Chemical Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, USA.
J Synchrotron Radiat. 2023 May 1;30(Pt 3):634-642. doi: 10.1107/S1600577523002783. Epub 2023 Apr 17.
Nucleation and growth of minerals has broad implications in the geological, environmental and materials sciences. Recent developments in fast X-ray nanotomography have enabled imaging of crystal growth in solutions in situ with a resolution of tens of nanometres, far surpassing optical microscopy. Here, a low-cost, custom-designed aqueous flow cell dedicated to the study of heterogeneous nucleation and growth of minerals in aqueous environments is shown. To gauge the effects of radiation damage from the imaging process on growth reactions, radiation-induced morphological changes of barite crystals (hundreds of nanometres to ∼1 µm) that were pre-deposited on the wall of the flow cell were investigated. Under flowing solution, minor to major crystal dissolution was observed when the tomography scan frequency was increased from every 30 min to every 5 min (with a 1 min scan duration). The production of reactive radicals from X-ray induced water radiolysis and decrease of pH close to the surface of barite are likely responsible for the observed dissolution. The flow cell shown here can possibly be adopted to study a wide range of other chemical reactions in solutions beyond crystal nucleation and growth where the combination of fast flow and fast scan can be used to mitigate the radiation effects.
矿物成核和生长在地质、环境和材料科学中具有广泛的意义。快速 X 射线纳米断层扫描技术的最新发展使得能够以数十纳米的分辨率原位成像溶液中的晶体生长,远远超过了光学显微镜。本文展示了一种低成本、定制设计的用于研究水相环境中矿物异质成核和生长的水相流池。为了评估成像过程中的辐射损伤对生长反应的影响,研究了预先沉积在流池壁上的重晶石晶体(数百纳米至约 1μm)的辐射诱导形貌变化。在流动溶液中,当断层扫描频率从每 30 分钟增加到每 5 分钟(扫描时间为 1 分钟)时,观察到较小到较大的晶体溶解。X 射线诱导水辐射分解产生的反应性自由基和重晶石表面附近 pH 值的降低可能是观察到的溶解的原因。这里展示的流池可能可以用于研究除晶体成核和生长以外的其他广泛的溶液化学反应,其中快速流动和快速扫描的组合可以用来减轻辐射影响。