Tuning d-band centers by coupling PdO nanoclusters to WO3 nanosheets to promote the oxygen reduction reaction,Journal of Materials Chemistry A

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Tuning d-band centers by coupling PdO nanoclusters to WO3 nanosheets to promote the oxygen reduction reaction
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-22 , DOI: 10.1039/d0ta02840a
Jun-Hyeong Lee _{1,

2,

3,

4} , DaBin Yim _{1,

2,

3,

4} , Jung Hyun Park _{1,

2,

3,

4} , Chi Ho Lee _{2,

3,

4,

5,

6} , Jong-Min Ju _{1,

2,

3,

4} , Sang Uck Lee _{2,

3,

4,

5,

6} , Jong-Ho Kim _{1,

2,

3,

4}

Affiliation

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 WO₃ nanosheets (PdO@WO₃S_x) via direct conversion of metallic 1T-WS₂ nanosheets into WO₃ by spontaneous deposition of PdO onto the nanosheets in H₂O at 50 °C for 1 h. Strong coupling in as-prepared PdO@WO₃S_x was confirmed by observing shifts in binding energy compared to those of pure PdO and WO₃. 1T-MoS₂ nanosheets were partially converted into MoO₃ in an analogous reaction to produce the hybrid MoS_xO₃ but in low yield due to preferential dissolution forming aqueous MoO₄²⁻. The hybrid PdO@WO₃S_x exhibited higher half-wave potential (0.89 V vs. RHE) and limiting current density (−6.24 mA cm⁻²) in the ORR than both PdO@MoS_xO₃ and commercial Pt/C. In addition to its higher electrocatalytic activity, PdO@WO₃S_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@WO₃S_x was upshifted to −2.57 eV, very close to that of Pt. This Pt-like d-band center of PdO@WO₃S_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.

中文翻译：

通过将PdO纳米团簇与WO3纳米片耦合来调节d带中心，以促进氧还原反应

将Pd负载在金属氧化物上是调节其电子结构以增强其在氧还原反应（ORR）中的电催化活性的有效方法。但是，Pd和金属氧化物之间的强耦合通常需要高温合成或退火。在这里，我们报告耦合到WO的PdO纳米团簇的合成温和和有效的方法_3个纳米片（PDO @ WO ₃小号_X）经由金属的直接转换1T-WS _2个纳米片成WO ₃由PdO构成自发沉积到H中纳米片在50°C下₂ O 1 h。制备的PdO @ WO ₃ S _x中的强耦合与纯PdO和WO ₃相比，通过观察结合能的改变证实了PbO3 。1T-MoS ₂纳米片在类似的反应中部分转化为MoO ₃，以生成杂化MoS _x O _3，但由于优先溶解而形成MoO ₄^2-水溶液，因此收率低。混合PdO @ WO ₃ S _x在ORR中显示出比PdO @ MoS _x O ₃和商用Pt / C更高的半波电势（相对于RHE为0.89 V ）和极限电流密度（-6.24 mA cm ^-2）。PdO @ WO ₃除了具有较高的电催化活性外在连续ORR期间，S _x在电催化活性方面显示出比Pt / C更高的耐久性。基于d带中心理论的计算仿真表明，PdO @ WO ₃ S _x中Pd的d带中心上移至-2.57 eV，非常接近Pt。PdO @ WO ₃ S _x的这种类似Pt的d带中心使其在ORR中具有出色的电催化活性。这项工作为PdO杂化催化剂的合成提供了一种简便的方法，并为他们对ORR增强的电催化活性提供了基本的见识。

更新日期：2020-07-14

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