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Detecting CO in complex gas mixtures is challenging due to the presence of competitive gases in the ambient atmosphere. Photoelectrochemical (PEC) techniques offer a solution, but material selection and specificity remain limiting. Here, we constructed a hydrogen-bonded organic framework material based on a porphyrin tecton decorated with diaminotriazine (DAT) moieties. The DAT moieties on the porphyrin molecules not only facilitate the formation of complementary hydrogen bonds between the tectons but also function as recognition sites in the resulting porous HOF materials for the selective adsorption of CO . In addition, the in-plane growth of FDU-HOF-2 into anisotropic molecular sheets with large areas of up to 23000 μm and controllable thickness between 0.298 and 2.407 μm were realized in yields of over 89 % by a simple solution-processing method. The FDU-HOF-2 can be directly grown and deposited onto different substrates including silica, carbon, and metal oxides by self-assembly in situ in formic acid. As a proof of concept, a screen-printing electrode deposited with FDU-HOF-2 was fabricate as a label-free photoelectrochemical (PEC) sensor for CO detection. Such a signal-off PEC sensor exhibits low detection limit for CO (2.3 ppm), reusability (at least 30 cycles), and long-term working stability (at least 30 days).
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http://dx.doi.org/10.1002/anie.202311482 | DOI Listing |
Chem Commun (Camb)
December 2024
School of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China.
Using temperature modulation, two distinct hydrogen bond organic frameworks HOF-C and HOF-K with different pore sizes were synthesized from the same ligands, tris(4-(4-1,2,4-triazole-4-yl)phenyl)amine. The pore size difference prevents TRZ from entering HOF-K, while allowing TRZ to selectively insert into the larger-pored HOF-C to form HOF-C-TRZ. The donor-acceptor (D-A) structure formed in HOF-C-TRZ enhances its photoelectric response and exhibits exceptional uranium reduction under visible light irradiation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Institute of Organic Chemistry and Biochemistry, Computational Chemistry, Flemingovo nam. 2, 16610, Prague 6, CZECHIA.
The binding free energy of hydrogen-bonded complexes is generally inversely proportional to the solvent dielectric constant. This occurs because the solvent-accessible surface area of the complex is always smaller than that of the individual subsystems, leading to a reduction in solvation energy. The present study explores the potential for stabilizing hydrogen-bonded complexes in a solvent with higher polarity.
View Article and Find Full Text PDFTalanta
December 2024
State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science & Engineering, Shanghai Institute of Pollution Control and Ecological Security, Tongji University, 1239 Siping Road, Shanghai, 200092, China. Electronic address:
The excessive presence of the metal ions Cu and Fe in the environment poses a serious threat to ecosystems and human health, so timely and accurate detection of them has become essential and urgent. In this paper, a novel hydrogel-based fluorescent sensor, named ME-IPA@SA-TbZn, was fabricated facilely through an in-situ cross-linking modification method and was used for the detection of Cu and Fe in water bodies. The ME-IPA@SA-TbZn is essentially a hybrid hydrogel bead that exhibits vibrant fluorescence, employing Tb and Zn functionalized hydrogen-bonded organic frameworks (HOFs) as the fluorescence functional core and sodium alginate (SA) as the hydrogel matrix.
View Article and Find Full Text PDFLangmuir
December 2024
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, People's Republic of China.
A coarse-grained model combining the acceptor-hydrogen-donor 3-body potential is first developed in this work to explore the fracture property and microscopic mechanisms of associative hydrogen-bonded polymers (AHBPs). Next, a triaxial deformation mode is performed to reveal that the fracture toughness of AHBPs initially improves and then is reduced as the number of active groups increases. By characterizing the stress decomposition, the strong hydrogen bond (HB) network improves the maximum stress but reduces the elongation.
View Article and Find Full Text PDFOrganic-crystal-based optical terahertz (THz) sources and detectors are powerful tools for THz spectroscopy, owing to the wide frequency tunability. A drawback of this technique lies in the inherent absorption peaks of nonlinear crystals, leaving several gaps in the spectral coverage. As an alternative type of organic crystal, hydrogen-bonded OH1 is promising to complement the existing gaps.
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