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Fast-Switching Vis-IR Electrochromic Covalent Organic Frameworks.

ABSTRACT: Electrochromic coatings are promising for applications in smart windows or energy-efficient optical displays. However, classical inorganic electrochromic materials such as WO₃ suffer from low coloration efficiency and slow switching speed. We have developed highly efficient and fast-switching electrochromic thin films based on fully organic, porous covalent organic frameworks (COFs). The low band gap COFs have strong vis-NIR absorption bands in the neutral state, which shift significantly upon electrochemical oxidation. Fully reversible absorption changes by close to 3 OD can be triggered at low operating voltages and low charge per unit area. Our champion material reaches an electrochromic coloration efficiency of 858 cm² C^-1 at 880 nm and retains >95% of its electrochromic response over 100 oxidation/reduction cycles. Furthermore, the electrochromic switching is extremely fast with response times below 0.4 s for the oxidation and around 0.2 s for the reduction, outperforming previous COFs by at least an order of magnitude and rendering these materials some of the fastest-switching frameworks to date. This combination of high coloration efficiency and very fast switching reveals intriguing opportunities for applications of porous organic electrochromic materials.

SUBMITTER: Bessinger D

PROVIDER: S-EPMC8154512 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Redox-triggered switching in three-dimensional covalent organic frameworks.

Project description:The tuning of molecular switches in solid state toward stimuli-responsive materials has attracted more and more attention in recent years. Herein, we report a switchable three-dimensional covalent organic framework (3D COF), which can undergo a reversible transformation through a hydroquinone/quinone redox reaction while retaining the crystallinity and porosity. Our results clearly show that the switching process gradually happened through the COF framework, with an almost quantitative conversion yield. In addition, the redox-triggered transformation will form different functional groups on the pore surface and modify the shape of pore channel, which can result in tunable gas separation property. This study strongly demonstrates 3D COFs can provide robust platforms for efficient tuning of molecular switches in solid state. More importantly, switching of these moieties in 3D COFs can remarkably modify the internal pore environment, which will thus enable the resulting materials with interesting stimuli-responsive properties.

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Ultra-fast single-crystal polymerization of large-sized covalent organic frameworks.

Project description:In principle, polymerization tends to produce amorphous or poorly crystalline materials. Efficiently producing high-quality single crystals by polymerization in solvent remains as an unsolved issue in chemistry, especially for covalent organic frameworks (COFs) with highly complex structures. To produce μm-sized single crystals, the growth time is prolonged to >15 days, far away from the requirements in practical applications. Here, we find supercritical CO2 (sc-CO2) accelerates single-crystal polymerization by 10,000,000 folds, and produces two-dimensional (2D) COF single crystals with size up to 0.2 mm within 2~5 min. Although it is the fastest single-crystal polymerization, the growth in sc-CO2 leads to not only the largest crystal size of 2D COFs, but also higher quality with improved photoconductivity performance. This work overcomes traditional concept on low efficiency of single-crystal polymerization, and holds great promise for future applications owing to its efficiency, industrial compatibility, environmental friendliness and universality for different crystalline structures and linkage bonds.

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Colloidal Covalent Organic Frameworks.

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| S-EPMC4974470 | biostudies-literature

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Project description:The discovery of tertiary lymphoid structures (TLS) within the tumor tissues provides a promising avenue to promote the response rate of cancer immunotherapy. Yet, the lack of effective strategies to promote TLS formation poses a substantial obstacle. Thus, the exploration of potential inducers for TLS formation is of great interest but remains challenging. Here, inspired by the mechanism of artificially cultivated pearls, a covalent organic frameworks (COFs) was employed to promote the formation of TLS. Single-cell sequencing analysis revealed that this was achieved by promoting the cytokine hypersecretion to facilitate the maturation, proliferation, and migration of T and B cells, critical for trigger TLS formation. Furthermore, the high efficacy of COF-mediated phototherapy in inducing TLS formation was validated in both the MC38 and 4MOSC1 tumor models. Moreover, an efficient synergism between COF-mediated phototherapy and αCTLA-4 was observed, which was able to effectively eradicate both primary and distant tumors, and inhibit tumor recurrence. This study underscores a new approach of boosting cancer immunotherapy through COF triggered TLS formation.

2024-10-31 | GSE268619 | GEO

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Project description:With vibrant colours and simple, room-temperature processing methods, electrochromic polymers have attracted attention as active materials for flexible, low-power-consuming devices. However, slow switching speeds in devices realized to date, as well as the complexity of having to combine several distinct polymers to achieve a full-colour gamut, have limited electrochromic materials to niche applications. Here we achieve fast, high-contrast electrochromic switching by significantly enhancing the interaction of light--propagating as deep-subwavelength-confined surface plasmon polaritons through arrays of metallic nanoslits, with an electrochromic polymer--present as an ultra-thin coating on the slit sidewalls. The switchable configuration retains the short temporal charge-diffusion characteristics of thin electrochromic films, while maintaining the high optical contrast associated with thicker electrochromic coatings. We further demonstrate that by controlling the pitch of the nanoslit arrays, it is possible to achieve a full-colour response with high contrast and fast switching speeds, while relying on just one electrochromic polymer.

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Project description:Two-dimensional covalent organic frameworks (2D-COFs) are crystalline, porous materials comprising aligned columns of π-stacked building blocks. With a view toward the application of these materials in organic electronics and optoelectronics, the construction of oligothiophene-based COFs would be highly desirable. The realization of such materials, however, has remained a challenge, in particular with respect to laterally conjugated imine-linked COFs. We have developed a new building block design employing an asymmetric modification on an otherwise symmetric backbone that allows us to construct a series of highly crystalline quaterthiophene-derived COFs with tunable electronic properties. Studying the optical response of these materials, we have observed for the first time the formation of a charge transfer state between the COF subunits across the imine bond. We believe that our new building block design provides a general strategy for the construction of well-ordered COFs from various extended building blocks, thus greatly expanding the range of applicable molecules.

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