Ion-neutral clustering alters gas-phase hydrogen–deuterium exchange rates
Ion-neutral clustering alters gas-phase hydrogen–deuterium exchange rates
复制标题
离子中性聚集改变气相氢氘交换率
DOI：
10.1039/d2cp04388b
复制
发表时间：
2023
影响因子：
3.3
通讯作者：
Clowers, Brian H.
中科院分区：
文献类型：
--
作者：
Schramm, Haley M.;Tamadate, Tomoya;Hogan, Christopher J.;Clowers, Brian H.
相界处发生的化学反应的速率和机制通常与本体溶液中的化学行为有很大不同，但仍然难以量化。离子-中性相互作用就是这样一类化学反应，其在溶剂化初期阶段的行为与本体溶液不同，但在气溶胶形成、大气化学和气相离子分离中起着关键作用。通过利用氘蒸气逆流的气相离子分离技术，我们量化了一系列模型化学系统（即氨基酸）上氢-氘交换（HDX）和离子中性聚类的程度。通过同时量化蒸气缔合度和 HDX，可以了解簇形成对反应动力学的影响。这些结果意味着在模拟复杂的成核过程和生物聚合物结构动力学时不能忽视簇的形成。
The rates and mechanisms of chemical reactions that occur at a phase boundary often differ considerably from chemical behavior in bulk solution, but remain difficult to quantify. Ion–neutral interactions are one such class of chemical reactions whose behavior during the nascent stages of solvation differs from bulk solution while occupying critical roles in aerosol formation, atmospheric chemistry, and gas-phase ion separations. Through a gas-phase ion separation technique utilizing a counter-current flow of deuterated vapor, we quantify the degree of hydrogen–deuterium exchange (HDX) and ion–neutral clustering on a series of model chemical systems (i.e. amino acids). By simultaneously quantifying the degree of vapor association and HDX, the effects of cluster formation on reaction kinetics are realized. These results imply that cluster formation cannot be ignored when modeling complex nucleation processes and biopolymer structural dynamics.