Interface Confinement in Metal Nanosheet for High-Efficiency Semi-Hydrogenation of Alkynes

Shen，Chenqi1; Ji，Yujin2; Wang，Pengtang1; Bai，Shuxing3; Wang，Man4; Li，Youyong2; Huang，Xiaoqing1,5; Shao，Qi1

2021-05-07

10.1021/acscatal.1c00200

ACS Catalysis   影响因子和分区

2155-5435

Designing high-performance catalysts with high activity and selectivity toward semihydrogenation of alkynes is one of the major goals of fine chemical industry, yet full of challenges due to the difficulties in semihydrogenation of carbon- carbon triple bond (C C) to carbon-carbon double bond (C=C) without further hydrogenation. Herein, we demonstrate a twodimensionality (2D) enhanced interface-confined effect that leads to the strong interaction between lead (Pb) species and the ultrathin 2D palladium nanosheets (Pd NSs). As a result, the catalytic performance of the optimized Pd-Pb NSs in semi- hydrogenation of phenylacetylene can reach high conversion of 100%, high selectivity of 95.8%, and high activity of 2256 h(-1). It can also endure at least six cycles with limited conversion and selectivity decays. Detailed analyses reveal that the interface-confined effect in the 2D system is much stronger than that in the 3D system, making the Pd active sites more electron-deficient with greater positive shift of the binding energy and the weaker adsorption and binding capability of styrene. Such phenomenon disappears readily after destroying the interface structure. Density functional theory calculations further reveal that the confined interfaces cause the higher kinetic energy barriers of overhydrogenation processes of styrene into phenylethane as well as the weaker adsorption of styrene, resulting in the easier removal of styrene without further hydrogenation. More importantly, such 2D enhanced "interface-confined" strategy provides a general platform that achieves highefficiency semihydrogenation of a board range of alkynes.

interface surface confinement palladium semihydrogenation two dimensional

SCI ; EI

英语

其他

Ministry of Science and Technology of China["2017YFA0208200","2016YFA0204100"] ; National Natural Science Foundation of China[21571135,21905188] ; Jiangsu Province Natural Science Fund for Distinguished Young Scholars[BK20170003] ; China Postdoctoral Science Foundation[2019M651937] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University[KJS2019] ; project of scientific and technologic infrastructure of Suzhou[SZS201708]

Chemistry

Chemistry, Physical

WOS:000649106200029

AMER CHEMICAL SOC

20211910313146

Binding sites ; Carbon ; Catalyst activity ; Catalyst selectivity ; Chemical industry ; Density functional theory ; Hydrocarbons ; Hydrogenation ; Kinetic energy ; Kinetics ; Lead alloys ; Nanosheets ; Palladium alloys ; Styrene

Lead and Alloys:546.1 ; Precious Metals:547.1 ; Nanotechnology:761 ; Biochemistry:801.2 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Chemical Engineering, General:805 ; Classical Physics; Quantum Theory; Relativity:931 ; Solid State Physics:933

Web of Science

1.College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Jiangsu,215123,China
2.Institute of Functional Nano and Soft Materials (FUNSOM),Soochow University,Jiangsu,215123,China
3.College of Chemistry and Chemical Engineering,Qingdao University,Shandong,266071,China
4.Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,Southern University of Science and Technology,Shenzhen,518055,China
5.State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen,361005,China

Shen，Chenqi,Ji，Yujin,Wang，Pengtang,et al. Interface Confinement in Metal Nanosheet for High-Efficiency Semi-Hydrogenation of Alkynes[J]. ACS Catalysis,2021,11(9):5231-5239.

Shen，Chenqi.,Ji，Yujin.,Wang，Pengtang.,Bai，Shuxing.,Wang，Man.,...&Shao，Qi.(2021).Interface Confinement in Metal Nanosheet for High-Efficiency Semi-Hydrogenation of Alkynes.ACS Catalysis,11(9),5231-5239.

Shen，Chenqi,et al."Interface Confinement in Metal Nanosheet for High-Efficiency Semi-Hydrogenation of Alkynes".ACS Catalysis 11.9(2021):5231-5239.