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Incorporating Transition Metal Phosphides into Metal-Organic Frameworks for Enhanced Photocatalysis.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-09-08 , DOI: 10.1002/anie.202011614
Kang Sun 1 , Meng Liu 2 , Junzhe Pei 1 , Dandan Li 3 , Chunmei Ding 4 , Kaifeng Wu 2 , Hai-Long Jiang 1
Affiliation  

Metal‐organic frameworks (MOFs) have been shown to be an excellent platform in photocatalysis. However, to suppress electron–hole recombination, a Pt cocatalyst is usually inevitable, especially in photocatalytic H2 production, which greatly limits practical application. Herein, for the first time, monodisperse, small‐size, and noble‐metal‐free transitional‐metal phosphides (TMPs; for example, Ni2P, Ni12P5), are incorporated into a representative MOF, UiO‐66‐NH2, for photocatalytic H2 production. Compared with the parent MOF and their physical mixture, both TMPs@MOF composites display significantly improved H2 production rates. Thermodynamic and kinetic studies reveal that TMPs, behaving similar ability to Pt, greatly accelerate the linker‐to‐cluster charge transfer, promote charge separation, and reduce the activation energy of H2 production. Significantly, the results indicate that Pt is thermodynamically favorable, yet Ni2P is kinetically preferred for H2 production, accounting for the higher activity of Ni2P@UiO‐66‐NH2 than Pt@UiO‐66‐NH2.

中文翻译:

将过渡金属磷酸盐结合到金属有机骨架中以增强光催化作用。

金属有机骨架(MOF)已被证明是光催化的绝佳平台。然而,为了抑制电子-空穴复合,通常不可避免地需要Pt助催化剂,特别是在光催化H 2的生产中,这大大限制了实际应用。在此,首次将单分散,小尺寸和无贵金属的过渡金属磷化物(TMPs;例如,Ni 2 P,Ni 12 P 5)掺入代表性的MOF中,UiO-66- NH 2,用于光催化生产H 2。与母体MOF及其物理混合物相比,两种TMPs @ MOF复合材料均显示出显着改善的H 2生产率。热力学和动力学研究表明,具有与Pt相似的能力的TMP极大地加速了连接子到簇的电荷转移,促进了电荷分离,并降低了H 2产生的活化能。值得注意的是,结果表明,Pt在热力学上是有利的,但Ni 2 P在动力学上优选用于H 2产生,这是因为Ni 2 P @ UiO-66-NH 2的活性高于Pt @ UiO-66-NH 2
更新日期:2020-09-08
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