Jeon Mingyu, Lee Joon-Seok, Kim Minhyuk, Seo Jae-Woo, Kim Honghui, Moon Hoi Ri, Choi Seon-Jin, Kim Jihan
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
Division of Materials of Science and Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul 04763, Republic of Korea.
ACS Appl Mater Interfaces. 2024 Nov 13;16(45):62382-62391. doi: 10.1021/acsami.4c13269. Epub 2024 Oct 30.
Two-dimensional conductive metal-organic frameworks (2D cMOFs) stand at the forefront of chemiresistive sensing innovations due to their high surface areas, distinctive morphologies, and substantial electronic conductivity. Particularly, 2D cMOFs crafted using 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and 2,3,6,7,10,11-hexaiminotriphenylene (HITP) organic ligands have garnered a large amount of attention due to their designable active sites and proper conductive characteristics. Nevertheless, a deeper exploration into their sensing mechanisms is imperative for a comprehensive understanding of the intrinsic chemistry, which is crucial for the intricate design of specialized 2D cMOF chemiresistive sensors. In this study, we fabricate six M-HXTP (M = Co, Ni, and Cu; X = H and I) chemiresistive sensors, focusing on the application of hydrogen sulfide (HS) detection. Among these, the 2D cMOFs incorporating Cu metal manifested a remarkably enhanced response to HS. A combination of experimental and computational studies unveils the mechanisms of sulfur oxidation and Cu reduction, wherein distortion of the reduced MX cluster markedly amplifies the sensing response. Lastly, a real-time and portable wireless HS sensing module has been demonstrated by using the Cu-HHTP composite material, highlighting the substantial practical significance and potential applicability.
二维导电金属有机框架（2D cMOF）因其高表面积、独特形态和显著的电子导电性，在化学电阻传感创新领域处于前沿地位。特别是，使用2,3,6,7,10,11-六羟基三亚苯（HHTP）和2,3,6,7,10,11-六亚氨基三亚苯（HITP）有机配体制备的2D cMOF，因其可设计的活性位点和适当的导电特性而备受关注。然而，深入探究其传感机制对于全面理解其内在化学性质至关重要，这对于专门的2D cMOF化学电阻传感器的精细设计至关重要。在本研究中，我们制备了六种M-HXTP（M = Co、Ni和Cu；X = H和I）化学电阻传感器，重点关注硫化氢（HS）检测的应用。其中，含铜金属的2D cMOF对HS表现出显著增强的响应。实验和计算研究相结合揭示了硫氧化和铜还原的机制，其中还原的MX簇的畸变显著放大了传感响应。最后，通过使用Cu-HHTP复合材料展示了一种实时、便携式无线HS传感模块，突出了其重大的实际意义和潜在适用性。
