Abstract
We have studied the effect of unsupported Pd nanoparticle (NP) size in the selective C≡C semi-hydrogenation of alkynols with different alkyl chains, i.e., C16 in dehydroisophytol (DIP) (to isophytol (IP)) vs C1 in 2-methyl-3-butyn-2-ol (MBY) (to 2-methyl-3-buten-2-ol (MBE)). The Pd NPs were synthesized via colloidal technique with poly(N-vinyl-2-pyrrolidone) (PVP) as stabilizing agent where a range of crystal sizes (2.1–9.8 nm; confirmed by HRTEM) was generated. Both reactions show antipathetic structure sensitivity consistent with higher specific activity (TOF) over larger Pd NPs where the structure sensitivity effect is more pronounced for NPs ≤ 3.0 nm. All the Pd NPs exhibit high (≥88%) selectivity to the target alkenol product at almost complete (98%) conversion. Increased IP selectivity (SIP; XDIP=98%ca. 95%) was observed over smaller (2.1–3.0 nm) Pd NPs while ca. 98% selectivity to MBE (SMBE; XDIP=98%) is obtained irrespective of particle size. The kinetic results were consistent with a Langmuir–Hin...
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