Investigating active site of gold nanoparticle Au55(PPh 3)12Cl6 in selective oxidation

Yong Pei; Nan Shao; Yi Gao; Xiao Cheng Zeng

doi:10.1021/nn100184m

Investigating active site of gold nanoparticle Au₅₅(PPh ₃)₁₂Cl₆ in selective oxidation

Yong Pei, Nan Shao, Yi Gao, Xiao Cheng Zeng

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

82 Citations (Scopus)

Abstract

We present an ab initio investigation of structural, electronic, catalytic, and selective properties of the ligand-covered gold nanoparticle Au ₅₅(PPh₃)₁₂Cl₆ and associated model clusters. The catalytic activity of the Au₅₅(PPh₃) ₁₂Cl₆ nanoparticle in the presence of O₂ stems from a combined effect of triphenylphosphine ligands and surface structure of the "magic-number" quasi-icosahedral Au₅₅ core, which entails numerous ligand-encompassed triangle Au₆ faces as the active sites. Under the Eley-Rideal mechanism, the "triangle-socket" active site not only can accommodate one pre-adsorbed O₂ (which is subsequently activated to the superoxo species) with one styrene molecule at a time but also can provide spatial confinement which favors the formation of an oxametallacycle intermediate that leads to unique selectivity in styrene oxidation. © 2010 American Chemical Society.

Original language	English
Pages (from-to)	2009-2020
Journal	ACS Nano
Volume	4
Issue number	4
DOIs	https://doi.org/10.1021/nn100184m
Publication status	Published - 27 Apr 2010
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Research Keywords

Active sites
Catalytic properties and selectivity
Density-functional theory
Ligand-covered gold nanoparticles
Quasi-icosahedral Au55 core

Access Output

10.1021/nn100184m

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

Cite this

@article{c8d768a28c094a15bdf13f7fd643bc75,

title = "Investigating active site of gold nanoparticle Au55(PPh 3)12Cl6 in selective oxidation",

abstract = "We present an ab initio investigation of structural, electronic, catalytic, and selective properties of the ligand-covered gold nanoparticle Au 55(PPh3)12Cl6 and associated model clusters. The catalytic activity of the Au55(PPh3) 12Cl6 nanoparticle in the presence of O2 stems from a combined effect of triphenylphosphine ligands and surface structure of the {"}magic-number{"} quasi-icosahedral Au55 core, which entails numerous ligand-encompassed triangle Au6 faces as the active sites. Under the Eley-Rideal mechanism, the {"}triangle-socket{"} active site not only can accommodate one pre-adsorbed O2 (which is subsequently activated to the superoxo species) with one styrene molecule at a time but also can provide spatial confinement which favors the formation of an oxametallacycle intermediate that leads to unique selectivity in styrene oxidation. {\textcopyright} 2010 American Chemical Society.",

keywords = "Active sites, Catalytic properties and selectivity, Density-functional theory, Ligand-covered gold nanoparticles, Quasi-icosahedral Au55 core",

author = "Yong Pei and Nan Shao and Yi Gao and Zeng, {Xiao Cheng}",

note = "Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].",

year = "2010",

month = apr,

day = "27",

doi = "10.1021/nn100184m",

language = "English",

volume = "4",

pages = "2009--2020",

journal = "ACS Nano",

issn = "1936-0851",

publisher = "American Chemical Society",

number = "4",

}

TY - JOUR

T1 - Investigating active site of gold nanoparticle Au55(PPh 3)12Cl6 in selective oxidation

AU - Pei, Yong

AU - Shao, Nan

AU - Gao, Yi

AU - Zeng, Xiao Cheng

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

PY - 2010/4/27

Y1 - 2010/4/27

N2 - We present an ab initio investigation of structural, electronic, catalytic, and selective properties of the ligand-covered gold nanoparticle Au 55(PPh3)12Cl6 and associated model clusters. The catalytic activity of the Au55(PPh3) 12Cl6 nanoparticle in the presence of O2 stems from a combined effect of triphenylphosphine ligands and surface structure of the "magic-number" quasi-icosahedral Au55 core, which entails numerous ligand-encompassed triangle Au6 faces as the active sites. Under the Eley-Rideal mechanism, the "triangle-socket" active site not only can accommodate one pre-adsorbed O2 (which is subsequently activated to the superoxo species) with one styrene molecule at a time but also can provide spatial confinement which favors the formation of an oxametallacycle intermediate that leads to unique selectivity in styrene oxidation. © 2010 American Chemical Society.

AB - We present an ab initio investigation of structural, electronic, catalytic, and selective properties of the ligand-covered gold nanoparticle Au 55(PPh3)12Cl6 and associated model clusters. The catalytic activity of the Au55(PPh3) 12Cl6 nanoparticle in the presence of O2 stems from a combined effect of triphenylphosphine ligands and surface structure of the "magic-number" quasi-icosahedral Au55 core, which entails numerous ligand-encompassed triangle Au6 faces as the active sites. Under the Eley-Rideal mechanism, the "triangle-socket" active site not only can accommodate one pre-adsorbed O2 (which is subsequently activated to the superoxo species) with one styrene molecule at a time but also can provide spatial confinement which favors the formation of an oxametallacycle intermediate that leads to unique selectivity in styrene oxidation. © 2010 American Chemical Society.

KW - Active sites

KW - Catalytic properties and selectivity

KW - Density-functional theory

KW - Ligand-covered gold nanoparticles

KW - Quasi-icosahedral Au55 core

UR - http://www.scopus.com/inward/record.url?scp=77951704002&partnerID=8YFLogxK

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-77951704002&origin=recordpage

U2 - 10.1021/nn100184m

DO - 10.1021/nn100184m

M3 - RGC 21 - Publication in refereed journal

SN - 1936-0851

VL - 4

SP - 2009

EP - 2020

JO - ACS Nano

JF - ACS Nano

IS - 4

ER -