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CO-Terminated Platinum Electrodeposition on Nb-Doped Bulk Rutile TiO2

机译：掺N的块状金红石型TiO2上的Co终止的铂电沉积

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摘要

Nanoparticulate platinum on carbon as oxygen reduction electrocatalyst suffers from two major drawbacks, namely, low specific activity of the Pt particles and corrosion instability of the carbon support under hydrogen starvation conditions (reverse current degradation). Both issues can be tackled by Pt thin films on TiO2 support. Platinum films were synthesized on commercially available Nb-doped bulk TiO2 electrodes via electrodeposition from Ar- (bulk amounts) and CO-saturated solutions (monolayer amounts). The platinized electrodes were tested for ORR activity in a voltammetric fashion, and the field-free semiconductor properties were evaluated by a combination of X-ray photoelectron spectroscopy (XPS), spectroscopic ellipsometry (SE), photoelectron yield spectroscopy (PYS), electrochemical impedance spectroscopy (EIS), and bulk conductivity measurements. The deposition of bulk amounts of Pt leads to a situation where the catalytic activity is directly correlated to the conductivity of the electrode. Raising the majority carrier density in the Nb-doped TiO2, via proton intercalation in aqueous HClO4 or glycol, drastically increased the activity. In case of monolayer deposits (CO-terminated deposition), intercalation has practically no effect on activity. Thus, the hypothesis is formed that unfavorable electronic interaction of the TiO2 support with small amounts of platinum drastically reduces ORR activity, an effect which is not observed for monolayer amounts of Pt deposited on gold.
机译：碳上的纳米颗粒铂作为氧还原电催化剂具有两个主要缺点，即Pt颗粒的比活度低和在氢缺乏条件下碳载体的腐蚀不稳定性（逆电流降解）。 TiO2载体上的Pt薄膜可以解决这两个问题。通过电沉积从Ar-（大量）和CO饱和溶液（单层）中，在市售Nb掺杂的块状TiO2电极上合成了铂膜。用伏安法测试了镀铂电极的ORR活性，并通过X射线光电子能谱（XPS），椭圆偏振能谱（SE），光电子屈服能谱（PYS），电化学阻抗的组合来评估无场半导体性能光谱（EIS）和体积电导率测量。大量Pt的沉积导致催化活性与电极的电导率直接相关的情况。通过在HClO4或乙二醇水溶液中插入质子，提高了Nb掺杂的TiO2中的多数载流子密度，从而大大提高了活性。在单层沉积（CO终止沉积）的情况下，插层实际上对活性没有影响。因此，形成了这样的假设：TiO 2载体与少量铂的不利电子相互作用极大地降低了ORR活性，这对于沉积在金上的单层Pt没有观察到。

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