Metal–support interaction is of great significance for catalysis as it can induce charge transfer between metal and support, tame electronic structure of supported metals, impact adsorption energy of reaction intermediates, and eventually change the catalytic performance. Here, we report the metal size-dependent charge transfer reversal, that is, electrons transfer from platinum single atoms to sulfur-doped carbons and the carbon supports conversely donate electrons to Pt when their size is expanded to ~1.5 nm cluster. The electron-enriched Pt nanoclusters are far more active than electron-deficient Pt single atoms for catalyzing hydrogen evolution reaction, exhibiting only 11 mV overpotential at 10 mA cm−2 and a high mass activity of 26.1 A mg−1 at 20 mV, which is 38 times greater than that of commercial Pt/C. Our work manifests that the manipulation of metal size-dependent charge transfer between metal and support opens new avenues for developing high-active catalysts.
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机译：金属与载体的相互作用对于催化具有重要意义，因为它可以诱导金属与载体之间的电荷转移，载体金属的驯服电子结构，影响反应中间体的吸附能并最终改变催化性能。在这里，我们报道了与金属尺寸有关的电荷转移逆转，即电子从铂单原子转移到掺杂硫的碳，当碳的尺寸扩展到约1.5 nm簇时，碳载体反过来将电子捐赠给Pt。富电子的Pt纳米团簇比缺电子的Pt单个原子具有更高的催化氢释放反应的活性，在10 mA cm −2 时仅表现出11 mV的超电势，质量活性高达26.1 A mg -1 在20 mV时，是商用Pt / C的38倍。我们的工作表明，操纵金属在金属与载体之间的尺寸依赖性电荷转移，为开发高活性催化剂开辟了新途径。
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