April 2025
·
6 Reads
Water Research
This page lists works of an author who doesn't have a ResearchGate profile or hasn't added the works to their profile yet. It is automatically generated from public (personal) data to further our legitimate goal of comprehensive and accurate scientific recordkeeping. If you are this author and want this page removed, please let us know.
April 2025
·
6 Reads
Water Research
March 2025
·
4 Reads
Journal of the American Chemical Society
March 2025
·
17 Reads
The reduction of carbon dioxide (CO₂) into valuable products will contribute to sustainable carbon use. Here we report the photocatalytic reduction of CO₂ to carbon monoxide, formate, and oxalate ions using a redox‐active phenazine‐based 2D covalent organic framework (Phen‐COF) and its phenazine monomer. Under similar irradiation conditions, Phen‐COF produced 2.9 times more CO, 11 times more formate, and 13 times more oxalate compared to equimolar amounts of the monomeric phenazine, demonstrating that the COF architecture enhances catalytic performance (TOFCOF: 10⁻⁷ s⁻¹ CO, 10⁻⁸ s⁻¹ formate, and 10⁻¹¹ s⁻¹ oxalate). Structural analysis, including X‐ray diffraction and N₂ porosimetry, confirmed the COF's long‐range order and porosity. Mechanistic studies suggest a sequential formate‐to‐oxalate pathway, with CO and formate acting as intermediates. These results demonstrate the potential of the COF architecture to improve the performance of metal‐free, redox‐active aromatic systems such as phenazines to facilitate efficient and selective CO₂ conversion under mild conditions.
March 2025
·
5 Reads
Macromolecules
March 2025
·
7 Reads
Angewandte Chemie
The reduction of carbon dioxide (CO2) into valuable products will contribute to sustainable carbon use. Here we report the photocatalytic reduction of CO2 to carbon monoxide, formate, and oxalate ions using a redox‐active phenazine‐based two‐dimensional covalent organic framework (Phen‐COF) and its phenazine monomer. Under similar irradiation conditions, Phen‐COF produced 2.9 times more CO, 11 times more formate and 13 times more oxalate compared to equimolar amounts of the monomeric phenazine, demonstrating that the COF architecture enhances catalytic performance (TOFCOF: 10‐7 s‐1 CO, 10‐8 s‐1 formate, 10‐11 s‐1 oxalate). Structural analysis, including X‐ray diffraction and N2 porosimetry, confirmed the COF’s long‐range order and porosity. Mechanistic studies suggest a sequential formate‐to‐oxalate pathway, with CO and formate acting as intermediates. These results demonstrate the potential of the COF architecture to improve the performance of metal‐free, redox‐active aromatic systems such as phenazines to facilitate efficient and selective CO2 conversion under mild conditions.
March 2025
·
32 Reads
Chemical Engineering Journal
January 2025
·
118 Reads
·
2 Citations
Science
Mechanical bonds arise between molecules that contain interlocked subunits, such as one macrocycle threaded through another. Within polymers, these linkages will confer distinctive mechanical properties and other emergent behaviors, but polymerizations that form mechanical bonds efficiently and use simple monomeric building blocks are rare. In this work, we introduce a solid-state polymerization in which one monomer infiltrates crystals of another to form a macrocycle and mechanical bond at each repeat unit of a two-dimensional (2D) polymer. This mechanically interlocked 2D polymer is formed as a layered solid that is readily exfoliated in common organic solvents, enabling spectroscopic characterization and atomic-resolution imaging using advanced electron microscopy techniques. The 2D mechanically interlocked polymer is easily prepared on multigram scales, which, along with its solution processibility, enables the facile fabrication of composite fibers with Ultem that exhibit enhanced stiffness and strength.
October 2024
·
11 Reads
·
4 Citations
ACS Applied Materials & Interfaces
October 2024
·
12 Reads
·
4 Citations
Journal of the American Chemical Society
July 2024
·
20 Reads
·
2 Citations
Chemical Engineering Journal
... Catenanes (i.e., from the latin word catena, which means chain) are chainlike molecules mechanically interlocked where the molecules forming the chain are interlocked by mechanical bonds [21][22][23] instead of covalent bonds. Therefore, are classified as MIMs 24,25 . To separate one of the mechanically interlocked components, it is necessary to cleave a chemical bond; thus, the whole interlocked structure can be considered a molecule 26 . ...
January 2025
Science
... This state of play requires immediate action, including the development of PFAS removal approaches [2][3][4] and responsible management of PFAS-contaminated waste streams 8,9 . The PFAS degradation methods reported to date include chemical-and photochemical-initiated oxidation and reduction processes [10][11][12][13] , mechanical [14][15][16][17][18][19][20][21][22][23][24] and base-assisted destruction, including low-temperature mineralization 25,26 , and incineration 27 among other techniques 28,29 (Fig. 1a). ...
June 2024
Journal of the American Chemical Society
... Therefore, there is a need for new sustainable and cost-efficient treatment processes. Previous research on adsorption-based methods has focused on GAC filtration [14][15][16], biochar [17,18], cyclodextrin-based adsorbents, amorphous aluminium hydroxide, (organo)clays [17,[19][20][21], styrenic β-cyclodextrin polymers [22], and polymeric anion exchange resins (AERs) [23,24]. AERs are particularly promising due to their established use in treating other common water contaminants such as sulphate, chromate, nitrate, chloride, and perchlorate [14], as well as due to their demonstrated effectiveness to treat PFASs for groundwater remediation [24,25]. ...
June 2024
Water Research
... [8,12] On the other hand, a deeper understanding of the crystallization mechanism of COFs could significantly address the challenges associated with crystal growth, thereby circumventing the traditional, labor-intensive process of empirical synthesis and screening. [13] However, a systematic investigation into the driving forces, kinetics, and mechanisms underlying the growth of single-crystal COFs has yet to be reported. ...
June 2024
Journal of the American Chemical Society
... Adsorbents incorporated by alginate (alg.) and cyclodextrin (β-CD) polymers, including hydrogels and IERs have recently been utilized to remove PFAS [67][68][69][70][71]. The cyclodextrin polymers outperform activated carbon for the removal of PFAS under real groundwater matrices [28]. ...
May 2024
ACS Applied Materials & Interfaces
... This synthesis is achieved through the copolymerization of [2-(methacryloyloxy)ethyl] trimethylammonium chloride (MATMA) solution and StyDex (Figures 18a and b). [96] Batch adsorption experiments indicate that this polymer selectively adsorbs contaminants, successfully removing sixout of 13 tested pollutants and demonstrating reduced adsorption inhibition in wastewater compared to granular AC. It reaches equilibrium removal within one hour for PFOA, perfluorohexanoic acid (PFHxA), PFHxS, and DCF, with observed rate constants of 6.42, 4.48, 11.0, and 3.57 g μg À 1 h À 1 , respectively. ...
November 2023
Environmental Science and Technology
... 48 and 49). Laboratory SAXS analysis shows that the DTMP-TFT films catalyzed by acid or base exhibit a similar degree of crystallinity ( Supplementary Fig. 50) 41,42 . The weakened crystallinity of 2DCP thin film and powder probably originates from the fact that the long alkyl chain affects the stacking and crystallizing process (Supplementary Fig. 51). ...
September 2023
Journal of the American Chemical Society
... Additionally, DCC enables the creation of foams that are easier to recycle, reducing the environmental impact of foam waste and increasing the lifetime of foam-based products. 16,21,22 3D printing offers a way to create polymer objects with simple or complex structures. 23,24 With 3D printing, foam architectures not possible by traditional manufacturing can be achieved, creating foams with better resolutions and complex shapes. ...
August 2023
Macromolecules
... Porphyrins are ubiquitous in biology and chemistry and play crucial roles in, for example, oxygen transport and storage in blood, charge transfer in cellular respiration, and photosynthesis in plants. 1,2 Their synthetic tunability 3 make porphyrins ideal in advancing bioinspired charge and energy transport and storage technologies, 4-7 especially as they offer a convenient chemical scaffold that can be functionalized with substituents, 8,9 paired with transition metals, 10 or wreathed together in polymer chains [11][12][13][14] to tailor and exploit their optoelectronic properties. Numerous studies have turned to sophisticated multidimensional spectroscopies to disentangle the palette of spectral features generated by porphyrin and porphyrin-like systems. ...
August 2023
Journal of the American Chemical Society
... The two bands observed between 2936 and 2860 cm −1 are attributed to symmetric and nonsymmetric stretching of the C─H bond of carbonyl groups. [21] The apparent absorption peaks at 1720 cm −1 and 1235 cm −1 are typical bands for the stretching vibrations of C═O and C─O (from ─N─CO─), respectively. [22] Notably, the peak at 1630 cm −1 is associated with the stretching vibration of C═O, which is not present in PBU, thus providing convincing evidence for the introduction of piperazine monomers. ...
September 2023