Although proton transport in water ice is well understood, proton–hole transfer (PHT) involving proton abstraction by anions remains less explored. This study investigates PHT in H₂S and NH₃ solids at low temperatures, aiming to determine whether these solids exhibit negative charge transport similar to that in ice. In H₂S and NH₃ solids at 10 K, surface HS^– and NH₂^– anions in hydrogen-bonded systems trigger negative current flow, providing a clear signature of PHT. This negative current is controlled by electron flow and 193 nm ultraviolet irradiation, which generates HS^– and NH₂^– anions on the solid surfaces. In bilayer H₂S/H₂O and NH₃/H₂O solids, a significant negative current is observed only in the NH₃/H₂O solid, which is attributed to the exothermic proton abstraction by NH₂^– from H₂O at the bilayer interface, a process not available for H₂S on ice. This study is the first to demonstrate PHT-induced electrochemical behavior in hydrogen-bonded solids other than ice.

中文翻译：

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10 K 氢键固体中质子-空穴转移的特征


尽管水冰中的质子传输已广为人知，但涉及阴离子提取质子的质子-空穴转移 （PHT） 仍未得到充分探索。本研究调查了低温下 H₂S 和 NH₃ 固体中的 PHT，旨在确定这些固体是否表现出类似于冰中的负电荷传输。在 10 K 的 H₂S 和 NH₃ 固体中，氢键系统中的表面 HS^- 和 NH₂^- 阴离子会触发负电流，提供 PHT 的明显特征。该负电流由电子流和 193 nm 紫外线照射控制，从而在固体表面产生 HS^– 和 NH₂^– 阴离子。在双层 H₂S/H₂O 和 NH₃/H₂O 固体中，仅在 NH₃/H₂O 固体中观察到显着的负电流，这归因于 NH₂^– 在双层界面处从 H₂O 中抽出放热质子，这一过程不适用于冰上的 H₂S。这项研究首次证明了 PHT 在除冰以外的氢键固体中诱导的电化学行为。