1 research outputs found
Atomically Dispersed Pd‑N<sub>1</sub>C<sub>3</sub> Sites on a Nitrogen-Doped Carbon Nanosphere for Semi-hydrogenation of Acetylene
Rationally designing efficient catalysts for semi-hydrogenation
of acetylene is significant but challenging. Herein, Pd isolated single-atom
sites (ISAS) on a covalent-organic-framework (COF)-derived nanosphere
(Pd-ISAS/CN) are synthesized by a COF-absorption–pyrolysis
strategy. This synthetic strategy is also applicable for Pt and Ru
ISAS catalysts, demonstrating that it is a general method to synthesize
noble-metal ISAS on COF-derived carbon materials. Pd-ISAS/CN exhibits
outstanding reactivity and high selectivity for semi-hydrogenation
of acetylene, with 92% conversion of acetylene, 80% selectivity toward
ethylene at 100 °C, and corresponding activity is as high as
712 molacetylene molmetal–1 h–1. Extended X-ray absorption fine structure
(EXAFS) measurement and density functional theory (DFT) calculation
reveal the Pd-N1C3 sites from Pd-ISAS/CN efficiently
boost the reactivity for semi-hydrogenation of acetylene. This work
will bring inspiration to rationally design noble-metal-based ISAS
catalysts derived from COF materials and boost catalytic performance
by optimizing the coordination environment of catalytic sites