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Charge Transport and Carrier Polarity Tuning by Electrolyte Gating in Nickel Benzenehexathiol Coordination Nanosheets
Advanced Materials ( IF 27.4 ) Pub Date : 2025-06-04 , DOI: 10.1002/adma.202500164
Tian Wu, Xinglong Ren, Zhengkang Qu, Ian E. Jacobs, Lu Zhang, Naoya Fukui, Xin Chen, Hiroshi Nishihara, Henning Sirringhaus

Coordination nanosheets (CONASHs) or conjugated metal organic frameworks (MOFs) with distinctive metal-organic bonding structures exhibit promise for electronics, sensing, and energy storage. Porous Nickel-Benzene hexathiol complex (Ni-BHT) with noteworthy conductivity was first reported a decade ago, and recent synthetic modifications produced non-porous Ni-BHT with enhanced conductivity (≈50 S cm−1). Here the charge transport physics of such non-porous Ni-BHT films are studied with even higher conductivity (≈112 S cm−1). In contrast to the thermally activated electrical conductivity, thermoelectric measurements suggest an intrinsic metallic nature of Ni-BHT. It is shown that it is possible to tune the Fermi level and carrier polarity in Ni-BHT by electrolyte gating; gating is initially governed by the formation of an interfacial, electric double layer and then evolves into an electrochemical (de)doping process. These findings not only contribute to a deeper understanding of charge transport in CONASHs, but also show that Fermi level tuning is an effective approach for enhancing the thermoelectric performance of CONASHs.

中文翻译:

镍苯六硫醇配位纳米片中电解质门控的电荷传输和载流子极性调节

具有独特金属有机键合结构的配位纳米片 (CONASH) 或共轭金属有机框架 (MOF) 在电子学、传感和储能方面前景广阔。具有显着导电性的多孔镍-苯六硫醇络合物 (Ni-BHT) 在十年前首次被报道,最近的合成改性产生了具有增强导电性 (≈50 S cm-1) 的无孔 Ni-BHT。在这里,以更高的电导率 (≈112 S cm-1) 研究了这种无孔 Ni-BHT 薄膜的电荷传输物理学。与热激活电导率相反,热电测量表明 Ni-BHT 具有固有的金属性质。结果表明,可以通过电解质门控来调节 Ni-BHT 中的费米能级和载流子极性;选通最初由表面双电层的形成控制,然后演变为电化学(去)掺杂过程。这些发现不仅有助于更深入地理解 CONASH 中的电荷传输,而且还表明费米能级调谐是增强 CONASH 热电性能的有效方法。
更新日期:2025-06-04
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