Multi-component self-assembled molecular-electronic films: towards new high-performance thermoelectric systems.
Multi-component self-assembled molecular-electronic films: towards new high-performance thermoelectric systems.
复制标题
DOI：
10.1039/d2sc00078d
复制
发表时间：
2022-05-11
期刊：
影响因子：
8.4
通讯作者：
中科院分区：
文献类型：
--
作者：
有机分子在表面平行排列的热电性能为大面积、柔性、溶液处理、能量收集的薄膜提供了可能性，其室温传输特性由量子干涉(QI)控制。最近的研究表明，构造性QI(CQI)可以从单分子转变为自组装单分子膜(SAM)，从而提高电导率和Seebeck系数。然而，这些CQI增强系统受到组件分子与金属电极的刚性耦合的限制，阻止了有利于其进一步发展的额外层的引入。这些刚性耦合也限制了我们抑制声子通过这些系统的传输的能力，这些系统可以提高它们的热电输出，而不是利用它们令人印象深刻的电子特性。在这里，通过实验和理论相结合的研究，我们证明了通过引入额外的分子层可以增强自组装膜中的跨平面热电性。我们利用自下而上的方法组装多组分薄膜，这种薄膜结合了由炔基功能化的菲形成的刚性、高导电性的粘性连接体，以及由功能化的金属卟啉组成的滑性连接体。从一种基于蒽的SAM出发，我们证明了随后加入一层卟啉或一层石墨烯都会增加Seebeck系数，而这两种化合物的加入都会进一步提高它们的Seebeck系数。此次展示的塞贝克增强型多组分自组装膜是此类材料中的第一个，并为薄膜热电材料的设计提供了一种新的策略。通过实验和理论研究，通过引入额外的分子层来提高自组装单分子膜的跨平面热电性，为高温差电材料的设计提供了一种新的策略。
The thermoelectric properties of parallel arrays of organic molecules on a surface offer the potential for large-area, flexible, solution processed, energy harvesting thin-films, whose room-temperature transport properties are controlled by quantum interference (QI). Recently, it has been demonstrated that constructive QI (CQI) can be translated from single molecules to self-assembled monolayers (SAMs), boosting both electrical conductivities and Seebeck coefficients. However, these CQI-enhanced systems are limited by rigid coupling of the component molecules to metallic electrodes, preventing the introduction of additional layers which would be advantageous for their further development. These rigid couplings also limit our ability to suppress the transport of phonons through these systems, which could act to boost their thermoelectric output, without comprising on their impressive electronic features. Here, through a combined experimental and theoretical study, we show that cross-plane thermoelectricity in SAMs can be enhanced by incorporating extra molecular layers. We utilize a bottom-up approach to assemble multi-component thin-films that combine a rigid, highly conductive ‘sticky’-linker, formed from alkynyl-functionalised anthracenes, and a ‘slippery’-linker consisting of a functionalized metalloporphyrin. Starting from an anthracene-based SAM, we demonstrate that subsequent addition of either a porphyrin layer or a graphene layer increases the Seebeck coefficient, and addition of both porphyrin and graphene leads to a further boost in their Seebeck coefficients. This demonstration of Seebeck-enhanced multi-component SAMs is the first of its kind and presents a new strategy towards the design of thin-film thermoelectric materials. Through an experimental and theoretical study, cross-plane thermoelectricity in Self-Assembled Monolayers (SAMs) was enhanced by adding extra molecular layers, presenting a new strategy towards the design of high thermoelectric materials.
登录
查看更多内容
影响因子：
16.6
作者：
Ismael, Ali Khalid;Wang, Kun;Higgins, Simon J.
通讯作者：
Higgins, Simon J.
影响因子：
3.9
作者：
Castner, DG;Hinds, K;Grainger, DW
通讯作者：
Grainger, DW
影响因子：
6.7
作者：
Grace, Iain M.;Olsen, Gunnar;Lambert, Colin J.
通讯作者：
Lambert, Colin J.
影响因子：
4.6
作者：
Ikbal, Sk Asif;Brahma, Sanfaori;Rath, Sankar Prasad
通讯作者：
Rath, Sankar Prasad
影响因子：
4.6
作者：
Gantenbein M;Wang L;Al-Jobory AA;Ismael AK;Lambert CJ;Hong W;Bryce MR
通讯作者：
Bryce MR