期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 8, 期 27, 页码 13490-13500出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta02840a
关键词
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资金
- National Research Foundation of Korea - Ministry of Science and ICT [NRF-2017R1A2B2008455, NRF-2018R1A2B6006320]
- National Research Foundation of Korea [22A20130012456] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Supporting Pd on a metal oxide is an effective way to modulate its electronic structure to enhance its electrocatalytic activity in the oxygen reduction reaction (ORR). However, strong coupling between Pd and metal oxides typically requires high-temperature synthesis or annealing. Here, we report a mild and effective approach for synthesis of PdO nanoclusters coupled to WO(3)nanosheets (PdO@WO3Sx)viadirect conversion of metallic 1T-WS(2)nanosheets into WO(3)by spontaneous deposition of PdO onto the nanosheets in H2O at 50 degrees C for 1 h. Strong coupling in as-prepared PdO@WO(3)S(x)was confirmed by observing shifts in binding energy compared to those of pure PdO and WO3. 1T-MoS(2)nanosheets were partially converted into MoO(3)in an analogous reaction to produce the hybrid MoS(x)O(3)but in low yield due to preferential dissolution forming aqueous MoO42-. The hybrid PdO@WO(3)S(x)exhibited higher half-wave potential (0.89 Vvs.RHE) and limiting current density (-6.24 mA cm(-2)) in the ORR than both PdO@MoS(x)O(3)and commercial Pt/C. In addition to its higher electrocatalytic activity, PdO@WO(3)S(x)showed greater durability compared to Pt/C in the electrocatalytic activity during the continuous ORR. Computational simulations based on d-band center theory reveal that the d-band center of Pd in PdO@WO(3)S(x)was upshifted to -2.57 eV, very close to that of Pt. This Pt-like d-band center of PdO@WO(3)S(x)enabled its excellent electrocatalytic activity in the ORR. This work presents a facile approach to the synthesis of PdO hybrid catalysts and provides fundamental insight into their enhanced electrocatalytic activity for the ORR.
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