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Anchoring Pt Single Atoms on Te Nanowires for Plasmon‐Enhanced Dehydrogenation of Formic Acid at Room Temperature

机译:在室温下将Te纳米线上的Pt单原子固定用于等离子体的甲酸增强脱氢

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摘要

Formic acid (HCOOH), as a promising hydrogen carrier, is renewable, safe, and nontoxic. However, the catalytic dehydrogenation of HCOOH is typically conducted at elevated temperature. Here, HCOOH decomposition is successfully achieved for hydrogen production on the developed Pt single atoms modified Te nanowires with the Pt mass loading of 1.1% (1.1%Pt/Te) at room temperature via a plasmon‐enhanced catalytic process. Impressively, 1.1%Pt/Te delivers 100% selectivity for hydrogen and the highest turnover frequency number of 3070 h−1 at 25 °C, which is significantly higher than that of Pt single atoms and Pt nanoclusters coloaded Te nanowires, Pt nanocrystals decorated Te nanowires, and commercial Pt/C. A plasmonic hot‐electron driven mechanism rather than photothermal effect domains the enhancement of catalytic activity for 1.1%Pt/Te under light. The transformation of HCOO* to CO2 δ * on Pt atoms is proved to be the rate‐determining step by further mechanistic studies. 1.1%Pt/Te exhibits tremendous catalytic activity toward the decomposition of HCOOH owing to its plasmonic hot‐electron driven mechanism, which efficiently stimulates the rate‐determining step. In addition, hot electrons generated by the Te atoms nearby Pt single atoms are regarded to directly inject into the reactants adsorbed and activated on Pt single atoms.
机译:甲酸(HCOOH)作为有前途的氢载体,具有可再生,安全且无毒的特点。但是,HCOOH的催化脱氢通常在高温下进行。在这里,已开发的Pt单原子修饰的Te纳米线成功地实现了HCOOH分解,该氢在室温下通过等离激元增强的催化过程实现了1.1%(1.1%Pt / Te)的Pt质量负载。令人印象深刻的是,1.1%Pt / Te对氢具有100%的选择性,并且在25°C时的最高周转频率为3070 h -1 ,远高于Pt单原子和Pt纳米团簇的载频Te纳米线,Pt纳米晶体装饰了Te纳米线,以及商用Pt / C。等离子体热电子驱动机制而非光热效应决定了在光下对1.1%Pt / Te的催化活性的增强。进一步的机理研究证明,HCOO *向Pt原子上的CO2 δ - *的转化是决定速率的步骤。 1.1%Pt / Te由于其等离子体热电子驱动机理,对HCOOH的分解具有巨大的催化活性,从而有效地刺激了速率确定步骤。另外,Pt单原子附近的Te原子产生的热电子被认为直接注入吸附和活化在Pt单原子上的反应物中。

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