Abstract
A series of Cu@Pd/C with different Pd contents was prepared using the galvanic reduction method to disperse Pd on the surface of Cu nanoparticles on Cu/C. The dispersion of Pd was regulated by the Cu(I) on the surface, which was introduced by pulse oxidation. The Cu2O did not react during the galvanic reduction process and restricted the Pd atoms to a specific area. The pulse oxidation method was demonstrated to be an effective process to control the oxidization degree of Cu on Cu/C and then to govern the dispersion of Pd. The catalysts were characterized by transmission electron microscopy (TEM), high-resolution transmission electron microscope (HRTEM), high angular annular dark field scanning TEM (HAADF-STEM), energy-dispersive spectroscopy (EDS) mapping, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), auger electron spectroscopy (AES), and inductively coupled plasma optical emission spectrometer (ICP-OES), which were used to catalyze the hydrogen evolution from ammonia borane. The Cu@Pd/C had much higher activity than the PdCu/C, which was prepared by the impregnation method. The TOF increased as the Cu2O in Cu/C used for the preparation of Cu@Pd/C increased, and the maximum TOF was 465 molH2 min−1 molPd−1 at 298 K on Cu@Pd0.5/C-640 (0.5 wt % of Pd, 640 mL of air was pulsed during the preparation of Cu/C-640). The activity could be maintained in five continuous processes, showing the strong stability of the catalysts.
Highlights
Safe and convenient hydrogen storage is one of the key problems that have emerged in the application of hydrogen as clean energy
In Cu/C used for the preparation of Cu@Pd/C increased, and the maximum turnover frequency (TOF) was 465 molH2 min−1 molPd −1 at 298 K on Cu@Pd0.5 /C-640 (0.5 wt % of Pd, 640 mL of air was pulsed during the preparation of Cu/C-640)
The dispersion of Pd atoms based on our previous work on the preparation of Pd catalysts [73–78], we synthesized Cu@Pd/C with on the surface of Cu nanoparticles was regulated by partial oxidation of the surface of Cu controllable Pd dispersion through the galvanic reduction method
Summary
Safe and convenient hydrogen storage is one of the key problems that have emerged in the application of hydrogen as clean energy. How to control the distribution of galvanic reduction process, the noble metal atoms tended to aggregate into large particles on the noble metals on the surface of non-noble metals needs further consideration. How to control the distribution of based on our previous work on the preparation of Pd catalysts [73–78], we synthesized Cu@Pd/C noble metals on the surface of non-noble metals needs further consideration In this manuscript, with controllable Pd dispersion through the galvanic reduction method. The dispersion of Pd atoms based on our previous work on the preparation of Pd catalysts [73–78], we synthesized Cu@Pd/C with on the surface of Cu nanoparticles was regulated by partial oxidation of the surface of Cu controllable Pd dispersion through the galvanic reduction method. The aggregation of Pd atoms to form larger particles was prevented by the surrounding Cu(I) species
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