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10-08-2023 | Letter

Engineering in amino acid-functionalized double-layer heteropolymolybdates: from structural control to catalytic activity

Authors: Lu-Lu Liu, Yan-Hu Wang, Xin-Yu Xiao, Ke-Wei Tong, Yue Zhao, Chao-Qin Chen, Jing Du, Peng Yang

Published in: Rare Metals | Issue 10/2023

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摘要

本文重新审视了Kortz等人在2002年报道的氨基酸功能化的杂多钼酸盐体系。通过调控自组装过程中的结构限制因素，得到了四种有机-无机杂化型钼多酸，即双层的[(SeO₃)₂Mo₁₂O₃₆(CH₃COO)³]⁷– (1), [(SeO₃)_1.3(HPO₃)_0.7Mo₁₂O₃₆(NH₃CH₂COO)₃]⁴– (2), [(SeO₃)_1.4(HPO₃)_0.6Mo₁₂O₃₆(L-NH₃C₂H₃OHCOO)₃]⁴– (3)和单层的[(SeO₃)Mo₆O₁₈(L-NH₃C₂H₃OHCOO)₃]²– (4)，并将其分别结晶为水合铵盐(NH₄)₇[(SeO₃)₂Mo₁₂O₃₆(CH₃COO)₃]·14H₂O (NH₄-1), (NH₄)₄[(SeO₃)_1.3(HPO₃)_0.7Mo₁₂O₃₆(NH₃CH₂COO)₃]·10H₂O (NH₄-2), (NH₄)₄[(SeO₃)_1.4(HPO₃)_0.6Mo₁₂O₃₆(L-NH₃C₂H₃OHCOO)₃]·18H₂O (NH₄-3)和(NH₄)₂[(SeO₃)Mo₆O₁₈(L-NH₃C₂H₃OHCOO)₃]·9H₂O (NH₄-4)。我们首次制备并表征（如X-射线单晶衍射、红外光谱和圆二色谱）了具有十二核双层模式的杂多钼酸结构（1‒3），其具体组成可通过中心杂原子和有机配体进行精准编辑。此外，通过对NH4-1‒4的质谱研究，分析了以上杂多钼酸盐在水中的主要离子片段结构，从而有助于从根本上理解其组装-解离机制。除了因氨基酸修饰引入的手征性外，该类化合物可以显著促进肼与1,3-二酮制备吡唑类药物的缩合-环化反应，进一步拓展了其作为高效稳定的Lewis酸碱催化剂的功能与应用。

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Title: Engineering in amino acid-functionalized double-layer heteropolymolybdates: from structural control to catalytic activity
Authors: Lu-Lu Liu
Yan-Hu Wang
Xin-Yu Xiao
Ke-Wei Tong
Yue Zhao
Chao-Qin Chen
Jing Du
Peng Yang
Publication date: 10-08-2023
Publisher: Nonferrous Metals Society of China
Published in: Rare Metals / Issue 10/2023
Print ISSN: 1001-0521
Electronic ISSN: 1867-7185
DOI: https://doi.org/10.1007/s12598-023-02371-4

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