Noble Metal Ion‐Directed Assembly of 2D Materials for Heterostructured Catalysts and Metallic Micro‐Texturing
Noble Metal Ion‐Directed Assembly of 2D Materials for Heterostructured Catalysts and Metallic Micro‐Texturing
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DOI：
10.1002/adfm.202215222
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发表时间：
2023-05
影响因子：
19
通讯作者：
Joshua M. Little;Jia-yue Sun;A. Kamali;Amy Chen;A. Leff;Yang Li;Leah K. Borden;T. Dissanayake;Deborah Essumang;Benita O. Oseleononmen;Dongxia Liu;T. Woehl;Po‐Yen Chen
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文献类型：
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作者：
Joshua M. Little;Jia-yue Sun;A. Kamali;Amy Chen;A. Leff;Yang Li;Leah K. Borden;T. Dissanayake;Deborah Essumang;Benita O. Oseleononmen;Dongxia Liu;T. Woehl;Po‐Yen Chen
将2D材料（2DM）纳米片组装成具有增强功能的微观和宏观架构需要有效的策略来克服纳米片的重新堆叠。传统的组装方法涉及外部粘合剂和/或功能化，这不可避免地牺牲了2DM的纳米级特性。贵金属离子（NMI）是一种很有前途的离子交联剂，它可以同时组装2DM纳米片并诱导协同性能。在此，筛选了NMI-2DM复合物的集合并将其分类为两个亚组。基于zeta电位，开发了两种组装方法以获得1）用于异质结构催化剂的NMI交联的2DM水凝胶/气凝胶和2）用于模板合成的NMI-2DM油墨。首先，硝酸四氨铂（II）（TPtN）作为一种有效的离子交联剂团聚各种2DM分散体。通过利用微纹理组装平台，以可扩展的方式制造各种TPtN-2DM水凝胶。之后，将这些水凝胶冻干并热还原以合成Pt修饰的2DM气凝胶（Pt@2DM）。Pt@2DM异质结构表现出高的底物依赖性催化活性，并在3-硝基苯乙烯的氢化中促进不同的反应途径。第二，PtCl 4可以以高NMI摩尔浓度掺入2DM分散体中以制备一系列具有高胶体稳定性的PtCl 4 -2DM油墨。通过采用PtCl 4-氧化石墨烯油墨，合成了具有复制形貌的各种Pt微结构，并精确控制了晶粒尺寸和孔隙率。
Assembling 2D‐material (2DM) nanosheets into micro‐ and macro‐architectures with augmented functionalities requires effective strategies to overcome nanosheet restacking. Conventional assembly approaches involve external binders and/or functionalization, which inevitably sacrifice 2DM's nanoscale properties. Noble metal ions (NMI) are promising ionic crosslinkers, which can simultaneously assemble 2DM nanosheets and induce synergistic properties. Herein, a collection of NMI–2DM complexes are screened and categorized into two sub‐groups. Based on the zeta potentials, two assembly approaches are developed to obtain 1) NMI‐crosslinked 2DM hydrogels/aerogels for heterostructured catalysts and 2) NMI–2DM inks for templated synthesis. First, tetraammineplatinum(II) nitrate (TPtN) serves as an efficient ionic crosslinker to agglomerate various 2DM dispersions. By utilizing micro‐textured assembly platforms, various TPtN–2DM hydrogels are fabricated in a scalable fashion. Afterward, these hydrogels are lyophilized and thermally reduced to synthesize Pt‐decorated 2DM aerogels (Pt@2DM). The Pt@2DM heterostructures demonstrate high, substrate‐dependent catalytic activities and promote different reaction pathways in the hydrogenation of 3‐nitrostyrene. Second, PtCl4 can be incorporated into 2DM dispersions at high NMI molarities to prepare a series of PtCl4–2DM inks with high colloidal stability. By adopting the PtCl4–graphene oxide ink, various Pt micro‐structures with replicated topographies are synthesized with accurate control of grain sizes and porosities.