ExperimIn the light of these experi

实验根据这些实验观察结果，为了揭示CSP的机理，我们将建模工作的重点放在研究酸浓度对原子级界面动力学的影响上。我们利用反作用力场（ReaxFF）电位进行了分子动力学（MD）模拟[8]。ReaxFF是一种MD程序，能够对高温和高压下的反应性液体/固体界面进行建模。ReaxFF力场参数经过优化，可重现参考反应事件的能量，这些反应是通过使用更精确的方法（例如密度泛函理论）获得的。请注意，ReaxFF可能不会以与参考反应相同的精度再现参数优化过程中未包含的反应事件； [9]因此，应有意识地应用ReaxFF。<br>具有相似化学性质的不同研究，并成功再现了相关的实验结果。[10] 通过使用相同的酸浓度，准备了模拟计算系统以模拟实验条件。准备了初始原子系统以表示CSP最终阶段的开始，在该阶段假定系统处于热力学平衡状态。因此，在孔隙和GB区域之间没有化学势差（即，假定GB和孔隙流体中的溶解物质浓度相等且恒定）。因此，模拟盒涉及ZnO表面和溶剂分子（水，HAc）饱和，并溶解有固定数量的Zn + 2离子。有关计算研究的详细信息，请参见支持信息。为了减少液体含量，

ExperimIn the light of these experimental observations, in order to reveal the mechanism of CSP, we focused our modeling efforts on investigating the impact of acid concentration on interfacial kinetics at the atomistic level. We conducted molecular dynamics (MD) simulations using the reactive force field (ReaxFF) potential[8]. The ReaxFF is an MD procedure that is capable of modeling reactive liquid/solid interfaces at elevated temperatures and pressures. The ReaxFF force field parameters are optimized to reproduce the energetics of reference reaction events which were obtained by using more accurate methods such as density functional theory. Note that ReaxFF may not reproduce reaction events that are not included in the parameter optimization process with same accuracy as reference reactions;[9] therefore, ReaxFF should be applied deliberately. The force field used in this study has been used in several<br>different studies with similar chemistry and successfully reproduced relevant experimental results.[10] Systems in computational simulations were prepared to mimic experimental conditions by using the same acid concentrations. The initial atomistic system was prepared to represent the beginning of the final stage of CSP at which the system was assumed to be at thermodynamic equilibrium; thus, there is no chemical potential difference between the pore and the GB region (i.e., the dissolved material concentrations in the GB and the pore fluid are assumed to be equal and constant).Thereby, the simulation boxes involved the ZnO surface and solvent molecules (water, HAc) saturated with a fixed number of dissolved Zn+2 ions. For details of the computational studies, see the Supporting Information. In order to decrease the liquid content, the systems were slowly heated up to the temperatures at which recrystallization starts.

实验根据这些实验观察，为了揭示CSP的机理，我们将建模的重点放在研究酸浓度对界面动力学的影响上。我们使用反应力场（ReaxFF）势进行分子动力学（MD）模拟[8]。ReaxFF是一个MD程序，能够在高温和高压下模拟反应性液体/固体界面。对ReaxFF力场参数进行了优化，以再现用密度泛函理论等更精确方法获得的参考反应事件的能量学。请注意，ReaxFF不能以与参考反应相同的精度再现参数优化过程中未包含的反应事件；因此，应谨慎使用ReaxFF。本研究中使用的力场已用于<br>不同的研究具有相似的化学性质，并成功地再现了相关的实验结果。[10]在计算模拟系统中，通过使用相同的酸浓度来模拟实验条件。制备初始原子系统是为了表示CSP最后阶段的开始，在此阶段，假设系统处于热力学平衡；因此，孔隙和GB区域之间没有化学电位差（即。，假定溶解物质在GB中的浓度与孔隙流体中的浓度相等且恒定，因此，模拟盒涉及到氧化锌表面和溶剂分子（水，HAc）与一定数量的溶解Zn+2离子饱和。有关计算研究的详细信息，请参阅支持信息。为了降低液相含量，系统被缓慢加热到再结晶开始的温度。<br>