Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H2 on Au
Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H2 on Au
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DOI：
10.1021/nl303940z
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发表时间：
2013-01-01
期刊：
影响因子：
10.8
通讯作者：
Halas, Naomi J.
中科院分区：
文献类型：
--
作者：
Mukherjee, Shaunak;Libisch, Florian;Halas, Naomi J.
多相催化在化学和能源应用中具有极其重要的意义。以定向的、轨道特定的方式将光能耦合到化学反应中的催化剂将大大减少化学转化的能量输入需求，从而彻底改变催化驱动的化学。在这里，我们报告的室温解离的H-2的金纳米粒子使用可见光。在Au纳米颗粒中激发的表面等离子体衰变成热电子，其能量在真空能级和金属的功函数之间。在这种瞬态中，热电子可以转移到吸附在Au纳米颗粒表面上的H-2分子的Feshbach共振中，触发解离。我们通过检测H-2和D-2的解离形成HD分子来探测这一过程，并研究了Au纳米颗粒尺寸和入射光波长对HD形成速率的影响。这项工作为控制金属催化剂上的化学反应开辟了一条新途径。
Heterogeneous catalysis is of paramount importance in chemistry and energy applications. Catalysts that couple light energy into chemical reactions in a directed, orbital-specific manner would greatly reduce the energy input requirements of chemical transformations, revolutionizing catalysis-driven chemistry. Here we report the room temperature dissociation of H-2 on gold nanoparticles using visible light. Surface plasmons excited in the Au nanoparticle decay into hot electrons with energies between the vacuum level and the work function of the metal. In this transient state, hot electrons can transfer into a Feshbach resonance of an H-2 molecule adsorbed on the Au nanoparticle surface, triggering dissociation. We probe this process by detecting the formation of HD molecules from the dissociations of H-2 and D-2 and investigate the effect of Au nanoparticle size and wavelength of incident light on the rate of HD formation. This work opens a new pathway for controlling chemical reactions on metallic catalysts.