Help Privacy Policy Disclaimer
  Advanced SearchBrowse


  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.

Item is


show Files




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: -



Legal Case


Project information


Source 1

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