A mechanistic insight into rhodium-doped gold clusters as a better hydrogenation catalyst

被引：6

作者：

Sengupta, Turbasu ^{[1
]}

Chung, Jin Suk ^{[1
]}

Kang, Sung Gu ^{[1
]}

机构：

[1] Univ Ulsan, Sch Chem Engn, 93 Daehakro, Ulsan 44610, South Korea

来源：

NANOSCALE | 2020年 / 12卷 / 08期

基金：

新加坡国家研究基金会;

关键词：

TRANSITION-METAL NANOCLUSTERS; BASIS-SETS; ELECTRONIC-PROPERTIES; ARENE HYDROGENATION; AU-20; CLUSTERS; NANOPARTICLES; ACTIVATION; OXIDATION; MODEL; SIZE;

D O I：

10.1039/c9nr10258b

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The reaction mechanism of the hydrogenation of ethylene on pristine (Au-n, n = 8 and 20) and rhodium-doped (AunRh) gold clusters was unveiled by theoretical calculations. All reaction pathways are predicted and the thermodynamic and kinetic parameters are computed and compared. Doping a rhodium atom on the magic gold cluster surface is effective in reducing the activation barriers for hydrogenation and in creating two competitive pathways with significantly higher turnover frequencies. The lower barriers of hydrogenation on the AunRh clusters were analyzed and explained based on distortion/interaction activation strain (DIAS) analysis. Further insights into the reaction mechanism on both types of clusters are provided by intrinsic bond orbital (IBO) calculations. This theoretical study provides an idea to elucidate the hydrogenation mechanism on Au clusters and the effect of the rhodium dopant on the catalytic process.

引用

页码：5125 / 5138

页数：14

共 34 条

[11] Ethene hydrogenation on zeolite-supported rhodium clusters. A mechanistic study by density functional and microkinetic modeling
Markova, Velina K.
Vayssilov, Georgi N.
Genest, Alexander
Roesch, Notker
APPLIED CATALYSIS A-GENERAL, 2017, 543 : 201 - 208
[12] Homogeneous hydrogenation of benzo[b]thiophene by use of rhodium and iridium complexes as the catalyst precursors: Kinetic and mechanistic aspects
Herrera, V
Fuentes, A
Rosales, M
SanchezDelgado, RA
Bianchini, C
Meli, A
Vizza, F
ORGANOMETALLICS, 1997, 16 (11) : 2465 - 2471
[13] Mechanistic insight into the CO oxidation reaction at pure, Nb-doped and Mo-doped medium size Pt clusters
Molina, L. M.
Arranz-Simon, C.
Alonso, J. A.
MOLECULAR CATALYSIS, 2022, 533
[14] Mechanistic insight into catalytic carbon dioxide hydrogenation to formic acid over Pt-doped boron nitride nanosheets
Injongkol, Yuwanda
Intayot, Ratchadaree
Yodsin, Nuttapon
Montoya, Alejandro
Jungsuttiwong, Siriporn
MOLECULAR CATALYSIS, 2021, 510
[15] Systematic theoretical investigation of structures, stabilities, and electronic properties of rhodium-doped silicon clusters: Rh2Sinq (n = 1–10; q = 0, ±1)
Shuai Zhang
Yu Zhang
Xingqiang Yang
Cheng Lu
Genquan Li
Zhiwen Lu
Journal of Materials Science, 2015, 50 : 6180 - 6196
[16] Fe clusters embedded on N-doped graphene as a photothermal catalyst for selective CO2 hydrogenation
Szalad, Horatiu
Peng, Lu
Primo, Ana
Albero, Josep
Garcia, Hermenegildo
CHEMICAL COMMUNICATIONS, 2021, 57 (78) : 10075 - 10078
[17] Mechanistic insight into the catalytic activities of metallic sites on nitrogen-doped graphene quantum dots for CO2 hydrogenation
Mahmoudi, Armin
Movahed, Siyavash Kazemi
Farrokhpour, Hossein
Carbon Trends, 2024, 17
[18] A Highly Selective Catalyst for Partial Hydrogenation of 1,3-Butadiene: MgO-Supported Rhodium Clusters Selectively Poisoned with CO
Yardimci, Dicle
Serna, Pedro
Gates, B. C.
CHEMCATCHEM, 2012, 4 (10) : 1547 - 1550
[19] Mechanistic insight into the C1 product selectivity for the catalytic hydrogenation of CO2 over metal-doped graphene
Chen, Hao-ze
Liu, Ji
Hu, Bin
Liu, Xin-ru
Wang, Hao-yu
Li, Ji-Hong
Lu, Qiang
CARBON NEUTRALITY, 2024, 3 (01):
[20] Systematic theoretical investigation of structures, stabilities, and electronic properties of rhodium-doped silicon clusters: Rh2Sin q (n=1-10; q=0, ±1)
Zhang, Shuai
Zhang, Yu
Yang, Xingqiang
Lu, Cheng
Li, Genquan
Lu, Zhiwen
JOURNAL OF MATERIALS SCIENCE, 2015, 50 (18) : 6180 - 6196

← 1 2 3 4 →