Delivery of electrons by proton-hole transfer in ice at 10 K: Role of surface OH radicals
Delivery of electrons by proton-hole transfer in ice at 10 K: Role of surface OH radicals
复制标题
10 K 冰中质子空穴转移传递电子：表面 OH 自由基的作用
DOI：
10.1021/acs.jpclett.0c03345
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发表时间：
2021
影响因子：
4.4
通讯作者：
N. Watanabe
中科院分区：
文献类型：
--
作者：
K. Kitajima;Y. Nakai;W. M. C. Sameera;M. Tsuge;A. Miyazaki;H. Hidaka;A. Kouchi;N. Watanabe
尽管水冰被广泛接受为通过氢键系统转移过量质子来携带正电荷，但最近发现冰在低于50 K的温度下同时暴露于电子和紫外光子时是负电荷导体。在这项工作中，电子传递的机制被证实实验通过测量电流通过冰和监测光解的OH自由基在冰上通过使用一种新的方法。表面OH自由基显着减少后出现的负电流，表明电子传递的质子空穴（OH-）转移引发的冰表面上的OH-生产。通过密度泛函理论计算，对质子-空穴转移机制进行了合理化解释。
Although water ice has been widely accepted to carry a positive charge via the transfer of excess protons through a hydrogen-bonded system, ice was recently found to be a negative charge conductor upon simultaneous exposure to electrons and ultraviolet photons at temperatures below 50 K. In this work, the mechanism of electron delivery was confirmed experimentally by both measuring currents through ice and monitoring photodissociated OH radicals on ice by using a novel method. The surface OH radicals significantly decrease upon the appearance of negative current flow, indicating that the electrons are delivered by proton-hole (OH–) transfer in ice triggered by OH–production on the surface. The mechanism of proton-hole transfer was rationalized by density functional theory calculations.