Platinum single-atom adsorption on graphene: a density functional theory study

Abstract

Single-atom catalysis, which utilizes single atoms as active sites, is one of promising ways to enhance the catalytic activity and to reduce the amount of precious metals used. Here by means of density functional theory based thermodynamics we show that the single platinum atoms preferentially adsorb on the substitutional carbon sites at the hydrogen terminated graphene edge.

Single Pt Atoms on N-Doped Graphene: Atomic Structure and Local Electronic States

“…6 It has been confirmed that graphene in the first layer does not affect the binding energy of Pt atoms in the second layer. 8 The atomic structures used for the calculations are shown in Figures S8− S12. We optimized the structure and calculated the binding energy defined by…”

“…3−5 We have achieved single Pt atoms adsorbed on graphene by plasma sputtering. 6 Because the catalytic activity of a single atom depends largely on its atomic structure, the adsorption structure of Pt atoms has been experimentally 7 and theoretically 8,9 studied. There is a report on the catalytic activity of single Pt atoms adsorbed on the edge of graphene, 10,11 but the atomic arrangement has not been clarified.…”

Electron-beam introduction of heteroatomic Pt–Si structures in graphene

“…Pt attached to a topological defect (5-7-5 member rings) shows a slightly higher binding energy of 2.55 eV (not shown). 30 During the acquisition of a HAADF-STEM image (as shown in Figure 2e, for example), on the order of four million electron impacts are delivered to the Pt atom without inducing any instability and thus, it is likely there is an underlying defect in the graphene acting as a stabilizer.…”

Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies

“…The DFT calculations in the present paper are carried out using the STATE [34,68] code with norm-conserving pseudopotentials [69]. The plane-wave basis set is used to expand wave functions (charge density) with cutoff energy of 64 Ry (400 Ry).…”

“…In addition, more recent HAADF-STEM measurements have even observed single Pt atoms dispersed on undoped [15,16] and nitrogendoped [17] graphene, which show high catalytic activities and CO tolerance. Theoretically, on the other hand, firstprinciples calculations based on density functional theory (DFT) have been performed extensively to clarify the properties of graphene-supported Pt clusters from viewpoints of geometric [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34] and magnetic [35][36][37][38][39][40][41][42][43][44] structures, molecular adsorptions [45][46][47][48][49][50], CO tolerance [51][52][53][54], and catalytic reactions such as CO oxidation [55][56][57][58][59][60], decomposition of O 3…”