Pacific Northwest National Laboratory , Richland, Washington 99354, United States.
ACS Appl Mater Interfaces. 2017 Sep 27;9(38):32907-32919. doi: 10.1021/acsami.7b10290. Epub 2017 Sep 14.
In this paper, aluminosilicate aerogels were used as scaffolds for silver nanoparticles to capture I(g). The starting materials for these scaffolds included Na-Al-Si-O and Al-Si-O aerogels, both synthesized from metal alkoxides. The Ag particles were added by soaking the aerogels in aqueous AgNO solutions followed by drying and Ag reduction under H/Ar to form Ag crystallites within the aerogel matrix. In some cases, aerogels were thiolated with 3-(mercaptopropyl)trimethoxysilane as an alternative method for binding Ag. During the Ag-impregnation steps, for the Na-Al-Si-O aerogels, Na was replaced with Ag, and for the Al-Si-O aerogels, Si was replaced with Ag. The Ag-loading of thiolated versus nonthiolated Na-Al-Si-O aerogels was comparable at ∼35 atomic %, whereas the Ag-loading in unthiolated Al-Si-O aerogels was significantly lower at ∼7 atomic % after identical treatment. Iodine loadings in both thiolated and unthiolated Ag-functionalized Na-Al-Si-O aerogels were >0.5 m m (denoting the mass of iodine captured per starting mass of the sorbent) showing almost complete utilization of the Ag through chemisorption to form AgI. Iodine loading in the thiolated and Ag-functionalized Al-Si-O aerogel was 0.31 m m. The control of Ag uptake over solution residence time and [Ag] demonstrates the ability to customize the Ag-loading in the base sorbent to regulate the loading capacity of iodine.
本文使用铝硅酸盐气凝胶作为银纳米粒子的支架来捕获 I(g)。这些支架的起始材料包括由金属醇盐合成的 Na-Al-Si-O 和 Al-Si-O 气凝胶。通过将气凝胶浸泡在含有 AgNO3 的水溶液中,然后在 H/Ar 下干燥和还原 Ag,在气凝胶基质中形成 Ag 晶体,从而添加 Ag 颗粒。在某些情况下,气凝胶通过 3-(巯丙基)三甲氧基硅烷进行巯基化,作为结合 Ag 的替代方法。在 Ag 浸渍步骤中,对于 Na-Al-Si-O 气凝胶,Na 被 Ag 取代,而对于 Al-Si-O 气凝胶,Si 被 Ag 取代。巯基化和非巯基化 Na-Al-Si-O 气凝胶的 Ag 负载量相当,约为 35 个原子%,而经过相同处理后,非巯基化 Al-Si-O 气凝胶的 Ag 负载量明显较低,约为 7 个原子%。在巯基化和非巯基化的 Ag 功能化 Na-Al-Si-O 气凝胶中,碘的负载量均大于 0.5mm(表示每起始质量的吸附剂捕获的碘的质量),表明通过化学吸附形成 AgI 几乎完全利用了 Ag。巯基化和 Ag 功能化 Al-Si-O 气凝胶中的碘负载量为 0.31mm。通过控制 Ag 在溶液中的停留时间和[Ag]的吸收量,证明可以控制基础吸附剂中的 Ag 负载量来调节碘的负载能力。