Accessing Frustrated Lewis Pair Chemistry through Robust Gold@N-Doped Carbon for Selective Hydrogenation of Alkynes

Author(s)

Fiorio, Jhonatan Luiz ^[1] ; Goncalves, Renato Vitalino ^[2] ; Teixeira-Neto, Erico ^[3] ; Ortuno, Manuel A. ^[4] ; Lopez, Nuria ^[4] ; Rossi, Liane Marcia ^[1]

Affiliation

^[1] Univ Sao Paulo, Inst Quim, Dept Quim Fundamental, Av Prof Lineu Prestes 748, BR-05508000 Sao Paulo, SP - Brazil

^[2] Univ Sao Paulo, Inst Fis Sao Carlos, CP 369, BR-13560970 Sao Carlos, SP - Brazil

^[3] Brazilian Ctr Res Energy & Mat CNPEM, Brazilian Nanotechnol Natl Lab LNNano, BR-13083970 Campinas, SP - Brazil

^[4] BIST, Inst Chem Res Catalonia, ICIQ, Av Paisos Catalans 16, Tarragona 43007 - Spain

• Document type: Journal article
• Source: ACS CATALYSIS; v. 8, n. 4, p. 3516-3524, APR 2018.
• Web of Science Citations: 20

Abstract

Pyrolysis of Au(OAc)(3) in the presence of 1,10-phenanthroline over TiO2 furnishes a highly active and selective Au nanoparticle (NP) catalyst embedded in a nitrogen-doped carbon support, Au@N-doped carbon/TiO2 catalyst. Parameters such as pyrolysis temperature, type of support, and nitrogen ligands as well as Au/ligand molar ratios were systematically investigated. Highly selective hydrogenation of numerous structurally diverse alkynes proceeded in moderate to excellent yield under mild conditions. The high selectivity toward the industrially important alkene substrates, functional group tolerance, and the high recyclability makes the catalytic system unique. Both high activity and selectivity are correlated with a frustrated Lewis pairs interface formed by the TiO2 combination of gold and nitrogen atoms of N-doped carbon that, according to density functional theory calculations, can serve as a basic site to promote the heterolytic activation of H-2 under very mild conditions. This ``fully heterogeneous{''} and recyclable gold catalyst makes the selective hydrogenation process environmentally and economically attractive. (AU)

• FAPESP's process: 16/16738-7 - Study of the influence of organic ligands on the reactivity of gold nanoparticles
• Grantee: Liane Marcia Rossi
• Support Opportunities: Regular Research Grants