caa a22 4500 606174265 CHVBK 20210128100737.0 cr unu---uuuuu 210128e20150801xx s 000 0 eng 10.1007/s11244-015-0398-5 doi (NATIONALLICENCE)springer-10.1007/s11244-015-0398-5 Conquering Catalyst Complexity: Nanoparticle Synthesis and Instrument Development for Molecular and Atomistic Characterisation Under In Situ Conditions [Elektronische Daten] [G. Somorjai, S. Beaumont] Most heterogeneous, homogeneous and enzyme catalysts are nanoparticles. Conquering the complexity of such materials' mode of operation at the atomic and molecular level necessitates being able to elucidate their structure under operational conditions. Here, we show examples of the crucial interplay of atomic or molecular resolution in situ techniques with atomically and molecularly well-defined nanoparticle catalysts to achieve this goal. In particular we focus on mono-dispersed metal nanoparticles in the 0.8-10nm range with precise size distribution provided by modern colloidal synthetic techniques. These have been used in conjunction with a range of in situ techniques for understanding the complexity of a number of catalytic phenomena. Drawing on the nanoparticle size discrimination afforded by this approach, most metal nanoparticle catalysed covalent bond making/breaking reactions are identified as being structure sensitive, even when that was previously not thought to be the case. Small nanoparticles, below 2nm, have been found to have changes of electronic structure that give rise to high oxidation state clusters under reaction conditions. These have been utilized to heterogenize typically homogeneous catalytic reactions using metal nanoclusters in the range of 40 atoms or less to carry out reactions on their heterogenized surfaces that would typically be expected only to occur at the higher oxidation state metal centre of a homogeneous organometallic catalyst. The combination of in situ techniques and highly controlled metal nanoparticle structure also allows valuable insights to be achieved in understanding the mechanisms of multicomponent catalysts, catalysis occurring in different fluid phases and phenomena occurring at the metal-oxide interface. Springer Science+Business Media New York, 2015 Heterogeneous catalysis nationallicence In situ spectroscopy nationallicence Nanoparticles nationallicence Particle-size nationallicence Oxidation state nationallicence Somorjai G. Department of Chemistry, University of California, 94720, Berkeley, CA, USA aut Beaumont S. Department of Chemistry, Durham University, Science Site, South Road, DH1 3LE, Durham, UK aut Topics in Catalysis Springer US; http://www.springer-ny.com 58/10-11(2015-08-01), 560-572 1022-5528 58:10-11<560 2015 58 11244 https://doi.org/10.1007/s11244-015-0398-5 text/html Onlinezugriff via DOI BK010053 XK010053 XK010000 Metadata rights reserved Springer special CC-BY-NC licence nationallicence 1 research-article jats NATIONALLICENCE NATIONALLICENCE NL-springer NATIONALLICENCE 856 40 https://doi.org/10.1007/s11244-015-0398-5 text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Somorjai G. Department of Chemistry, University of California, 94720, Berkeley, CA, USA aut NATIONALLICENCE 700 1- Beaumont S. Department of Chemistry, Durham University, Science Site, South Road, DH1 3LE, Durham, UK aut NATIONALLICENCE 773 0- Topics in Catalysis Springer US; http://www.springer-ny.com 58/10-11(2015-08-01), 560-572 1022-5528 58:10-11<560 2015 58 11244