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

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 CO2δ −* 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. Pt single atoms modified Te nanowires with 1.1% Pt mass loading exhibit excellent catalytic activity and selectivity for hydrogen production from formic acid at room temperature via plasmonic catalysis. The HCOO*‐to‐CO2δ −* transformation on Pt single atoms is proved to be the rate‐determining step, which is efficiently stimulated by the plasmonic hot‐electron driven mechanism.