Plasmon-Generated Solvated Electrons for Chemical Transformations.
Plasmon-Generated Solvated Electrons for Chemical Transformations.
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用于化学转化的等离激元产生的溶剂化电子。
DOI：
10.1021/jacs.2c07768
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发表时间：
2022
影响因子：
15
通讯作者：
Halas,NaomiJ
中科院分区：
文献类型：
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作者：
Solti,David;Chapkin,KyleD;Renard,David;Bayles,Aaron;Clark,BenjaminD;Wu,Gang;Zhou,Jingyi;Tsai,Ah-Lim;Kürti,László;Nordlander,Peter;Halas,NaomiJ
产生溶剂化电子（溶液中的自由电子）的方法主要集中在碱金属离子化或高能电子或光子上。在这里，我们报告的溶剂化电子的产生，通过激发等离子体共振的铝纳米晶体悬浮在溶液中的可见光。进行了两个化学反应：与自旋捕获2-甲基-2-亚硝基丙烷的自由基加成反应和与自由基时钟6-溴己-1-烯的模型环化反应。从测量的自由基时钟反应浓度可以推断出等离子体吸收光子到溶剂化电子产生的至少1.1%的量子效率。这项研究展示了一种简单的方法来产生溶剂化电子驱动还原有机化学反应在一个可量化和控制的方式。
Methods for generating solvated electrons─free electrons in solution─have focused primarily on alkali metal ionization or high-energy electrons or photons. Here we report the generation of solvated electrons by exciting the plasmon resonance of Al nanocrystals suspended in solution with visible light. Two chemical reactions were performed: a radical-addition reaction with the spin-trap 2-methyl-2-nitrosopropane, and a model cyclization reaction with the radical clock 6-bromohex-1-ene. A quantum efficiency of at least ∼1.1% for plasmon absorbed photon to solvated electron generation can be inferred from the measured radical clock reaction concentration. This study demonstrates a simple way to generate solvated electrons for driving reductive organic chemical reactions in a quantifiable and controlled manner.