文献类型：期刊文献

英文题名：pH-Dependent Water Clusters in Photoacid Solution: Real-Time Observation by ToF-SIMS at a Submicropore Confined Liquid-Vacuum Interface

作者：Liu, Ying-Ya[1];Hua, Xin[1];Zhang, Zhiwei[1];Zhang, Junji[1];Zhang, Shaoze[2,3];Hu, Ping[1];Long, Yi-Tao[4]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai, Peoples R China;[2]Kunming Univ Sci & Technol, Natl Engn Lab Vacuum Met, Kunming, Yunnan, Peoples R China;[3]Kunming Univ Sci & Technol, Engn Lab Adv Battery & Mat Yunnan Prov, Kunming, Yunnan, Peoples R China;[4]Nanjing Univ, Sch Chem & Chem Engn, State Key Lab Analyt Chem Life Sci, Nanjing, Peoples R China

年份：2020

卷号：8

外文期刊名：FRONTIERS IN CHEMISTRY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000568314000001)】；

基金：This research was supported by the National Natural Science Foundation of China (21705046), Shanghai Sailing Program (17YF1403000), and Shanghai Natural Science Foundation (17ZR1407700).

语种：英文

外文关键词：in-situliquid ToF-SIMS; liquid-vacuum interface; photoacid; water cluster; hydrogen-bonding network

摘要：Water clusters are ubiquitously formed in aqueous solutions by hydrogen bonding, which is quite sensitive to various environment factors such as temperature, pressure, electrolytes, and pH. Investigation of how the environment has impact on water structure is important for further understanding of the nature of water and the interactions between water and solutes. In this work, pH-dependent water structure changes were studied by monitoring the changes for the size distribution of protonated water clusters byin-situliquid ToF-SIMS. In combination with a light illumination system,in-situliquid ToF-SIMS was used to real-time measure the changes of a light-activated organic photoacid under different light illumination conditions. Thus, the proton transfer and pH-mediated water cluster changes were analyzed in real-time. It was found that higher concentration of free protons could lead to a strengthened local hydrogen bonding network as well as relatively larger protonated water clusters in both organic acid and inorganic acid. Besides, the accumulation of protons at the liquid-vacuum interface under light illumination was observed owing to the affinity of organic molecules to the low-pressure gas phase. The application ofin-situliquid ToF-SIMS analysis in combination within-situlight illumination system opened up an avenue to real-time investigate light-activated reactions. Besides, the results regarding water structure changes in acidic solutions showed important insights in related atmospheric and physiochemical processes.