV. In addition, Hg species adsorbed preferentially at lower temperatures. Pt/3N-GN exhibits a higher adsorption ability than Pt/SV-GN. The strong interaction of Hg⁰ with Pt SACs contributed to atomic-orbital hybridization between them. Further analysis revealed that s, p orbitals of Hg contribute significantly to orbital hybridization with Pt SACs. Moreover, the charge decomposition analysis confirmed that s, p orbitals of Hg hybridized with d, s orbitals of Pt SACs. The net charge transfer from Hg⁰ to Pt/SV-GN and Pt/3N-GN are 0.059 and 0.097 e^-, respectively. The higher the charge transfers, the more intense the electron and orbital interaction between Hg and the surface. Consequently, Pt/3N-GN is a highly effective catalyst for Hg adsorption.

SUBMITTER: Ji W

PROVIDER: S-EPMC8981981 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Theoretical insight into mercury species adsorption on graphene-based Pt single-atom catalysts.

Ji Wenchao W Xiao Xiuhua X Li Feiyue F Fan Xingjun X Meng Yuanyuan Y Fan Maohong M

RSC advances 20220216 10

Mercury emission from coal-fired flue gases is environmentally crucial. Revealing the interaction between mercury (Hg) and functional materials is significant to controlling emission. We conducted an investigation into the adsorption mechanism of mercury species onto graphene-based Platinum (Pt) single-atom catalysts (SACs). Single-atom Pt is the active center for Hg species chemisorption, with an adsorption energy range of 0.555-3.792 eV. In addition, Hg species adsorbed preferentially at lower ...[more]

PMID: 35424583

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Project description:The advancement of efficient and stable single-atom catalysts (SACs) has become a pivotal pursuit in the field of proton exchange membrane fuel cells (PEMFCs) and metal-air batteries (MABs), aiming to enhance the utilization of clean and sustainable energy sources. The development of such SACs has been greatly significant in facilitating the oxygen reduction reaction (ORR) process, thereby contributing to the progress of these energy conversion technologies. However, while transition metal-based SACs have been extensively studied, there has been comparatively less exploration of SACs based on p-block main-group metals. In this study, we conducted an investigation into the potential of p-block main-group Sn-based SACs as a cost-effective and efficient alternative to platinum-based catalysts for the ORR. Our approach involved employing density functional theory (DFT) calculations to systematically examine the catalyst properties of Sn-based N-doped graphene SACs, the ORR mechanism, and their electrocatalytic performance. Notably, we employed an H atom-decorated N-based graphene matrix as a support to anchor single Sn atoms, creating a contrast catalyst to elucidate the differences in activity and properties compared to pristine Sn-based N-doped graphene SACs. Through our theoretical analysis, we gained a comprehensive understanding of the active structure of Sn-based N-doped graphene electrocatalysts, which provided a rational explanation for the observed high four-electron reactivity in the ORR process. Additionally, we analyzed the relationship between the estimated overpotential and the electronic structure properties, revealing that the single Sn atom was in a +2 oxidation state based on electronic analysis. Overall, this work represented a significant step towards the development of efficient and cost-effective SACs for ORR which could alleviate environmental crises, advance clean and sustainable energy sources, and contribute to a more sustainable future.

Project description:Pt/C catalysts have been considered the ideal cathodic catalyst for proton exchange membrane fuel cells (PEMFCs) due to their superior oxygen reduction reaction (ORR) catalytic activity at low temperatures. However, oxidation and corrosion of the carbon black support at the cathode result in the agglomeration of Pt particles, which reduces the active sites in the Pt/C catalyst. Graphene supports have shown great promise to address this issue, and therefore, finding out the main structural features of the graphene support is of great significance for guiding the rational construction of graphene-based Pt (Pt/graphene) catalysts for optimized ORR catalysts. In order to systematically study the influence of the structural features of the graphene support on the electro-catalytic properties of Pt/graphene catalysts, we prepared porous nitrogen-doped reduced graphene oxide (P-NRGO), nitrogen-doped reduced graphene oxide (NRGO), treated P-NRGO (TP-NRGO) and reduced graphene oxide (RGO) with different nitrogen species contents (7.76, 7.54, 3.24, and 0.14 at%), oxygen species contents (18.68, 18.12, 6.34 and 21.12 at%), specific surface areas (370.4, 70.6, 347.7 and 276.2 m2 g-1) and pore volumes (1.366, 0.1424, 1.3299 and 1.0414 cm3 g-1). The ORR activity of the four Pt/graphene catalysts when listed in the order of their half-wave potentials (E 1/2) and peak power densities was found to be as Pt/P-NRGO > Pt/NRGO > Pt/TP-NRGO > Pt/RGO. The long-term durability of Pt/P-NRGO for the operation of H2-air PEMFCs is better than that of commercial Pt/C catalysts. The excellent ORR catalytic performance of Pt/P-NRGO compared to that of the other three Pt/graphene catalysts is ascribed to the high nitrogen species content of P-NRGO that can facilitate the uniform dispersion of Pt particles and provide accessible active sites for ORR. The results indicate that the specific surface area (SSA) and heteroatom dopants have strong influence on the Pt particle size, and that the nitrogen species of graphene supports play a more important role than the oxygen species, specific surface area and pore volume for the Pt/graphene catalysts in providing accessible active sites.

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Theoretical insight into mercury species adsorption on graphene-based Pt single-atom catalysts.

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Theoretical insight into mercury species adsorption on graphene-based Pt single-atom catalysts.

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