Dataset Information

Nickel@Siloxene catalytic nanosheets for high-performance CO₂ methanation.

ABSTRACT: Two-dimensional (2D) materials are of considerable interest for catalyzing the heterogeneous conversion of CO₂ to synthetic fuels. In this regard, 2D siloxene nanosheets, have escaped thorough exploration, despite being composed of earth-abundant elements. Herein we demonstrate the remarkable catalytic activity, selectivity, and stability of a nickel@siloxene nanocomposite; it is found that this promising catalytic performance is highly sensitive to the location of the nickel component, being on either the interior or the exterior of adjacent siloxene nanosheets. Control over the location of nickel is achieved by employing the terminal groups of siloxene and varying the solvent used during its nucleation and growth, which ultimately determines the distinct reaction intermediates and pathways for the catalytic CO₂ methanation. Significantly, a CO₂ methanation rate of 100?mmol?g_Ni^-1?h^-1 is achieved with over 90% selectivity when nickel resides specifically between the sheets of siloxene.

SUBMITTER: Yan X

PROVIDER: S-EPMC6565710 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Nickel@Siloxene catalytic nanosheets for high-performance CO<sub>2</sub> methanation.

Yan Xiaoliang X Sun Wei W Fan Liming L Duchesne Paul N PN Wang Wu W Kübel Christian C Wang Di D Kumar Sai Govind Hari SGH Li Young Feng YF Tavasoli Alexandra A Wood Thomas E TE Hung Darius L H DLH Wan Lili L Wang Lu L Song Rui R Guo Jiuli J Gourevich Ilya I Ali Feysal M FM Lu Jingjun J Li Ruifeng R Hatton Benjamin D BD Ozin Geoffrey A GA

Nature communications 20190613 1

Two-dimensional (2D) materials are of considerable interest for catalyzing the heterogeneous conversion of CO<sub>2</sub> to synthetic fuels. In this regard, 2D siloxene nanosheets, have escaped thorough exploration, despite being composed of earth-abundant elements. Herein we demonstrate the remarkable catalytic activity, selectivity, and stability of a nickel@siloxene nanocomposite; it is found that this promising catalytic performance is highly sensitive to the location of the nickel componen ...[more]

PMID: 31197151

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Project description:The molecular functionalization of two-dimensional MoS2 is of practical relevance with a view to, for example, facilitating its liquid-phase processing or enhancing its performance in target applications. While derivatization of metallic 1T-phase MoS2 nanosheets has been relatively well studied, progress involving their thermodynamically stable, 2H-phase counterpart has been more limited due to the lower chemical reactivity of the latter. Here, we report a simple electrolytic strategy to functionalize 2H-phase MoS2 nanosheets with molecular groups derived from organoiodides. Upon cathodic treatment of a pre-expanded MoS2 crystal in an electrolyte containing the organoiodide, water-dispersible nanosheets derivatized with acetic acid or aniline moieties (∼0.10 molecular groups inserted per surface sulfur atom) were obtained. Analysis of the functionalization process indicated it to be enabled by the external supply of electrons from the cathodic potential, although they could also be sourced from a proper reducing agent, as well as by the presence of intrinsic defects in the 2H-phase MoS2 lattice (e.g., sulfur vacancies), where the molecular groups can bind. The acetic acid-functionalized nanosheets were tested as a non-noble metal-based catalyst for nitroarene and organic dye reduction, which is of practical utility in environmental remediation and chemical synthesis, and exhibited a markedly enhanced activity, surpassing that of other (1T- or 2H-phase) MoS2 materials and most non-noble metal catalysts previously reported for this application. The reduction kinetics (reaction order) was seen to correlate with the net electric charge of the nitroarene/dye molecules, which was ascribed to the distinct abilities of the latter to diffuse to the catalyst surface. The functionalized MoS2 catalyst also worked efficiently at realistic (i.e., high) reactant concentrations, as well as with binary and ternary mixtures of the reactants, and could be immobilized on a polymeric scaffold to expedite its manipulation and reuse.

Dataset Information

Nickel@Siloxene catalytic nanosheets for high-performance CO₂ methanation.

Publications

Nickel@Siloxene catalytic nanosheets for high-performance CO<sub>2</sub> methanation.

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Dataset Information

Nickel@Siloxene catalytic nanosheets for high-performance CO2 methanation.

Publications

Nickel@Siloxene catalytic nanosheets for high-performance CO<sub>2</sub> methanation.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

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Nickel@Siloxene catalytic nanosheets for high-performance CO₂ methanation.