Polyoxometalate-Derived Ultrasmall Pt2W/WO3 Heterostructure Outperforms Platinum for Large-Current-Density H2 Evolution
Polyoxometalate-Derived Ultrasmall Pt2W/WO3 Heterostructure Outperforms Platinum for Large-Current-Density H2 Evolution
复制标题
多金属氧酸盐 — 衍生的超小型 Pt 2 W/WO 3 异质结构在大电流 — 密度 H 2 演化方面优于铂
DOI：
10.1002/aenm.201900597
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发表时间：
2019-07-01
影响因子：
27.8
通讯作者：
Lu, Tong-Bu
中科院分区：
文献类型：
--
作者：
Peng, Ye-Wang;Shan, Changsheng;Lu, Tong-Bu
为解决能源消耗和环境污染问题，具有高铂利用率的铂基催化剂引起了广泛关注。本文采用一步电化学方法，通过向Preyssler阴离子[NaP 5 W30 O 110]（14-）中注入多电子，与阳极易潮解的Pt阳离子共沉积，在还原氧化石墨烯（RGO）上构建了超细异质结构Pt 2 W/WO 3。该催化剂在大电流密度下的析氢性能远高于商业Pt催化剂，其析氢电流密度可达500 mA cm-2，过电位仅为394 mV，远低于20%Pt/C的析氢过电位（578 mV）。与对照实验和密度泛函理论（DFT）计算结果的比较表明，Pt 2 W/WO 3/RGO催化剂活性的提高主要是由于不同组分的协同作用，使其能够快速、连续地脱氢，而20%Pt/C催化剂在相同条件下由于电极表面形成大气泡而不能正常运行.将高催化活性和放氢能力有效地整合到单一材料中，可以产生具有显著稳定性的用于大电流密度析氢的先进材料。
Platinum (Pt)-based catalysts with high Pt utilization efficiency for efficient H-2 evolution are attracting extensive attention to meet the issues of energy exhaustion and environmental pollution. Herein, a one-step electrochemical method is demonstrated to construct ultrafine heterostructure Pt2W/WO3 on reduced graphene oxide (RGO) by injecting multielectrons into the Preyssler anion [NaP5W30O110](14-) to codeposit with anodic deliquescent Pt cations. The resulting Pt2W/WO3/RGO shows much higher performance than that of commercial Pt catalysts for large-current-density H-2 evolution, which can deliver a large current density of 500 mA cm(-2) with an overpotential of only 394 mV, much lower than that of 20% Pt/C (578 mV). Comparisons with control experiments and density functional theory (DFT) calculations both suggest that the much enhanced activity can be mainly attributed to the synergistic cooperation of different components to drive fast and continuous hydrogen desorption on Pt2W/WO3/RGO, while it could not run normally for 20% Pt/C under similar conditions due to the formation of huge bubbles on the electrode surface. The effective integration of high catalytic activity and hydrogen desorption ability into a single material can yield advanced materials for large-current-density H-2 evolution with remarkable stability.