| 1. |
- Liu, Yuzhong, et al.
(författare)
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Weaving of organic threads into a crystalline covalent organic framework
- 2016
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 351:6271, s. 365-369
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Tidskriftsartikel (refereegranskat)abstract
- A three-dimensional covalent organic framework (COF-505) constructed from helical organic threads, designed to be mutually weaving at regular intervals, has been synthesized by imine condensation reactions of aldehyde functionalized copper(I)-bisphenanthroline tetrafluoroborate, Cu(PDB)2(BF4), and benzidine (BZ). The copper centers are topologically independent of the weaving within the COF structure and serve as templates for bringing the threads into a woven pattern rather than the more commonly observed parallel arrangement. The copper(I) ions can be reversibly removed and added without loss of the COF structure, for which a tenfold increase in elasticity accompanies its demetalation. The threads in COF-505 have many degrees of freedom for enormous deviations to take place between them, throughout the material, without undoing the weaving of the overall structure.
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| 2. |
- Chai, Gaoda, et al.
(författare)
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Deciphering the Role of Chalcogen-Containing Heterocycles in Nonfullerene Acceptors for Organic Solar Cells
- 2020
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Ingår i: ACS Energy Letters. - : AMER CHEMICAL SOC. - 2380-8195. ; 5:11, s. 3415-3425
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Tidskriftsartikel (refereegranskat)abstract
- The field of organic solar cells has experienced paradigm-shifting changes in recent years because of the emergence of nonfullerene acceptors (NFAs). It is critically important to gain more insight into the structure-property relationship of the emerging A-DAD-A-type NFAs. In this Letter, a family of NFAs named BPF-4F, BPT-4F, and BPS-4F incorporating various chalcogen-containing heterocycles, i.e., furan, thiophene, and selenophene, respectively, was designed and synthesized. These NFAs exhibited dramatic differences in their photovoltaic performances with device efficiencies of 16.8% achieved by the thiophene-based cells, which was much higher than the furan-based ones (12.6%). In addition, the selenophene-based NFA showed a red-shifted absorption relative to the furan- and thiophene-based ones and obtained a decent efficiency of 16.3% owing to an improved J(SC). The reasons why these NFAs performed differently are systematically studied by comparing their optoelectronic properties and film morphology, which provides new understandings of the molecular design of high-performance NFAs.
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| 3. |
- Englund, Elias, et al.
(författare)
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Expanding Extender Substrate Selection for Unnatural Polyketide Biosynthesis by Acyltransferase Domain Exchange within a Modular Polyketide Synthase
- 2023
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 145:16, s. 8822-8832
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Tidskriftsartikel (refereegranskat)abstract
- Modular polyketide synthases (PKSs) are poly-merases that employ alpha-carboxyacyl-CoAs as extender substrates. This enzyme family contains several catalytic modules, where each module is responsible for a single round of polyketide chain extension. Although PKS modules typically use malonyl-CoA or methylmalonyl-CoA for chain elongation, many other malonyl-CoA analogues are used to diversify polyketide structures in nature. Previously, we developed a method to alter an extension substrate of a given module by exchanging an acyltransferase (AT) domain while maintaining protein folding. Here, we report in vitro polyketide biosynthesis by 13 PKSs (the wild-type PKS and 12 AT-exchanged PKSs with unusual ATs) and 14 extender substrates. Our similar to 200 in vitro reactions resulted in 13 structurally different polyketides, including several polyketides that have not been reported. In some cases, AT-exchanged PKSs produced target polyketides by >100-fold compared to the wild-type PKS. These data also indicate that most unusual AT domains do not incorporate malonyl-CoA and methylmalonyl-CoA but incorporate various rare extender substrates that are equal to in size or slightly larger than natural substrates. We developed a computational workflow to predict the approximate AT substrate range based on active site volumes to support the selection of ATs. These results greatly enhance our understanding of rare AT domains and demonstrate the benefit of using the proposed PKS engineering strategy to produce novel chemicals in vitro.
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| 4. |
- Luo, Zhenghui, et al.
(författare)
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Fine-Tuning Energy Levels via Asymmetric End Groups Enables Polymer Solar Cells with Efficiencies over 17%
- 2020
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Ingår i: Joule. - : CELL PRESS. - 2542-4351. ; 4:6, s. 1236-1247
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Tidskriftsartikel (refereegranskat)abstract
- Generally, it is important to fine-tune the energy levels of donor and acceptor materials in the field of polymer solar cell (PSCs) to achieve a minimal highest occupied molecular orbital (HOMO) energy offset, which yet is still sufficient for charge separation. Based on the high-performance small-molecule acceptor (SMA) of BTP-4F, we modified the end groups of BTP-4F from IC-2F to CPTCN-Cl. It was found that when both end groups were substituted by CPTCN-Cl, the energy level upshift was too large that caused unfavorable energetic alignment, thus poor device performance. By using the strategy of asymmetric end groups, we were able to achieve near optimal energy level match, resulting in higher open-circuit voltage (V-OC) and power conversion efficiency (PCE) compared with those given by the PM6:BTP-4F system. Our strategy can be useful and potentially applied to othermaterial systems for maximizing efficiency of non-fullerene PSCs.
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| 5. |
- Ma, Ruijie, et al.
(författare)
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Adding a Third Component with Reduced Miscibility and Higher LUMO Level Enables Efficient Ternary Organic Solar Cells
- 2020
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Ingår i: ACS Energy Letters. - : American Chemical Society (ACS). - 2380-8195. ; 5:8, s. 2711-2720
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Tidskriftsartikel (refereegranskat)abstract
- It is widely known that the miscibility between donor and acceptor is a crucial factor that affects the morphology and thus device performance of nonfullerene organic solar cells (OSCs). In this Letter, we show that incorporating a third component with lower miscibility and higher lowest unoccupied molecular orbital (LUMO) level into the state-of-the-art PM6:Y6 system can significantly enhance the performance of devices. The best results of the ternary devices are achieved by adding a small molecular acceptor named ITCPTC (similar to 5% w/w), which significantly improves the power conversion efficiency (PCE) of the host system from 16.44% to 17.42%. The higher LUMO of the third component increases the open-circuit voltage (V-oc), while the low miscibility enlarges the domains and leads to improved short-circuit current density (J(sc)) and fill factor (FF). The efficacy of this strategy is supported by using other nonfullerene third components including an asymmetric small molecule (N7IT) and a polymer acceptor (PF2-DTC), which play the same role as ITCPTC and boost the PCEs to 16.96% and 17.04%, respectively. Our approach can be potentially applied to a wide range of OSC material systems and should facilitate the development of the OSC field.
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| 6. |
- Ma, Ruijie, et al.
(författare)
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All-polymer solar cells with over 16% efficiency and enhanced stability enabled by compatible solvent and polymer additives
- 2022
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Ingår i: Aggregate. - : Wiley. - 2692-4560 .- 2766-8541. ; 3:3
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Tidskriftsartikel (refereegranskat)abstract
- Considering the robust and stable nature of the active layers, advancing the power conversion efficiency (PCE) has long been the priority for all-polymer solar cells (all-PSCs). Despite the recent surge of PCE, the photovoltaic parameters of the state-of-the-art all-PSC still lag those of the polymer:small molecule-based devices. To compete with the counterparts, judicious modulation of the morphology and thus the device electrical properties are needed. It is difficult to improve all the parameters concurrently for the all-PSCs with advanced efficiency, and one increase is typically accompanied by the drop of the other(s). In this work, with the aids of the solvent additive (1-chloronaphthalene) and the n-type polymer additive (N2200), we can fine-tune the morphology of the active layer and demonstrate a 16.04% efficient all-PSC based on the PM6:PY-IT active layer. The grazing incidence wide-angle X-ray scattering measurements show that the shape of the crystallites can be altered, and the reshaped crystallites lead to enhanced and more balanced charge transport, reduced recombination, and suppressed energy loss, which lead to concurrently improved and device efficiency and stability.
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| 7. |
- Zhan, Chunjun, 1986, et al.
(författare)
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Reprogramming methanol utilization pathways to convert Saccharomyces cerevisiae to a synthetic methylotroph
- 2023
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Ingår i: Nature Catalysis. - 2520-1158. ; 6:5, s. 435-450
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Tidskriftsartikel (refereegranskat)abstract
- Methanol, an organic one-carbon (C1) compound, represents an attractive alternative carbon source for microbial fermentation. Despite considerable advancements in methanol utilization by prokaryotes such as Escherichia coli, engineering eukaryotic model organisms such as Saccharomyces cerevisiae into synthetic methylotrophs remains challenging. Here, an engineered module circuit strategy combined with adaptive laboratory evolution was applied to engineer S. cerevisiae to use methanol as the sole carbon source. We revealed that the evolved glyoxylate-based serine pathway plays an important role in methanol-dependent growth by promoting formaldehyde assimilation. Further, we determined that the isoprenoid biosynthetic pathway was upregulated, resulting in an increased concentration of squalene and ergosterol in our evolved strain. These changes could potentially alleviate cell membrane damage in the presence of methanol. This work sets the stage for expanding the potential of exploiting S. cerevisiae as a potential organic one-carbon platform for biochemical or biofuel production. [Figure not available: see fulltext.].
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