RESUMO
Developing anode catalysts with substantially enhanced activity for hydrogen oxidation reaction (HOR) and CO tolerance performance is of great importance for the commercial applications of proton exchange membrane fuel cells (PEMFCs). Herein, an excellent CO-tolerant catalyst (Pd-WO3 /C) has been fabricated by loading Pd nanoparticles on WO3 via an immersion-reduction route. A remarkably high power density of 1.33 W cm-2 at 80 °C is obtained by using the optimized 3Pd-WO3 /C as the anode catalyst of PEMFCs, and the moderately reduced power density (73% remained) in CO/H2 mixed gas can quickly recover after removal of CO-contamination from hydrogen fuel, which is not possible by using Pt/C or Pd/C as anode catalyst. The prominent HOR activity of 3Pd-WO3 /C is attributed to the optimized interfacial electron interaction, in which the activated H* adsorbed on Pd species can be effectively transferred to WO3 species through hydrogen spillover effect and then oxidized through the H species insert/output effect during the formation of Hx WO3 in acid electrolyte. More importantly, a novel synergetic catalytic mechanism about excellent CO tolerance is proposed, in which Pd and WO3 respectively absorbs/activates CO and H2 O, thus achieving the CO electrooxidation and re-exposure of Pd active sites for CO-tolerant HOR.
RESUMO
Highly active and cost-efficient electrocatalysts for oxygen reduction reaction (ORR) are significant for developing renewable energy conversion devices. Herein, a nanocomposite Fe/ZnS-SNC electrocatalyst with an FeS and ZnS heterojunction on N,S-codoped carbon has been fabricated via a facile one-step sulfonating of the pre-designed Zn- and Fe-organic frameworks. Benefitting from the electron transfer from FeS to adjacent ZnS at the heterointerfaces, the optimized Fe/ZnS-SNC900 catalyst exhibits excellent ORR performances, featuring the half-wave potentials of 0.94 V and 0.81 V in alkaline and acidic media, respectively, which is competitive with the commercial 20 wt.% Pt/C (0.87 and 0.76 V). The flexible Zn-air battery equipping Fe/ZnS-SNC900 affords a higher open-circuit voltage (1.45 V) and power density of 30.2 mW cm-2. Fuel cells assembled with Fe/ZnS-SNC900 as cathodic catalysts deliver a higher power output of 388.3 and 242.8 mW cm-2 in H2-O2 and -air conditions. This work proposes advanced heterostructured ORR electrocatalysts that effectively promote renewable energy conversions.