Wu Qianbao, Yang Na, Xiao Mengjun, Wang Wei, Cui Chunhua
Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 611731, Chengdu, China.
School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, China.
Nat Commun. 2024 Oct 23;15(1):9145. doi: 10.1038/s41467-024-53526-5.
Near-neutral HCO aqueous solution plays an essential role in respiratory, mineralization and catalysis, yet the interconversion between hydrated CO, HCO and CO and the associated proton transfer under such proton-deficient conditions remain uncovered. Here we reveal that cation enables HCO to self-dissociate into OH and CO through a pH-independent process, where CO hydration and subsequent proton transfer in acid-base reactions lead to the overall exchange of oxygen isotopes between HCO and HO tracked by oxygen isotope-labeled Raman spectroscopy. Isolating HCO from cations with crown ether impedes HCO dissociation and the following reactions. Further molecular dynamics simulations demonstrate that the interplay between HCO and hydrated cations drives HCO dissociation. This study suggests a natural proton channel upon coupling HCO with cations.
近中性的HCO水溶液在呼吸、矿化和催化过程中起着至关重要的作用，然而在这种质子缺乏的条件下，水合CO、HCO和CO之间的相互转化以及相关的质子转移仍未被揭示。在这里，我们发现阳离子能够使HCO通过一个与pH无关的过程自解离为OH和CO，其中CO水合以及随后酸碱反应中的质子转移导致了通过氧同位素标记拉曼光谱追踪的HCO和HO之间氧同位素的整体交换。用冠醚将HCO与阳离子分离会阻碍HCO的解离及后续反应。进一步的分子动力学模拟表明，HCO与水合阳离子之间的相互作用驱动了HCO的解离。这项研究表明了一种将HCO与阳离子偶联的天然质子通道。
