Single-atom catalysts are promising platforms for heterogeneous catalysis, especially for clean energy conversion, storage, and utilization. Although great efforts have been made to examine the bonding and oxidation state of single-atom catalysts before and/or after catalytic reactions, when information about dynamic evolution is not sufficient, the underlying mechanisms are often overlooked. Herein, we report the direct observation of the charge transfer and bond evolution of a single-atom Pt/C3 N4 catalyst in photocatalytic water splitting by synchronous illumination X-ray photoelectron spectroscopy. Specifically, under light excitation, we observed Pt-N bond cleavage to form a Pt0 species and the corresponding C=N bond reconstruction; these features could not be detected on the metallic platinum-decorated C3 N4 catalyst. As expected, H2 production activity (14.7 mmol h-1  g-1 ) was enhanced significantly with the single-atom Pt/C3 N4 catalyst as compared to metallic Pt-C3 N4 (0.74 mmol h-1  g-1 ).

中文翻译：

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在单原子Pt / C3 N4催化剂中动态键演化的直接观察。

单原子催化剂是多相催化，特别是清洁能源转化，存储和利用的有前途的平台。尽管在检查催化反应之前和/或之后付出了巨大的努力来检查单原子催化剂的键合和氧化态，但是当有关动态演变的信息不足时，通常会忽略潜在的机理。在这里，我们报告通过同步照明X射线光电子能谱直接观察光催化水分解中单原子Pt / C3 N4催化剂的电荷转移和键演化。具体而言，在光激发下，我们观察到Pt-N键断裂形成Pt0物种并进行相应的C = N键重构。这些特征在金属铂装饰的C3 N4催化剂上无法检测到。不出所料