Design of Effective Catalysts for Selective Alkyne Hydrogenation by Doping of Ceria with a Single-Atom Promotor

Journal of the American Chemical Society
Christopher RileyAbhaya Datye

Abstract

Since the discovery that ceria is an active catalyst for selective hydrogenation of alkynes, there has been much debate on the catalytic mechanism. In this work, we propose, based on density functional theory (DFT) investigations, a mechanism that involves the heterolytic dissociation of H2 at oxygen vacancies of CeO2(111), facilitated by frustrated Lewis pairs consisting of spatially separated O and Ce sites. The resulting O-H and Ce-H species effectively catalyze the hydrogenation of acetylene, avoiding the overstabilization of the C2H3* intermediate in a previously proposed mechanism. On the basis of our mechanism, we propose the doping of ceria by Ni as a means to create oxygen vacancies. Interestingly, the Ni dopant is not directly involved in the catalytic reaction, but serves as a single-atom promoter. Experimental studies confirm the design principles and demonstrate much higher activity for Ni-doped ceria in selective hydrogenation of acetylene. The combined results from DFT calculations and experiment provide a basis to further develop selective hydrogenation catalysts based on earth-abundant materials.

References

Dec 15, 1994·Physical Review. B, Condensed Matter·P E Blöchl
Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Jul 6, 2001·Journal of the American Chemical Society·K SohlbergS J Pennycook
Jul 30, 2005·Science·Friedrich EschRenzo Rosei
Jul 21, 2006·The Journal of Physical Chemistry. B·Stefano FabrisStefano Baroni
Sep 29, 2006·The Journal of Physical Chemistry. B·Gianpaolo VicarioStefano Baroni
Mar 23, 2007·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Hsin-Tsung ChenM C Lin
Mar 5, 2009·Physical Review Letters·M Verónica Ganduglia-PirovanoJoachim Sauer
Jul 20, 2012·Angewandte Chemie·Gianvito ViléJavier Pérez-Ramírez
Jan 29, 2013·Chemical Reviews·Eric W McFarland, Horia Metiu
Jul 10, 2014·The Journal of Chemical Physics·Delia Fernández-TorreRubén Pérez
Aug 26, 2014·Angewandte Chemie·Gianvito ViléJavier Pérez-Ramírez
Dec 24, 2014·Physical Chemistry Chemical Physics : PCCP·Xin-Ping WuGuanzhong Lu
May 15, 2015·Angewandte Chemie·Douglas W Stephan, Gerhard Erker
Jun 28, 2017·Journal of the American Chemical Society·Zili WuAnibal J Ramirez-Cuesta
Jul 12, 2017·Angewandte Chemie·Davide AlbaniJavier Pérez-Ramírez
Nov 14, 2017·Journal of the American Chemical Society·Kristin WernerHans-Joachim Freund
Mar 28, 2018·Physical Chemistry Chemical Physics : PCCP·Tian CaoWeixin Huang
Jul 8, 2018·Nature Communications·Davide AlbaniJavier Pérez-Ramírez

❮ Previous
Next ❯

Citations

Aug 14, 2019·Angewandte Chemie·Zhaorui LiHans-Joachim Freund
Jan 11, 2020·Chemical Society Reviews·Xiao WangHongjie Zhang
Sep 2, 2020·Chemical Society Reviews·Lulu LiJinlong Gong
Jul 23, 2020·Environmental Science and Pollution Research International·Yanli LiangYaoqiang Chen
Feb 14, 2019·Journal of Materials Chemistry. B, Materials for Biology and Medicine·Wei SongXiaofeng Lu
Feb 18, 2021·Chemical Society Reviews·Yalan WangDe Chen
Mar 17, 2021·Journal of the American Chemical Society·Kunlong LiuNanfeng Zheng
Jul 27, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Zhaorui Li, Weixin Huang
Oct 30, 2019·The Journal of Physical Chemistry Letters·Wenhui ZhongJun Jiang
Feb 23, 2020·Journal of the American Chemical Society·K B Sravan KumarBert D Chandler
Apr 4, 2020·Chemical Reviews·Shufang JiYadong Li
Aug 14, 2020·Chemical Reviews·Ruixuan QinNanfeng Zheng
Oct 22, 2020·Chemical Reviews·Selina K KaiserJavier Pérez-Ramírez
Oct 29, 2020·Chemical Reviews·Rui LangTao Zhang
May 24, 2019·The Journal of Physical Chemistry Letters·Tongtong YangJun Jiang
Nov 18, 2021·Journal of the American Chemical Society·Douglas W Stephan
Dec 3, 2021·Journal of the American Chemical Society·Xin DengLandong Li

❮ Previous
Next ❯

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.