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Facet-Selective Dissociation and Radical-Mediated Reaction of Dibenzotetrathiafulvalene Molecules on Low-Index Copper Surfaces
journal contribution
posted on 2022-01-14, 17:34 authored by Jun Zhang, Linwei Zhou, Pengcheng Chen, Bingkai Yuan, Zhihai Cheng, Wei Ji, Xiaohui QiuCatalytic
bond cleavage and formation of transient intermediates
on metal substrates play an essential role in surface synthesis and
heterogeneous catalysis. Previous studies usually focus on the bond-breaking
process, whereas the knowledge regarding the construction of dissociative
moieties that lead to the final products is limited. Here, we investigate
the facet-selective dissociation of dibenzotetrathiafulvalene (DBTTF)
molecules on Cu(110) and Cu(100) surfaces using low-temperature scanning
tunneling microscopy and first-principles calculations. Atomic resolution
images enable the identification of various intermediates and reaction
pathways on different facets. The dissociation of DBTTF molecules
generated 1,2-BDT–Cu complex chains on Cu(110), while phenyl
diradical superstructure islands were observed on Cu(100). The various
chemical species found on different Cu facets were explained in the
context of their formation energies related to the spatial inhomogeneity
of surface electronic states. Our results address the effects of electronic
and geometrical diversities on the surface mobility of intermediate
products and subsequent on-surface reaction pathways.
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Keywords
metal substrates playsurfaces using lowformation energies relatedsurface electronic statessurface reaction pathwaysdifferent cu facetsdifferent facetsreaction pathwayssurface synthesissurface mobilitymediated reactionvarious intermediatestransient intermediatesspatial inhomogeneityresults addressprinciples calculationsknowledge regardingintermediate productsheterogeneous catalysisgeometrical diversitiesfinal productsessential roledissociative moietiesbreaking process