Pursuing both structural uniformity/crystallinity and functional complexity is a long-term goal in functional materials engineering. Often, efforts to enhance one attribute may compromise the other. Herein, we report an elaborate strategy of integrating a catalytic center into a modulator, which enables the one-pot synthesis of a bifunctional metal-organic framework (MOF), Zr-TBAPy-TSA (TBAPy = 1,3,6,8-tetrakis(p-benzoic acid)pyrene; TSA = o-thiosalicylic acid). TSA serves as both a modulator for metal-organic framework (MOF) preparation and a catalytic center. Zr-TBAPy-TSA is distinguished by its highly uniform and crystalline structure, as evidenced by detailed characterizations including single-crystal X-ray diffraction. Additionally, Zr-TBAPy-TSA incorporating both photosensitizer and thiol active centers showcases superior catalytic performance in the activation of element–H bonds (elements include C, B, Si, and P). Due to its less defective structure, extra high turnover numbers of up to 14,200 and good catalyst recyclability are obtained.

中文翻译：

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用于协同催化的双功能金属-有机框架的调制剂工程


追求结构均匀性/结晶度和功能复杂性是功能材料工程的长期目标。通常，增强一种属性的努力可能会损害另一种属性。在此，我们报告了一种将催化中心集成到调制剂中的详细策略，该策略能够一锅法合成双功能金属有机框架 （MOF），Zr-TBAPy-TSA（TBAPy = 1,3,6,8-四（对苯甲酸）芘;TSA = 邻硫代水杨酸）。TSA 既是金属有机框架 （MOF） 制备的调节剂，也是催化中心。Zr-TBAPy-TSA 以其高度均匀的晶体结构而著称，包括单晶 X 射线衍射在内的详细表征证明了这一点。此外，结合光敏剂和巯基活性中心的 Zr-TBAPy-TSA 在激活元素-H 键（元素包括 C、B、Si 和 P）方面表现出卓越的催化性能。由于其结构缺陷较少，因此获得了高达 14,200 的超高周转数和良好的催化剂可回收性。