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  Cooperative Chemisorption-Induced Physisorption of CO2 Molecules by Metal–Organic Chains

Feng, M., Petek, H., Shi, Y., Sun, H., Zhao, J., Calaza, F., et al. (2015). Cooperative Chemisorption-Induced Physisorption of CO2 Molecules by Metal–Organic Chains. ACS Nano, 9(12), 12124-12136. doi:10.1021/acsnano.5b05222.

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Feng, Min1, 2, Author
Petek, Hrvoje1, Author
Shi, Yongliang3, Author
Sun, Hao3, Author
Zhao, Jin1, 3, 4, Author
Calaza, Florencia5, Author           
Sterrer, Martin5, 6, Author           
Freund, Hans-Joachim5, Author           
1Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States, ou_persistent22              
2Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China, ou_persistent22              
3Hefei National Laboratory for Physical Sciences at Microscale and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China, ou_persistent22              
4Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China, ou_persistent22              
5Chemical Physics, Fritz Haber Institute, Max Planck Society, ou_24022              
6Institute of Physics, University of Graz, Universitätsplatz 5, A-8010 Graz, Austria, ou_persistent22              


Free keywords: CO2; CO2δ−; CO2 reduction; CO2 cluster; chemisorption induced physisorption; metal−organic chains; 1,4-phenylene diisocyanide
 Abstract: Effective CO2 capture and reduction can be achieved through a molecular scale understanding of interaction of CO2 molecules with chemically active sites and the cooperative effects they induce in functional materials. Self-assembled arrays of parallel chains composed of Au adatoms connected by 1,4-phenylene diisocyanide (PDI) linkers decorating Au surfaces exhibit self-catalyzed CO2 capture leading to large scale surface restructuring at 77 K (ACS Nano 2014, 8, 8644–8652). We explore the cooperative interactions among CO2 molecules, Au-PDI chains and Au substrates that are responsible for the self-catalyzed capture by low temperature scanning tunneling microscopy (LT-STM), X-ray photoelectron spectroscopy (XPS), infrared reflection absorption spectroscopy (IRAS), temperature-programmed desorption (TPD), and dispersion corrected density functional theory (DFT). Decorating Au surfaces with Au-PDI chains gives the interfacial metal–organic polymer characteristics of both a homogeneous and heterogeneous catalyst. Au-PDI chains activate the normally inert Au surfaces by promoting CO2 chemisorption at the Au adatom sites even at <20 K. The CO2δ− species coordinating Au adatoms in-turn seed physisorption of CO2 molecules in highly ordered two-dimensional (2D) clusters, which grow with increasing dose to a full monolayer and, surprisingly, can be imaged with molecular resolution on Au crystal terraces. The dispersion interactions with the substrate force the monolayer to assume a rhombic structure similar to a high-pressure CO2 crystalline solid rather than the cubic dry ice phase. The Au surface supported Au-PDI chains provide a platform for investigating the physical and chemical interactions involved in CO2 capture and reduction.


Language(s): eng - English
 Dates: 2015-08-182015-11-072015-11-072015-12-22
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acsnano.5b05222
 Degree: -



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Title: ACS Nano
Source Genre: Journal
Publ. Info: Washington, DC : American Chemical Society
Pages: 13 Volume / Issue: 9 (12) Sequence Number: - Start / End Page: 12124 - 12136 Identifier: Other: 1936-0851
CoNE: https://pure.mpg.de/cone/journals/resource/1936-0851