Abstract
Spinel-type oxides have been acknowledged for their eminent catalytic ability towards alkaline hydrogen evolution reaction (HER) due to the special metal occupying structures. To further improve conductivity, inherited cation doped spinel has been rapidly synthesized via scalable alloying-dealloying strategy. Specially, the resultant Al-doped CoFe2O4 possesses typical bi-continuous pore-ligament structure, showing a huge surface area for electrocatalysis. It only demands HER overpotentials of 22.9 and 275 mV to achieve 10 and 100 mA cm-2, respectively. Furthermore, it also exhibits ultra-stable hydrogen evolution for 1000 h Under the industrial conditions (6 M KOH, 60 °C), Al-CoFe2O4 || RuO2 couple just needs 1.75 V to reach high current density of 500 mA cm-2 and could steadily produce hydrogen for over 50 h with merely 8 % voltage loss. Theoretical calculation confirms that Al substitution could indeed increase valence electron concentration. Based on this optimized configuration, H2O molecule is preferred to adsorb on Co site and conducive to dissociate into *OH-*H co-adsorption. And thus, the energy barrier of alkaline HER can be reduced to 0.98 eV on Al-doping CoFe2O4 model. To further clarify the active species derived from HER, operando X-ray diffraction and Fourier transform infrared are used to prove that the superficial CoFe2O4 has been transformed into more active CoOOH/FeOOH. This work offers a guide to facilely fabricate cost-effective HER catalysts that are suitable for industrial hydrogen production.
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