In recent years, the use of single atoms (SAs) has become of a rapidly increasing significance in photocatalytic H₂ generation; here SA noble metals (mainly Pt SAs) can act as highly effective co-catalysts. The classic strategy to decorate oxide semiconductor surfaces with maximally dispersed SAs relies on “strong electrostatic adsorption” (SEA) of suitable noble metal complexes. In the case of TiO₂ – the classic benchmark photocatalyst – SEA calls for adsorption of cationic Pt complexes such as [(NH₃)₄Pt]²⁺ which then are thermally reacted to surface-bound SAs. While SEA is widely used in literature, in the present work it is shown by a direct comparison that reactive attachment based on the reductive anchoring of SAs, e.g., from hexachloroplatinic(IV) acid (H₂PtCl₆) leads directly to SAs in a configuration with a significantly higher specific activity than SAs deposited with SEA – and this at a significantly lower Pt loading and without any thermal post-deposition treatments. Overall, the work demonstrates that the reactive deposition strategy is superior to the classic SEA concept as it provides a direct electronically well-connected SA-anchoring and thus leads to highly active single-atom sites in photocatalysis.

中文翻译：

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反应沉积与强静电吸附 (SEA)：光催化制氢中高活性单原子助催化剂的关键

近年来，单原子（SA）的使用在光催化H ₂生成中的重要性迅速增加。SA贵金属（主要是Pt SA）可以作为高效的助催化剂。用最大分散的 SA 装饰氧化物半导体表面的经典策略依赖于合适的贵金属配合物的“强静电吸附”（SEA）。_{就 TiO 2} （经典基准光催化剂）而言，SEA 需要吸附阳离子 Pt 络合物，例如 [(NH ₃ ) ₄ Pt] ²⁺，然后与表面结合的 SA 发生热反应。虽然SEA在文献中广泛使用，但在目前的工作中，通过直接比较表明，基于SAs的还原锚定的反应性连接，例如，来自六氯铂(IV)酸(H 2 PtCl 6 )的反应性_连接直接_导致SAs配置比 SEA 沉积的 SA 具有显着更高的比活性，并且 Pt 负载量显着降低且无需任何热沉积后处理。总体而言，该工作表明，反应沉积策略优于经典的 SEA 概念，因为它提供了直接电子连接良好的 SA 锚定，从而在光催化中产生高活性的单原子位点。