Theoretical insight into the C–H and C–C scission mechanism of ethane on a tetrahedral Pt₄subnanocluster

Abstract

The activation mechanism of C2H6on a Pt4cluster has been theoretically investigated in the ground state and the first excited state potential energy surfaces at the BPW91/Lanl2tz, aug-cc-pvtz//BPW91/Lanl2tz, 6-311++G(d, p) level.

Density Functional Theory Study on the Nucleation and Growth of Ptn Clusters on γ-Al2O3(001) Surface

“…4 Later, theoretically, it was reported that the neutral clusters Pt 2 , Pt 3 , and Pt 4 can activate the first C–H bond of CH 4 with small barriers, accompanied by the breakage of the second C–H bond in CH 4 as the rate-determining step. 5−7 More recently, we have studied the competitive activation mechanism of C–H and C–C bonds in C 2 H 6 and/or C 3 H 8 catalyzed by the Pt n ( n = 1, 2, and 4) cluster 8−12 and explained why the C–H insertion product is experimentally observed while the C–C insertion product is not formed in observable quantity 8,9 and why both Pt 2 and Pt 4 clusters exhibit more promising catalytic performance toward C 2 H 6 activation compared with the Pt atom. 10,12 These experimental and theoretical studies emphasize that the size of transition-metal clusters plays an important role in the catalytic reactivity.…”