Atomically-thin two-dimensional sheets for understanding active sites in catalysis
Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called "active sites". However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to th...
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| Published in | Chemical Society reviews Vol. 44; no. 3; pp. 623 - 636 |
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| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
01.01.2015
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called "active sites". However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to the large difference between idealized models and real catalysts. This stimulates us to pursue a suitable material model for studying the active sites-catalytic activity relationship, in which the atomically-thin two-dimensional sheets could serve as an ideal model, owing to their relatively simple type of active site and the ultrahigh fraction of active sites that are comparable to the overall atoms. In this tutorial review, we focus on the recent progress in disclosing the factors that affect the activity of reactive sites, including characterization of atomic coordination number, structural defects and disorder in ultrathin two-dimensional sheets by X-ray absorption fine structure spectroscopy, positron annihilation spectroscopy, electron spin resonance and high resolution transmission electron microscopy. Also, we overview their applications in CO catalytic oxidation, photocatalytic water splitting, electrocatalytic oxygen and hydrogen evolution reactions, and hence highlight the atomic level interplay among coordination number, structural defects/disorder, active sites and catalytic activity in the two-dimensional sheets with atomic thickness. Finally, we also present the major challenges and opportunities regarding the role of active sites in catalysis. We believe that this review provides critical insights for understanding the catalysis and hence helps to develop new catalysts with high catalytic activity.
Atomically-thin two-dimensional sheets can serve as an ideal model to disclose the role of active sites in catalysis. |
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| AbstractList | Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called “active sites”. However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to the large difference between idealized models and real catalysts. This stimulates us to pursue a suitable material model for studying the active sites–catalytic activity relationship, in which the atomically-thin two-dimensional sheets could serve as an ideal model, owing to their relatively simple type of active site and the ultrahigh fraction of active sites that are comparable to the overall atoms. In this tutorial review, we focus on the recent progress in disclosing the factors that affect the activity of reactive sites, including characterization of atomic coordination number, structural defects and disorder in ultrathin two-dimensional sheets by X-ray absorption fine structure spectroscopy, positron annihilation spectroscopy, electron spin resonance and high resolution transmission electron microscopy. Also, we overview their applications in CO catalytic oxidation, photocatalytic water splitting, electrocatalytic oxygen and hydrogen evolution reactions, and hence highlight the atomic level interplay among coordination number, structural defects/disorder, active sites and catalytic activity in the two-dimensional sheets with atomic thickness. Finally, we also present the major challenges and opportunities regarding the role of active sites in catalysis. We believe that this review provides critical insights for understanding the catalysis and hence helps to develop new catalysts with high catalytic activity. Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called "active sites". However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to the large difference between idealized models and real catalysts. This stimulates us to pursue a suitable material model for studying the active sites-catalytic activity relationship, in which the atomically-thin two-dimensional sheets could serve as an ideal model, owing to their relatively simple type of active site and the ultrahigh fraction of active sites that are comparable to the overall atoms. In this tutorial review, we focus on the recent progress in disclosing the factors that affect the activity of reactive sites, including characterization of atomic coordination number, structural defects and disorder in ultrathin two-dimensional sheets by X-ray absorption fine structure spectroscopy, positron annihilation spectroscopy, electron spin resonance and high resolution transmission electron microscopy. Also, we overview their applications in CO catalytic oxidation, photocatalytic water splitting, electrocatalytic oxygen and hydrogen evolution reactions, and hence highlight the atomic level interplay among coordination number, structural defects/disorder, active sites and catalytic activity in the two-dimensional sheets with atomic thickness. Finally, we also present the major challenges and opportunities regarding the role of active sites in catalysis. We believe that this review provides critical insights for understanding the catalysis and hence helps to develop new catalysts with high catalytic activity.Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called "active sites". However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to the large difference between idealized models and real catalysts. This stimulates us to pursue a suitable material model for studying the active sites-catalytic activity relationship, in which the atomically-thin two-dimensional sheets could serve as an ideal model, owing to their relatively simple type of active site and the ultrahigh fraction of active sites that are comparable to the overall atoms. In this tutorial review, we focus on the recent progress in disclosing the factors that affect the activity of reactive sites, including characterization of atomic coordination number, structural defects and disorder in ultrathin two-dimensional sheets by X-ray absorption fine structure spectroscopy, positron annihilation spectroscopy, electron spin resonance and high resolution transmission electron microscopy. Also, we overview their applications in CO catalytic oxidation, photocatalytic water splitting, electrocatalytic oxygen and hydrogen evolution reactions, and hence highlight the atomic level interplay among coordination number, structural defects/disorder, active sites and catalytic activity in the two-dimensional sheets with atomic thickness. Finally, we also present the major challenges and opportunities regarding the role of active sites in catalysis. We believe that this review provides critical insights for understanding the catalysis and hence helps to develop new catalysts with high catalytic activity. Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called "active sites". However, the atomic level interplay between active sites and catalytic activity is still an open question, owing to the large difference between idealized models and real catalysts. This stimulates us to pursue a suitable material model for studying the active sites-catalytic activity relationship, in which the atomically-thin two-dimensional sheets could serve as an ideal model, owing to their relatively simple type of active site and the ultrahigh fraction of active sites that are comparable to the overall atoms. In this tutorial review, we focus on the recent progress in disclosing the factors that affect the activity of reactive sites, including characterization of atomic coordination number, structural defects and disorder in ultrathin two-dimensional sheets by X-ray absorption fine structure spectroscopy, positron annihilation spectroscopy, electron spin resonance and high resolution transmission electron microscopy. Also, we overview their applications in CO catalytic oxidation, photocatalytic water splitting, electrocatalytic oxygen and hydrogen evolution reactions, and hence highlight the atomic level interplay among coordination number, structural defects/disorder, active sites and catalytic activity in the two-dimensional sheets with atomic thickness. Finally, we also present the major challenges and opportunities regarding the role of active sites in catalysis. We believe that this review provides critical insights for understanding the catalysis and hence helps to develop new catalysts with high catalytic activity. Atomically-thin two-dimensional sheets can serve as an ideal model to disclose the role of active sites in catalysis. |
| Author | Lei, Fengcai Gao, Shan Xie, Yi Sun, Yongfu |
| AuthorAffiliation | Hefei National Laboratory for Physical Sciences at Microscale Collaborative Innovation Center of Chemistry for Energy Materials University of Science & Technology of China |
| AuthorAffiliation_xml | – name: Hefei National Laboratory for Physical Sciences at Microscale – name: University of Science & Technology of China – name: Collaborative Innovation Center of Chemistry for Energy Materials |
| Author_xml | – sequence: 1 givenname: Yongfu surname: Sun fullname: Sun, Yongfu – sequence: 2 givenname: Shan surname: Gao fullname: Gao, Shan – sequence: 3 givenname: Fengcai surname: Lei fullname: Lei, Fengcai – sequence: 4 givenname: Yi surname: Xie fullname: Xie, Yi |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/25382246$$D View this record in MEDLINE/PubMed |
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| Notes | Yongfu Sun received his BS degree in the Department of Chemistry at Anhui University (2006) and PhD degree in Inorganic Chemistry from University of Science and Technology of China (2011). After that he worked as a postdoctoral fellow in National Synchrotron Radiation Laboratory. In 2013, Dr Sun joined the Hefei National Laboratory for Physical Sciences at the Microscale as a research associate professor. His current interests include the theoretical computation, controllable synthesis, fine structure characterization, device assembly and energy-related applications of atomically-thick two-dimensional sheets. Shan Gao received his BS degree in chemistry from West Anhui University, China, in 2011. He is currently pursuing his PhD degree in inorganic chemistry at the University of Science and Technology of China, under the supervision of Prof. Yi Xie. His current interests include the synthesis and characterization of nanostructures, especially two-dimensional inorganic graphene analogues and their applications in energy storage and conversion. Yi Xie received her BS degree from Xiamen University (1988) and a PhD from the University of Science and Technology of China (USTC, 1996). She is now a Principal Investigator of Hefei National Laboratory for Physical Sciences at the Microscale and a full professor of the Department of Chemistry, USTC. She was appointed as the Cheung Kong Scholar Professor of inorganic chemistry in 2000 and elected as a member of the Chinese Academy of Sciences in 2013, also a recipient of many awards, including the Chinese National Nature Science Award (2001 and 2012), China Young Scientist Award (2002), China Young Female Scientist Award (2006) and IUPAC Distinguished Women in Chemistry/Chemical Engineering Award (2013). Her research interests are cutting-edge research at four major frontiers: solid state materials chemistry, nanotechnology, energy science and theoretical physics. Fengcai Lei received her BS degree in physics from Shandong Normal University, China, in 2011. She is currently pursuing her PhD in inorganic chemistry at the University of Science and Technology of China, under the supervision of Prof. Yi Xie. Her current interests include the theoretical computation and the underlying physics during studying the atomically thin inorganic graphene analogues. ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
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| Snippet | Catalysis can speed up chemical reactions and it usually occurs on the low coordinated steps, edges, terraces, kinks and corner atoms that are often called... |
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| SubjectTerms | active sites Atomic properties Atomic structure Catalysis Catalysts Catalytic activity Defects Disorders electron paramagnetic resonance spectroscopy electrons hydrogen production oxidation oxygen photocatalysis transmission electron microscopy Two dimensional X-ray absorption spectroscopy |
| Title | Atomically-thin two-dimensional sheets for understanding active sites in catalysis |
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