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Selective Covalent Modification of Layered Double Hydroxide Nanoparticles with Tripodal Ligands on Outer and Interlayer Surfaces.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-03-18 , DOI: 10.1021/acs.inorgchem.0c00192 Keisuke Muramatsu 1 , Shiori Hayashi 2 , Yoshiyuki Kuroda 3 , Yuya Oka 2 , Hiroaki Wada 2 , Atsushi Shimojima 2, 4 , Kazuyuki Kuroda 2, 4
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-03-18 , DOI: 10.1021/acs.inorgchem.0c00192 Keisuke Muramatsu 1 , Shiori Hayashi 2 , Yoshiyuki Kuroda 3 , Yuya Oka 2 , Hiroaki Wada 2 , Atsushi Shimojima 2, 4 , Kazuyuki Kuroda 2, 4
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Layered double hydroxides (LDHs) have occupied an important place in the fields of catalysts, electrocatalysts, and fillers, and their applicability can be greatly enhanced by interlayer organic modifications. In contrast to general organic modification based on noncovalent modification using ionic organic species, this study has clarified in situ interlayer covalent modification of LDH nanoparticles (LDHNPs) with the tripodal ligand tris(hydroxymethyl)aminomethane (Tris-NH2). Interlayer-modified CoAl LDHNPs were obtained by a one-pot hydrothermal treatment of an aqueous solution containing metal salts and Tris-NH2 at 180 °C for 24 h. Tris-NH2 was covalently bonded on the interlayer surface of LDHNPs. Interlayer-modified NiAl LDHNPs were also similarly synthesized. Some comparative experiments under different conditions indicate that the important parameters for interlayer modification are the number of bonding sites per a modifier, the electronegativity of a constituent divalent metal element, and the concentration of a modifier; this is because these parameters affect the hydrolytic stability of alkoxy-metal bonds between a modifier and a layer of LDHNPs. The synthesis of interlayer-modified MgAl LDHNPs was achieved by adjusting these parameters. This achievement will enable new potential applications because modification of only the outer surface has been achieved until now. Interlayer-modified LDHNPs possessing CO32- in the interlayer space were delaminated into monolayers under ultrasonication in water. The proposed method provides a rational approach for interlayer modification and facile delamination of LDHNPs.
中文翻译：
在外表面和中间层表面上使用三脚架配体对层状双氢氧化物纳米粒子进行选择性共价改性。
层状双氢氧化物（LDHs）在催化剂，电催化剂和填料领域中占有重要地位，并且可以通过层间有机改性大大提高其适用性。与基于使用离子有机物进行非共价修饰的一般有机修饰相反，本研究阐明了使用三脚架配体三（羟甲基）氨基甲烷（Tris-NH2）对LDH纳米颗粒（LDHNPs）进行原位层间共价修饰。通过在180°C下对包含金属盐和Tris-NH2的水溶液进行一锅水热处理，获得层间修饰的CoAl LDHNP。Tris-NH2共价键合在LDHNPs的层间表面上。还类似地合成了层间修饰的NiAl LDHNP。在不同条件下的一些对比实验表明，层间改性的重要参数是每个改性剂的键合位点数，组成的二价金属元素的电负性和改性剂的浓度。这是因为这些参数影响改性剂和LDHNPs层之间烷氧基-金属键的水解稳定性。通过调整这些参数可以实现层间修饰的MgAl LDHNP的合成。迄今为止，由于仅对外表面进行了修改，因此该成就将使新的潜在应用成为可能。在水中超声作用下，将在层间空间中具有CO32-的层间修饰LDHNPs分层为单层。
更新日期：2020-03-18
中文翻译：
在外表面和中间层表面上使用三脚架配体对层状双氢氧化物纳米粒子进行选择性共价改性。
层状双氢氧化物（LDHs）在催化剂，电催化剂和填料领域中占有重要地位，并且可以通过层间有机改性大大提高其适用性。与基于使用离子有机物进行非共价修饰的一般有机修饰相反，本研究阐明了使用三脚架配体三（羟甲基）氨基甲烷（Tris-NH2）对LDH纳米颗粒（LDHNPs）进行原位层间共价修饰。通过在180°C下对包含金属盐和Tris-NH2的水溶液进行一锅水热处理，获得层间修饰的CoAl LDHNP。Tris-NH2共价键合在LDHNPs的层间表面上。还类似地合成了层间修饰的NiAl LDHNP。在不同条件下的一些对比实验表明，层间改性的重要参数是每个改性剂的键合位点数，组成的二价金属元素的电负性和改性剂的浓度。这是因为这些参数影响改性剂和LDHNPs层之间烷氧基-金属键的水解稳定性。通过调整这些参数可以实现层间修饰的MgAl LDHNP的合成。迄今为止，由于仅对外表面进行了修改，因此该成就将使新的潜在应用成为可能。在水中超声作用下，将在层间空间中具有CO32-的层间修饰LDHNPs分层为单层。
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