Exploring the synergistic effect of palladium nanoparticles and highly dispersed transition metals on carbon nitride/super-activated carbon composites for boosting electrocatalytic activity
2024
Alemany Molina, Gabriel | Navlani-García, Miriam | Juan Juan, Jerónimo | Morallon, Emilia | Cazorla-Amorós, Diego | Alemany Molina, Gabriel | Cazorla-Amorós, Diego | Morallon, Emilia | Navlani-García, Miriam | Universidad de Alicante. Departamento de Química Inorgánica | Universidad de Alicante. Departamento de Química Física | Universidad de Alicante. Instituto Universitario de Materiales | Materiales Carbonosos y Medio Ambiente | Electrocatálisis y Electroquímica de Polímeros
In the present work, multifunctional electrocatalysts formed by palladium nanoparticles (Pd NPs) loaded on Fe or Cu-containing composite supports, based on carbon nitride (C3N4) and super-activated carbon with a high porosity development (SBET 3180 m2/g, VDR 1.57 cm3/g, and VT 1.65 cm3/g), were synthesised. The presence of Fe or Cu sites favoured the formation of Pd NPs with small average particle size and a very narrow size distribution, which agreed with Density Functional Theory (DFT) calculations showing that the interaction of Pd clusters with C3N4 flakes is weaker than with Cu- or Fe-C3N4 sites. The electroactivity was also dependent on the composition and, as suggested by preliminary DFT calculations, the Pd-Cu catalyst showed lower overpotential for hydrogen evolution reaction (HER) while bifunctional oxygen reduction reaction/ oxygen evolution reaction (ORR/OER) behaviour was superior in Pd-Fe sample. The Pd-Fe electrocatalyst was studied in a zinc-air battery (ZAB) for 10 h, showing a performance similar to a commercial Pt/C + RuO2 catalyst with a high content of precious metal. This study demonstrates the synergistic effect between Pd species and transition metals and shows that transition metals anchored on C3N4-based composite materials promote the electroactivity of Pd NPs in HER, ORR and OER due to the interaction between both species.
显示更多 [+] 显示较少 [-]The authors would like to thank PID2021-123079OB-I00 project funded by MCIN/AEI/10.13039/501100011033 and “ERDF A way of making Europe”. G. Alemany-Molina thanks Ministerio de Universidades for the FPU20/03969 grant. M. Navlani-García acknowledges the Ramón y Cajal contract (RYC2021-034199-I) funded by MCIN/AEI/10.13039/501100011033 and the European Union «NextGenerationEU»/PRTR».
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