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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect
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Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect

机译:光催化剂的光合作用:由铁(iii)工程缺陷捕获和稳定的单个原子铂

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摘要

Single atom (SA), noble metal catalysts are of interest due to high projected catalytic activity while minimizing cost. Common issues facing many synthesis methodologies include complicated processes, low yields of SA product, and production of mixtures of SA and nanoparticles (NPs). Herein we report a simple, room-temperature synthesis of single Pt-atom decorated, anatase Fe-doped TiO_(2) particles that leverages the Fe dopant as an engineered defect site to photodeposit and stabilize atomically dispersed Pt. Both particle morphology and Fe dopant location are based on thermodynamic principles (Gibbs–Wulff construction). CO–DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) reveals absence of bridge-bonded CO signal, confirming atomically dispersed Pt. XAS (X-ray absorption spectroscopy) of both Pt and Fe indicates Fe–O–Pt bonding that persists through catalytic cycling. Mass balance indicates that the Pt loading on single particles is 2.5 wt % Pt; the single Pt-atom decorated nanoparticle yield is 17%. Pt-containing particles show more than an order-of-magnitude increased photooxidation efficiency relative to particles containing only Fe. High single-atom-Pt yield, ease of synthesis, and high catalytic activity demonstrate the utility and promise of this method. The principles of this photodeposition synthesis allow for its generalizability toward other SA metals of catalytic interest.
机译:单原子(SA)贵金属催化剂因其高的预期催化活性而备受关注,同时将成本降至最低。许多合成方法面临的共同问题包括复杂的工艺、SA产品的低产率以及SA和纳米颗粒(NPs)混合物的生产。在此,我们报道了一种简单的室温合成单铂原子修饰的锐钛矿型掺杂铁的TiO_2粒子的方法,该粒子利用铁掺杂剂作为工程缺陷位点来光沉积和稳定原子分散的铂。颗粒形态和铁掺杂剂位置均基于热力学原理(吉布斯-伍尔夫结构)。CO–DRIFTS(漫反射红外傅里叶变换光谱)显示没有桥结CO信号,证实铂原子分散。Pt和Fe的X射线吸收光谱(XAS)表明,Fe–O–Pt键通过催化循环持续存在。质量平衡表明,单个颗粒上的铂含量为2.5 wt%Pt;单铂原子修饰的纳米颗粒产率为17%。与仅含铁的颗粒相比,含铂颗粒的光氧化效率提高了一个数量级以上。高单原子铂收率、易合成性和高催化活性证明了该方法的实用性和前景。这种光沉积合成的原理可以推广到其他具有催化作用的SA金属。

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