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具有可逆镧系元素结合三联吡啶中心的光活性超薄分子纳米片。

Photoactive ultrathin molecular nanosheets with reversible lanthanide binding terpyridine centers.

作者信息

Tang Zian, Chulanova Elena, Küllmer Maria, Winter Andreas, Picker Julian, Neumann Christof, Schreyer Kristin, Herrmann-Westendorf Felix, Arnlind Andreas, Dietzek Benjamin, Schubert Ulrich S, Turchanin Andrey

机构信息

Institute of Physical Chemistry (IPC), Friedrich Schiller University Jena, Lessingstr. 10, 07743 Jena, Germany.

Institute of Organic Chemistry, Siberian Branch, Russian Academy of Sciences, 630090 Novosibirsk, Russia.

出版信息

Nanoscale. 2021 Dec 16;13(48):20583-20591. doi: 10.1039/d1nr05430a.

DOI:10.1039/d1nr05430a
PMID:34874038
Abstract

In recent years, functional molecular nanosheets have attracted much attention in the fields of sensors and energy storage. Here, we present an approach for the synthesis of photoactive metal-organic nanosheets with ultimate molecular thickness. To this end, we apply low-energy electron irradiation induced cross-linking of 4'-(2,2':6',2''-terpyridine-4'-yl)-1,1'-biphenyl-4-thiol self-assembled monolayers on gold to convert them into functional ∼1 nm thick carbon nanomembranes possessing the ability to reversibly complex lanthanide ions (Ln-CNMs). The obtained Ln-CNMs can be prepared on a large-scale (>10 cm) and inherit the photoactivity of the pristine terpyridine lanthanide complex (Ln(III)-tpy). Moreover, they possess mechanical stability as free-standing sheets over micrometer sized openings. The presented methodology paves a simple and robust way for the preparation of ultrathin nanosheets with tailored photoactive properties for application in photocatalytic and energy conversion devices.

摘要

近年来,功能性分子纳米片在传感器和能量存储领域备受关注。在此,我们提出一种合成具有极限分子厚度的光活性金属有机纳米片的方法。为此,我们对金表面的4'-(2,2':6',2''-三联吡啶-4'-基)-1,1'-联苯-4-硫醇自组装单分子层施加低能电子辐照诱导交联,将其转化为具有可逆络合镧系离子能力的功能性约1纳米厚的碳纳米膜(Ln-CNMs)。所获得的Ln-CNMs可大规模(>10厘米)制备,并继承了原始三联吡啶镧系配合物(Ln(III)-tpy)的光活性。此外,它们作为独立的薄片在微米级开口上具有机械稳定性。所提出的方法为制备具有定制光活性特性的超薄纳米片用于光催化和能量转换装置铺平了一条简单而稳健的道路。

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