Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles

Nature Communications
Yang-Gang WangRoger Rousseau

Abstract

Catalysis by gold supported on reducible oxides has been extensively studied, yet issues such as the nature of the catalytic site and the role of the reducible support remain fiercely debated topics. Here we present ab initio molecular dynamics simulations of an unprecedented dynamic single-atom catalytic mechanism for the oxidation of carbon monoxide by ceria-supported gold clusters. The reported dynamic single-atom catalytic mechanism results from the ability of the gold cation to strongly couple with the redox properties of the ceria in a synergistic manner, thereby lowering the energy of redox reactions. The gold cation can break away from the gold nanoparticle to catalyse carbon monoxide oxidation, adjacent to the metal/oxide interface and subsequently reintegrate back into the nanoparticle after the reaction is completed. Our study highlights the importance of the dynamic creation of active sites under reaction conditions and their essential role in catalysis.

References

Mar 1, 1985·Physical Review A: General Physics·W G Hoover
Jul 15, 1996·Physical Review. B, Condensed Matter·S GoedeckerJ Hutter
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Sep 19, 2002·Journal of the American Chemical Society·Nuria Lopez, Jens K Nørskov
Aug 11, 2005·Physical Review Letters·Zhi-Pan LiuDavid A King
Jul 27, 2007·Chemical Communications : Chem Comm·Veronica Aguilar-Guerrero, Bruce C Gates
Sep 25, 2007·The Journal of Chemical Physics·Joost VandeVondele, Jürg Hutter
Nov 26, 2008·The Journal of Chemical Physics·Changjun ZhangStephen J Jenkins
Jan 28, 2010·Journal of the American Chemical Society·Changjun ZhangStephen J Jenkins
Nov 4, 2010·Physical Chemistry Chemical Physics : PCCP·Changjun ZhangStephen J Jenkins
Jul 23, 2011·Nature Chemistry·Botao QiaoTao Zhang
Dec 24, 2011·Journal of the American Chemical Society·Hyun You KimGraeme Henkelman
Dec 27, 2012·Journal of the American Chemical Society·Na TaWenjie Shen
Jul 3, 2013·Accounts of Chemical Research·Xiao-Feng YangTao Zhang
Aug 2, 2013·Chemical Communications : Chem Comm·Bruce C Gates
Nov 26, 2013·Accounts of Chemical Research·Maria Flytzani-Stephanopoulos
Jan 1, 2014·Accounts of Chemical Research·Isabel X GreenJohn T Yates

❮ Previous
Next ❯

Citations

Jan 13, 2016·Journal of the American Chemical Society·Jun WangJohn T Yates
Mar 10, 2016·Nature Communications·Chang Hyuck ChoiMinkee Choi
Jul 15, 2016·Journal of the American Chemical Society·Matteo Farnesi CamelloneStefano Fabris
Aug 3, 2016·Journal of the American Chemical Society·Yang-Gang WangRoger Rousseau
Apr 14, 2017·Journal of the American Chemical Society·Jin-Cheng LiuJun Li
May 27, 2017·Physical Chemistry Chemical Physics : PCCP·Sandra HoppeStefan Müller
Oct 21, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Fengyu LiZhongfang Chen
May 14, 2016·Chemistry : a European Journal·Xiao-Na LiSheng-Gui He
Mar 18, 2017·Nanoscale·Ashkan MoradabadiPayam Kaghazchi
Nov 21, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Dragoş-Adrian RoşcaManfred Bochmann
Mar 18, 2016·Physical Chemistry Chemical Physics : PCCP·Xun-Lei DingHua-Yong Zhang
Jul 28, 2017·Nature Communications·Zailei ZhangNing Yan
Jul 28, 2018·Advanced Materials·Max J HülseyNing Yan
Sep 28, 2018·Physical Chemistry Chemical Physics : PCCP·Katherine A ParrishHeriberto Hernández
Aug 7, 2018·Angewandte Chemie·Sharon MitchellJavier Pérez-Ramírez
Oct 26, 2018·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Lan QinXiang-Fei Zhang
Sep 10, 2019·Physical Chemistry Chemical Physics : PCCP·Yongli ShenZihui Xiao
Oct 12, 2019·Physical Chemistry Chemical Physics : PCCP·Xing WangDennis Palagin
Jan 4, 2020·Chemical Communications : Chem Comm·Shubo TianJianping Xie
Jan 11, 2020·Chemical Society Reviews·Xiao WangHongjie Zhang
Feb 14, 2020·Physical Chemistry Chemical Physics : PCCP·Peiyu ChenMartin R Castell
Mar 3, 2020·Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada·Milivoj PlodinecThomas Lunkenbein
Mar 13, 2020·Advanced Materials·Chao LuXi Chen
Aug 13, 2015·Angewandte Chemie·Li-Na WangTong-Mei Ma
Apr 22, 2020·Nature Communications·Atsushi BeniyaYoshihide Watanabe
Aug 25, 2019·Nature Communications·Shu ZhaoTao Zhang
Sep 2, 2020·Chemical Society Reviews·Lulu LiJinlong Gong
Jul 11, 2018·Proceedings of the National Academy of Sciences of the United States of America·Yang HeChongmin Wang
Jan 30, 2020·Nature Communications·Shaobo HanJun Li

❮ Previous
Next ❯

Methods Mentioned

BETA
transmission electron microscopy

Software Mentioned

CP2K

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.