碱金属交换在沸石模板碳合成中的作用

Erin E. Taylor, D. Compton, Gary F. Wyss, N. Stadie
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引用次数: 1

摘要

尽管在最大孔径沸石的孔隙网络中实现理想的碳原子填充已经付出了巨大的努力,但目前合成的沸石模板碳(ZTC)材料普遍存在镀膜不准确的问题。理想化的模型表明,如果选择合适的沸石模板(例如,D表面schwarzite的faujasite),并且可以实现完美的模板保真度(直接在沸石表面插入原始的纯碳层),原则上可以通过沸石模板获得长期寻找的类schwarzite结构。实现这种结构的要求是增加沸石内的碳密度。我们报告了一系列碱金属阳离子交换沸石的调查,以确定第1族元素的周期趋势如何影响沸石模板,特别关注结构堆积密度(SPD)的测量,通过非原位热重法解决。在一项基于受控合成温度、时间和流动条件的调查中,观察到SPD随着阳离子尺寸的减小而增加,这一效应与阳离子-π相互作用强度的增加相一致。这一效应有望在未来的工作中提高ztc的SPD,用于合成闭管、类施瓦茨石的碳质固体。
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The Role of Alkali Metal Exchange in Zeolite-Templated Carbon Synthesis
Despite great efforts to achieve ideal atomistic packing of carbon in the pore networks of even the largest pore zeolites, tem - plating inaccuracies are ubiquitous in all presently synthesized zeolite-templated carbon (ZTC) materials. Idealized models suggest that the long-sought schwarzite-like structures could in principle be obtained by zeolite templating if the appropriate zeolite template were chosen ( e.g. , faujasite for D surface schwarzites) and if perfect template fidelity (insertion of a pristine layer of pure carbon directly on the surface of the zeolite) could be achieved. A requirement to achieve such structures is increased carbon density within the zeolite. We report the investigation of a series of alkali metal cation-exchanged zeolites to determine how the periodic trends in the group 1 elements influence zeolite templating, with a specific focus on the metric of structural packing density (SPD) as resolved by ex situ thermogravimetry. In a survey based on controlled synthesis tempera - ture, time, and flow conditions, an increasing SPD was observed with decreasing cation size, an effect that is consistent with the increasing strength of cation-π interactions. This effect could be promising for future work to increase the SPD of ZTCs for the synthesis of closed-tube, schwarzite-like carbonaceous solids.
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