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Novel approach to study diffusion of hydrogen bearing species in silicate glasses at low temperatures
Chemical Geology ( IF 3.9 ) Pub Date : 2020-12-29 , DOI: 10.1016/j.chemgeo.2020.120037
Thilo Bissbort , Hans-Werner Becker , Sara Fanara , Sumit Chakraborty

Diffusion of hydrogen bearing species in glasses plays a significant role in numerous applications in commercial as well as scientific domains. The investigation of diffusion of water in glasses at low temperatures led to experimental and analytical difficulties in the past. We present a new approach that lets us overcome these complications. Diffusion couples of An50Di50 glass (mol %, NBO/T = 0.67) were produced by coating anhydrous glass substrates with thin films of hydrated glass (~200 nm, ~2 wt% H2O) using pulsed laser deposition (PLD). Bonding the diffusant to the glass matrix of the thin film instead of using free water at the interface during experiments precludes other glass altering processes such as dissolution and precipitation. This allows us to confidently interpret the measured profiles to be a result of diffusion only. Nanoscale concentration profiles that result from diffusion at low temperatures on experimentally feasible time scales were measured with the Nuclear Resonance Reaction Analysis (NRRA, 1H(15N,αγ)12C). The non-destructive nature of NRRA enables us to observe and better understand the evolution of diffusion profiles with time within one sample. Evaluation of the sample quality by EPMA, SEM, optical microscopy, Rutherford backscattering spectroscopy (RBS), and NRRA was performed and confirmed the suitability of the samples for diffusion studies. Experiments at 1 atm in a box furnace and at 2 kbar in a CSPV (pressure medium = water) and an IHPV (pressure medium = Argon) prove that the diffusion couples can be used under various experimental conditions. We present diffusion profiles that were measured in experiments carried out in these devices and discuss the distinct features of each that result from different boundary conditions in the experiments.



中文翻译:

研究低温下含氢物质在硅酸盐玻璃中扩散的新方法

玻璃中含氢物质的扩散在商业和科学领域的许多应用中都起着重要作用。过去,对低温在玻璃中水扩散的研究导致了实验和分析上的困难。我们提出了一种新方法,可以克服这些复杂问题。An50Di50玻璃的扩散对(摩尔%,NBO / T = 0.67)是通过在无水玻璃基板上涂覆水合玻璃薄膜(〜200 nm,〜2 wt%H 2)而制得的O)使用脉冲激光沉积(PLD)。在实验过程中,将扩散剂结合到薄膜的玻璃基体上,而不是在界面处使用游离水,排除了其他玻璃改变过程,例如溶解和沉淀。这使我们可以放心地将测得的轮廓解释为扩散的结果。使用核磁共振反应分析(NRRA,1 H(15 N,αγ12)测量了在低温下在实验上可行的时间尺度上扩散所产生的纳米级浓度分布C)。NRRA的无损性质使我们能够观察并更好地理解一个样品中扩散曲线随时间的变化。通过EPMA,SEM,光学显微镜,卢瑟福背散射光谱(RBS)和NRRA对样品质量进行了评估,并确认了样品适用于扩散研究。在箱式炉中以1个大气压进行的实验以及在CSPV(压力介质=水)和IHPV(压力介质=氩气)中以2 kbar进行的实验证明,该扩散偶可以在各种实验条件下使用。我们介绍了在这些设备中进行的实验中测得的扩散曲线,并讨论了由实验中不同边界条件导致的每种扩散特征。

更新日期:2021-01-11
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