In situ observation of photo-induced shortening of single Au nanorod for plasmon-enhanced formic acid dehydrogenation

Fengxia Tong , Xiangxiang Zhang , Zeyan Wang , Yuanyuan Liu , Peng Wang , Hefeng Cheng , Ying. Dai , Zhaoke Zheng , Baibiao Huang
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Abstract

Photo-induced selective shortening strategy was developed to synthesize Au nanorods (NRs) with different aspect ratios, and in situ observation of photo-induced shortening of single Au nanorod was realized, which is helpful for understanding the relationship between SPR decay and geometric nanostructure. The as-synthesized plasmonic Pd–Au NRs exhibit efficient formic acid dehydrogenation. Very impressively, the interfacial interaction between plasmonic bimetallic nanostructures and adsorbed molecules (HCOOH) was explored in situ at the single-particle level. Significant photoluminescence (PL) quenching of Pd–Au NRs was observed when HCOOH contacted the catalyst, confirming the charge transfer between Pd–Au NRs and HCOOH molecules. Finally, we shed light on the catalytic mechanism of plasmon-induced HCOOH dehydrogenation by coupling single-particle PL measurement with finite difference time domain (FDTD) and density functional theory (DFT) calculations.

Abstract Image

等离子体增强甲酸脱氢光致单金纳米棒缩短的原位观察
采用光诱导选择性缩短策略合成不同长径比的金纳米棒,实现了单金纳米棒光诱导缩短的原位观察,有助于理解SPR衰减与几何纳米结构之间的关系。所合成的等离子体Pd-Au nmr表现出高效的甲酸脱氢反应。令人印象深刻的是,在单粒子水平上原位探索了等离子体双金属纳米结构与吸附分子(HCOOH)之间的界面相互作用。当HCOOH接触催化剂时,Pd-Au NRs发生了明显的光致发光(PL)猝灭,证实了Pd-Au NRs与HCOOH分子之间的电荷转移。最后,我们通过耦合单粒子PL测量与时域有限差分(FDTD)和密度泛函理论(DFT)计算,揭示了等离子体诱导HCOOH脱氢的催化机理。
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