超声波驱动的 TiO2–x 纳米管缺陷工程─迈向高效铂单原子增强光催化水分解,ACS Applied Materials & Interfaces

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超声波驱动的 TiO2–x 纳米管缺陷工程─迈向高效铂单原子增强光催化水分解
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-07-25 , DOI: 10.1021/acsami.3c04811
Mahdi Shahrezaei _{1,

2} , S M Hossein Hejazi _{1,

3} , Hana Kmentova ₁ , Veronika Sedajova ₁ , Radek Zboril _{1,

3} , Alberto Naldoni ₄ , Stepan Kment _{1,

3}

Affiliation

与纳米颗粒催化剂相比，单原子催化剂（SAC）由于其高反应活性和原子效率而表现出优异的催化活性和选择性。然而，稳定基质内的 SAC 及其可控负载以防止单原子聚集仍然是该领域的关键挑战。此外，直接比较单原子与纳米颗粒的（共）催化效果仍然具有很大的挑战性。在这里，我们提出了一种新颖的超声驱动策略，用于稳定高度有序的 TiO ₂纳米管上的 Pt 单原子位点。这种可控的低温缺陷工程能够捕获铂单原子并通过随后的化学浸渍的反应时间控制其含量。与原始二氧化钛纳米管相比，这种新颖的方法能够实现近 50 倍的归一化析氢量。此外，所开发的程序还允许通过在非常稀的六氯铂酸溶液中对基材进行较长的浸渍时间，用超小的纳米粒子来装饰二氧化钛。比较显示，与纳米颗粒相比，铂单原子的归一化氢产量高出 10 倍。机理研究表明，该新方法产生了均匀分布的缺陷，例如氧空位和Ti ³⁺物质，从而有效地捕获并稳定了Pt ²⁺和Pt ⁴⁺单原子。优化后的铂单原子光催化剂在一太阳模拟光下表现出优异的光催化水分解和析氢性能，与传统的热还原方法相比，TOF值提高了一个数量级。基于超声波触发化学陷阱的单原子工程为在金属氧化物支撑层上可控组装稳定且高活性的单原子位点催化剂提供了途径。

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Ultrasound-Driven Defect Engineering in TiO2–x Nanotubes─Toward Highly Efficient Platinum Single Atom-Enhanced Photocatalytic Water Splitting

Single-atom catalysts (SACs) have demonstrated superior catalytic activity and selectivity compared to nanoparticle catalysts due to their high reactivity and atom efficiency. However, stabilizing SACs within hosting substrates and their controllable loading preventing single atom clustering remain the key challenges in this field. Moreover, the direct comparison of (co-) catalytic effect of single atoms vs nanoparticles is still highly challenging. Here, we present a novel ultrasound-driven strategy for stabilizing Pt single-atomic sites over highly ordered TiO₂ nanotubes. This controllable low-temperature defect engineering enables entrapment of platinum single atoms and controlling their content through the reaction time of consequent chemical impregnation. The novel methodology enables achieving nearly 50 times higher normalized hydrogen evolution compared to pristine titania nanotubes. Moreover, the developed procedure allows the decoration of titania also with ultrasmall nanoparticles through a longer impregnation time of the substrate in a very dilute hexachloroplatinic acid solution. The comparison shows a 10 times higher normalized hydrogen production of platinum single atoms compared to nanoparticles. The mechanistic study shows that the novel approach creates homogeneously distributed defects, such as oxygen vacancies and Ti³⁺ species, which effectively trap and stabilize Pt²⁺ and Pt⁴⁺ single atoms. The optimized platinum single-atom photocatalyst shows excellent performance of photocatalytic water splitting and hydrogen evolution under one sun solar-simulated light, with TOF values being one order of magnitude higher compared to those of traditional thermal reduction-based methods. The single-atom engineering based on the creation of ultrasound-triggered chemical traps provides a pathway for controllable assembling stable and highly active single-atomic site catalysts on metal oxide support layers.

更新日期：2023-07-25

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