Broadband Dielectric Spectroscopic Detection of Aliphatic Alcohol Vapors with Surface-Mounted HKUST-1 MOFs as Sensing Media †
Abstract
:1. Introduction
Broadband Dielectric Spectroscopy (BDS) Background
2. Experimental
2.1. Preparation of the TCNQ Doped HKUST-1 MOF Sensing Material Preparation
2.2. BDS Setup and Measurements
3. Results and Discussion
3.1. Characterization of the HKUST-1 SURMOF Sensing Material
3.2. Aliphatic Alcohol Oxidation in TCNQ-Loaded HKUST-1 MOF
3.3. Proposed Mechanism for BDS Detection of Aliphatic Alcohols in HKUST-1 MOF
- Analyte molecules diffuse into accessible cavities to interact with the open Cu2+ active sites, some of which exist as Cu2+-Cu+-O2 defects, in the SURMOF. These defects appear to be responsible for many of the electronic properties of the SURMOF films [11,30]. The introduction of the analyte molecules also induces distortion of the mechanical structure, as well as changes in the electronic band structure that lead to changes in the conductivity of the MOF. In a pure nitrogen ambient, the N2 adsorbs on the metal sites [53], but in the presence of Lewis base molecules, such as aliphatic alcohols, the analyte is expected to displace pre-adsorbed N2 molecules to form adducts from the open metal sites.
- The aliphatic alcohol probably associates with the binuclear copper-oxo defects [30], or coordinates to the open metal center, via the hydroxyl-oxygen atom. The confined alcohol analyte is aerobically oxidized by the Cu sites [54] into carbonyl compounds (e.g., aldehydes from the primary) at room temperature [55], with electrons transferred into the MOF from the alcohol. This step is dependent on the presence of oxygen in the ambient conditions within the reactor, which is required for the reoxidation of the Cu(I) to Cu(II). The oxidative abilities HKUST-1 MOF are attributable to the presence of mixed-valent-Cu-oxo defects [31], which behave like aerobic functions such as in respiration [56]. These mixed valent Cu-oxo centers in the defective MOF are critical for the spontaneous oxidation of alcohols in aerobic conditions [4,57,58].
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Solvent | Dielectric Constant | Dipole Moment | Acceptor Number | Oxidation Potential (V/SHE) [45] | ΔG (kJmol−1) | Lower Detection Limit (mL) | Upper Linear Limit (mL) | Slope (dB/mL) |
---|---|---|---|---|---|---|---|---|
Methanol | 32.7 | 1.7 | 41.5 | 0.016 | −9.3 | 0.1 | 0.5 | −11.228 |
Ethanol | 24.5 | 1.69 | 37.9 | 0.084 | −97.3 | 0.2 | 0.5 | −8.160 |
2-Propanol | 18 | 1.66 | 33.5 | 0.097 | −168 | 0.3 | 0.5 | −6.083 |
Acetone | 20.7 | 2.85 | 12.5 | −0.879 | 0.2 | 0.5 | −2.440 |
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Amoah, P.K.; Hassan, Z.M.; Franklin, R.R.; Baumgart, H.; Redel, E.; Obeng, Y.S. Broadband Dielectric Spectroscopic Detection of Aliphatic Alcohol Vapors with Surface-Mounted HKUST-1 MOFs as Sensing Media. Chemosensors 2022, 10, 408. https://0-doi-org.brum.beds.ac.uk/10.3390/chemosensors10100408
Amoah PK, Hassan ZM, Franklin RR, Baumgart H, Redel E, Obeng YS. Broadband Dielectric Spectroscopic Detection of Aliphatic Alcohol Vapors with Surface-Mounted HKUST-1 MOFs as Sensing Media. Chemosensors. 2022; 10(10):408. https://0-doi-org.brum.beds.ac.uk/10.3390/chemosensors10100408
Chicago/Turabian StyleAmoah, Papa K., Zeinab Mohammed Hassan, Rhonda R. Franklin, Helmut Baumgart, Engelbert Redel, and Yaw S. Obeng. 2022. "Broadband Dielectric Spectroscopic Detection of Aliphatic Alcohol Vapors with Surface-Mounted HKUST-1 MOFs as Sensing Media" Chemosensors 10, no. 10: 408. https://0-doi-org.brum.beds.ac.uk/10.3390/chemosensors10100408