SSZ-13 Crystallization by Particle Attachment and Deterministic Pathways to Crystal Size Control,Journal of the American Chemical Society

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SSZ-13 Crystallization by Particle Attachment and Deterministic Pathways to Crystal Size Control
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2015-09-30 , DOI: 10.1021/jacs.5b07477
Manjesh Kumar ₁ , Helen Luo ₂ , Yuriy Román-Leshkov ₂ , Jeffrey D. Rimer ₁

Affiliation

Many synthetic and natural crystalline materials are either known or postulated to grow via nonclassical pathways involving the initial self-assembly of precursors that serve as putative growth units for crystallization. Elucidating the pathway(s) by which precursors attach to crystal surfaces and structurally rearrange (postattachment) to incorporate into the underlying crystalline lattice is an active and expanding area of research comprising many unanswered fundamental questions. Here, we examine the crystallization of SSZ-13, which is an aluminosilicate zeolite that possesses exceptional physicochemical properties for applications in separations and catalysis (e.g., methanol upgrading to chemicals and the environmental remediation of NO(x)). We show that SSZ-13 grows by two concerted mechanisms: nonclassical growth involving the attachment of amorphous aluminosilicate particles to crystal surfaces and classical layer-by-layer growth via the incorporation of molecules to advancing steps on the crystal surface. A facile, commercially viable method of tailoring SSZ-13 crystal size and morphology is introduced wherein growth modifiers are used to mediate precursor aggregation and attachment to crystal surfaces. We demonstrate that small quantities of polymers can be used to tune crystal size over 3 orders of magnitude (0.1-20 μm), alter crystal shape, and introduce mesoporosity. Given the ubiquitous presence of amorphous precursors in a wide variety of microporous crystals, insight of the SSZ-13 growth mechanism may prove to be broadly applicable to other materials. Moreover, the ability to selectively tailor the physical properties of SSZ-13 crystals through molecular design offers new routes to optimize their performance in a wide range of commercial applications.

中文翻译：

SSZ-13 通过粒子附着结晶和晶体尺寸控制的确定性途径

许多合成和天然结晶材料是已知的或假定通过非经典途径生长，包括作为假定的结晶生长单元的前体的初始自组装。阐明前体附着到晶体表面并在结构上重新排列（后附着）以纳入底层晶格的途径是一个活跃且不断扩大的研究领域，包括许多未解决的基本问题。在这里，我们检查了 SSZ-13 的结晶，它是一种铝硅酸盐沸石，具有用于分离和催化应用的特殊物理化学性质（例如，甲醇升级为化学品和 NO(x) 的环境修复）。我们表明 SSZ-13 通过两种协同机制增长：非经典生长包括无定形铝硅酸盐颗粒与晶体表面的附着，以及通过分子的结合以推进晶体表面上的台阶的经典逐层生长。引入了一种简便、商业上可行的定制 SSZ-13 晶体尺寸和形态的方法，其中使用生长调节剂来调节前体聚集和附着到晶体表面。我们证明少量聚合物可用于调整超过 3 个数量级 (0.1-20 μm) 的晶体尺寸、改变晶体形状并引入介孔率。鉴于无定形前体在各种微孔晶体中普遍存在，对 SSZ-13 生长机制的了解可能被证明广泛适用于其他材料。而且，

更新日期：2015-09-30

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