Investigation of the Catalytic Performance of Pd/CNFs for Hydrogen Evolution from Additive-Free Formic Acid Decomposition

In recent years, research efforts have focused on the development of safe and efficient H2 generation/storage materials toward a fuel-cell-based H2 economy as a long-term solution in the near future. Herein, we report the development of Pd nanoparticles supported on carbon nanofibers (CNFs) via sol-immobilisation and impregnation techniques. Thorough characterisation has been carried out by means of XRD, XPS, SEM-EDX, TEM, and BET. The catalysts have been evaluated for the catalytic decomposition of formic acid (HCOOH), which has been identified as a safe and convenient H2 carrier under mild conditions. The influence of preparation method was investigated and catalysts prepared by the sol-immobilisation method showed higher catalytic performance (PdSI/CNF) than their analogues prepared by the impregnation method (PdIMP/CNF). A high turnover frequency (TOF) of 979 h−1 for PdSI/CNF and high selectivity (>99.99%) was obtained at 30 °C for the additive-free formic acid decomposition. Comparison with a Pd/AC (activated charcoal) catalyst synthesised with sol-immobilisation method using as a support activated charcoal (AC) showed an increase of catalytic activity by a factor of four, demonstrating the improved performance by choosing CNFs as the preferred choice of support for the deposition of preformed colloidal Pd nanoparticles