title: Enhancing Metal-Support Interactions by Molybdenum Carbide: An Efficient Strategy toward the Chemoselective Hydrogenation of α,β-Unsaturated Aldehydes.
abstract: Metal-support interactions are desired to optimize the catalytic turnover on metals. Herein, the enhanced interactions by using a Mo2C nanowires support were utilized to modify the charge density of an Ir surface, accomplishing the selective hydrogenation of α,β-unsaturated aldehydes on negatively charged Ir(δ-) species. The combined experimental and theoretical investigations showed that the Ir(δ-) species derive from the higher work function of Ir (vs. Mo2C) and the consequently electron transfer. In crotonaldehyde hydrogenation, Ir/Mo2C delivered a crotyl alcohol selectivity as high as 80%, outperforming those of counterparts (<30%) on silica. Moreover, such electronic metal-support interactions were also confirmed for Pt and Au, as compared with which, Ir/Mo2C was highlighted by its higher selectivity as well as the better activity. Additionally, the efficacy for various substrates further verified our Ir/Mo2C system to be competitive for chemoselective hydrogenation.
authors.affiliation: Department of Chemistry, Jinan University, Guangzhou, 510632, P. R. China.
authors.forename: Sina
authors.initials: S
authors.lastname: He
authors.affiliation: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science & Technology, Shanghai, 200237, P. R. China.
authors.forename: Zheng-Jiang
authors.initials: ZJ
authors.lastname: Shao
authors.affiliation: Department of Chemistry, Jinan University, Guangzhou, 510632, P. R. China.
authors.forename: Yijin
authors.initials: Y
authors.lastname: Shu
authors.affiliation: Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433, P. R. China.
authors.forename: Zhangping
authors.initials: Z
authors.lastname: Shi
authors.affiliation: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science & Technology, Shanghai, 200237, P. R. China. xmcao@ecust.edu.cn.
authors.forename: Xiao-Ming
authors.initials: XM
authors.lastname: Cao
authors.affiliation: Department of Chemistry, Jinan University, Guangzhou, 510632, P. R. China. tqsgao@jnu.edu.cn.
authors.forename: Qingsheng
authors.initials: Q
authors.lastname: Gao
authors.affiliation: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science & Technology, Shanghai, 200237, P. R. China.
authors.forename: Peijun
authors.initials: P
authors.lastname: Hu
authors.affiliation: Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433, P. R. China.
authors.forename: Yi
authors.initials: Y
authors.lastname: Tang
keywords: carbides; hydrogenation; iridium; metal-support interactions; unsaturated aldehydes