| 1. |
- Klionsky, Daniel J., et al.
(författare)
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Guidelines for the use and interpretation of assays for monitoring autophagy
- 2012
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Ingår i: Autophagy. - : Informa UK Limited. - 1554-8635 .- 1554-8627. ; 8:4, s. 445-544
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Forskningsöversikt (refereegranskat)abstract
- In 2008 we published the first set of guidelines for standardizing research in autophagy. Since then, research on this topic has continued to accelerate, and many new scientists have entered the field. Our knowledge base and relevant new technologies have also been expanding. Accordingly, it is important to update these guidelines for monitoring autophagy in different organisms. Various reviews have described the range of assays that have been used for this purpose. Nevertheless, there continues to be confusion regarding acceptable methods to measure autophagy, especially in multicellular eukaryotes. A key point that needs to be emphasized is that there is a difference between measurements that monitor the numbers or volume of autophagic elements (e.g., autophagosomes or autolysosomes) at any stage of the autophagic process vs. those that measure flux through the autophagy pathway (i.e., the complete process); thus, a block in macroautophagy that results in autophagosome accumulation needs to be differentiated from stimuli that result in increased autophagic activity, defined as increased autophagy induction coupled with increased delivery to, and degradation within, lysosomes (in most higher eukaryotes and some protists such as Dictyostelium) or the vacuole (in plants and fungi). In other words, it is especially important that investigators new to the field understand that the appearance of more autophagosomes does not necessarily equate with more autophagy. In fact, in many cases, autophagosomes accumulate because of a block in trafficking to lysosomes without a concomitant change in autophagosome biogenesis, whereas an increase in autolysosomes may reflect a reduction in degradative activity. Here, we present a set of guidelines for the selection and interpretation of methods for use by investigators who aim to examine macroautophagy and related processes, as well as for reviewers who need to provide realistic and reasonable critiques of papers that are focused on these processes. These guidelines are not meant to be a formulaic set of rules, because the appropriate assays depend in part on the question being asked and the system being used. In addition, we emphasize that no individual assay is guaranteed to be the most appropriate one in every situation, and we strongly recommend the use of multiple assays to monitor autophagy. In these guidelines, we consider these various methods of assessing autophagy and what information can, or cannot, be obtained from them. Finally, by discussing the merits and limits of particular autophagy assays, we hope to encourage technical innovation in the field.
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| 2. |
- Chen, Haiyang, et al.
(författare)
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A guest-assisted molecular-organization approach for >17% efficiency organic solar cells using environmentally friendly solvents
- 2021
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Ingår i: Nature Energy. - : NATURE PORTFOLIO. - 2058-7546. ; 6:11, s. 1045-1053
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Tidskriftsartikel (refereegranskat)abstract
- The power conversion efficiencies (PCEs) of laboratory-sized organic solar cells (OSCs), usually processed from low-boiling-point and toxic solvents, have reached high values of over 18%. However, there is usually a notable drop of the PCEs when green solvents are used, limiting practical development of OSCs. Herein, we obtain certificated PCEs over 17% in OSCs processed from a green solvent paraxylene (PX) by a guest-assisted assembly strategy, where a third component (guest) is employed to manipulate the molecular interaction of the binary blend. In addition, the high-boiling-point green solvent PX also enables us to deposit a uniform large-area module (36 cm(2)) with a high efficiency of over 14%. The strong molecular interaction between the host and guest molecules also enhances the operational stability of the devices. Our guest-assisted assembly strategy provides a unique approach to develop large-area and high-efficiency OSCs processed from green solvents, paving the way for industrial development of OSCs. Organic solar cells processed from green solvents are easier to implement in manufacturing yet their efficiency is low. Chen et al. devise a guest molecule to improve the molecular packing, enabling devices with over 17% efficiency.
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| 3. |
- Chen, Haiyang, et al.
(författare)
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Heterogeneous Nucleating Agent for High-Boiling-Point Nonhalogenated Solvent-Processed Organic Solar Cells and Modules
- 2024
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Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095.
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Tidskriftsartikel (refereegranskat)abstract
- High-boiling-point nonhalogenated solvents are superior solvents to produce large-area organic solar cells (OSCs) in industry because of their wide processing window and low toxicity; while, these solvents with slow evaporation kinetics will lead excessive aggregation of state-of-the-art small molecule acceptors (e.g. L8-BO), delivering serious efficiency losses. Here, a heterogeneous nucleating agent strategy is developed by grafting oligo (ethylene glycol) side-chains on L8-BO (BTO-BO). The formation energy of the obtained BTO-BO; while, changing from liquid in a solvent to a crystalline phase, is lower than that of L8-BO irrespective of the solvent type. When BTO-BO is added as the third component into the active layer (e.g. PM6:L8-BO), it easily assembles to form numerous seed crystals, which serve as nucleation sites to trigger heterogeneous nucleation and increase nucleation density of L8-BO through strong hydrogen bonding interactions even in high-boiling-point nonhalogenated solvents. Therefore, it can effectively suppress excessive aggregation during growth, achieving ideal phase-separation active layer with small domain sizes and high crystallinity. The resultant toluene-processed OSCs exhibit a record power conversion efficiency (PCE) of 19.42% (certificated 19.12%) with excellent operational stability. The strategy also has superior advantages in large-scale devices, showing a 15.03-cm2 module with a record PCE of 16.35% (certificated 15.97%). The heterogeneous nucleating agent (BTO-BO) is developed to suppress the excessive aggregation of L8-BO in high-boiling-point nonhalogenated solvents processing, achieving the active layer with high crystallinity and nano-scaled phase separation morphology. The resultant OSCs achieve record power conversion efficiencies of 19.42% (0.062-cm2) and 16.35% (15. 03-cm2) with excellent operational stabilities. image
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| 4. |
- Feng, Hongliang, et al.
(författare)
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Association between accelerometer-measured amplitude of rest-activity rhythm and future health risk : a prospective cohort study of the UK Biobank
- 2023
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Ingår i: The Lancet Healthy Longevity. - 2666-7568. ; 4:5, s. e200-e210
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Tidskriftsartikel (refereegranskat)abstract
- BACKGROUND: The health effects of rest-activity rhythm are of major interest to public health, but its associations with health outcomes remain elusive. We aimed to examine the associations between accelerometer-measured rest-activity rhythm amplitude and health risks among the general UK population.METHODS: We did a prospective cohort analysis of UK Biobank participants aged 43-79 years with valid wrist-worn accelerometer data. Low rest-activity rhythm amplitude was defined as the first quintile of relative amplitude; all other quintiles were classified as high rest-activity rhythm amplitude. Outcomes of interest were defined using International Classification of Diseases 10th Revision codes and consisted of incident cancer and cardiovascular, infectious, respiratory, and digestive diseases, and all-cause and disease-specific (cardiovascular, cancer, and respiratory) mortality. Participants with a current diagnosis of any outcome of interest were excluded. We assessed the associations between decreased rest-activity rhythm amplitude and outcomes using Cox proportional hazards models.FINDINGS: Between June 1, 2013, and Dec 23, 2015, 103 682 participants with available raw accelerometer data were enrolled. 92 614 participants (52 219 [56·4%] women and 40 395 [42·6%] men) with a median age of 64 years (IQR 56-69) were recruited. Median follow-up was 6·4 years (IQR 5·8-6·9). Decreased rest-activity rhythm amplitude was significantly associated with increased incidence of cardiovascular diseases (adjusted hazard ratio 1·11 [95% CI 1·05-1·16]), cancer (1·08 [1·01-1·16]), infectious diseases (1·31 [1·22-1·41]), respiratory diseases (1·26 [1·19-1·34]), and digestive diseases (1·08 [1·03-1·14]), as well as all-cause mortality (1·54 [1·40-1·70]) and disease-specific mortality (1·73 [1·34-2·22] for cardiovascular diseases, 1·32 [1·13-1·55] for cancer, and 1·62 [1·25-2·09] for respiratory diseases). Most of these associations were not modified by age older than 65 years or sex. Among 16 accelerometer-measured rest-activity parameters, low rest-activity rhythm amplitude had the strongest or second- strongest associations with nine health outcomes.INTERPRETATION: Our results suggest that low rest-activity rhythm amplitude might contribute to major health outcomes and provide further evidence to promote risk-modifying strategies associated with rest-activity rhythm to improve health and longevity.
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| 5. |
- Wang, Mengmeng, et al.
(författare)
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Statistical analysis of whistler precursors upstream of foreshock transient shocks : MMS observations
- 2024
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Ingår i: Geophysical Research Letters. - : American Geophysical Union (AGU). - 0094-8276 .- 1944-8007. ; 51:8
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Tidskriftsartikel (refereegranskat)abstract
- Using the high-time-resolution data from the Magnetospheric Multiscale mission, precursor waves upstream of foreshock transient (FT) shocks are statistically investigated using the four-spacecraft timing method. The wave frequencies and wave vectors determined in the plasma rest frame (PRF) are shown to follow the cold plasma dispersion relation for whistler waves. Combining with the feature of the right-hand polarization in the PRF, the precursors are identified as whistler-mode waves around the lower hybrid frequency. The occurrence of whistler precursors is independent of the Alfvén Mach number and the FT shock normal angle. More importantly, all the whistler precursors have group velocities pointing upstream in the shock frame, suggesting the dispersive radiation to be a possible generation mechanism. The study improves the understanding of not only the whistler precursors but also the overall FT shock dynamics.
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| 6. |
- Wei, Minrui, et al.
(författare)
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Vibronic fine structure in the nitrogen 1s photoelectron spectra of molecules from Franck-Condon simulations: Azines
- 2022
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society (APS). - 2469-9926 .- 2469-9934. ; 106:2
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Tidskriftsartikel (refereegranskat)abstract
- Vibronic coupling plays a pivotal role in molecular spectroscopy. We present a theoretical study on vibrationally resolved x-ray photoelectron spectra (XPS) of seven azines (CxHyNz; pyridine, three diazines, two triazines, and one tetrazine) at the nitrogen 1s edge, to explore the vibronic coupling effects as influenced by consecutive replacement of the CH group with a N atom. Franck-Condon simulations were performed with the Duschinsky rotation effect included, where the electronic structure was calculated by the density functional theory. Validations on pyrimidine show good agreement with the experiment, weak functional dependence, and weak mode mixing effect. We observed an evident blue shift in binding energies with the increasing number of N atoms in this series, together with molecule-dependent vibronic fine structures. These molecules have either C2v or Cs molecular symmetry at the optimized core-ionized geometries. Franck-Condon-active vibrational modes were identified to be low frequency (500–1650 cm−1), totally symmetric (A1 or A′), in-plane ring deformation modes. Core ionization on N∗ always leads to elongation of the N∗−N bond length, accompanied by an increase of the ∠C−N∗−X bond angle (X=C, N). Our study predicts accurate theoretical reference spectra for the azine family and provides useful information on the properties of the core-ionized states as influenced by the structural change of CH↔N replacement.
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| 7. |
- Zhang, Ben, et al.
(författare)
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Rapid solidification for green-solvent-processed large-area organic solar modules with >16% efficiency
- 2024
-
Ingår i: Energy & Environmental Science. - : ROYAL SOC CHEMISTRY. - 1754-5692 .- 1754-5706.
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Tidskriftsartikel (refereegranskat)abstract
- Enabling green-solvent-processed large-area organic solar cells (OSCs) is of great significance to their industrialization. However, precisely controlling the temperature-dependent fluid mechanics and evaporation behavior of green solvents with high-boiling points is challenging. Controlling these parameters is essential to prevent the non-uniform distribution of active layer components and severe molecule aggregation, which collectively degrade the power conversion efficiency (PCE) of large-scale devices. In this study, we revealed that the temperature gradient distribution across a wet film is the root of the notorious Marangoni effect, which leads to the formation of a severely non-uniform active layer on a large scale. Thus, a rapid solidification strategy was proposed to accelerate the evaporation of toluene, a green solvent, at room temperature. This strategy simultaneously inhibits the Marangoni effect and suppresses molecular aggregation in the wet film, allowing the formation of a nano-scale phase separation active layer with uniform morphology. The resultant toluene-processed 15.64-cm2 large-area OSC module achieves an outstanding PCE of 16.03% (certified: 15.69%), which represents the highest reported PCE of green-solvent-processed OSC modules. Notably, this strategy also exhibits a weak scale dependence on the PCE, and we successfully achieved a state-of-the-art PCE of 14.45% for a 72.00-cm2 OSC module. A rapid solidification strategy was developed for simultaneously avoiding the Marangoni effect and suppressing molecular aggregation. The resultant 15.64 cm2 large-area OSC module exhibited a record power conversion efficiency of 16.03%.
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| 8. |
- Zhang, Ting, et al.
(författare)
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Microstructure evolution and deformation mechanism of alpha plus beta dual-phase Ti-xNb-yTa-2Zr alloys with high performance
- 2022
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Ingår i: Journal of Materials Science & Technology. - : Elsevier BV. - 1005-0302. ; 131, s. 68-81
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Tidskriftsartikel (refereegranskat)abstract
- Biomedical beta-phase Ti-Nb-Ta-Zr alloys usually exhibit low elastic modulus with inadequate strength. In the present work, a series of newly developed dual-phase Ti-xNb-yTa-2Zr (wt.%) alloys with high performance were investigated in which the stability of beta-phase was reduced under the guidelines of ab initio calculations and d-electronic theory. The effects of Nb and Ta contents on the microstructure, compressive and tensile properties were investigated. Results demonstrate that the designed Ti-xNb-yTa-2Zr alloys exhibit typical characteristics of alpha+beta dual-phase microstructure. The microstructure of the alloys is more sensitive to Nb rather than Ta. The as-cast alloys exhibit needle-like alpha' martensite at a lower Nb content of 3 wt.% and lamellar alpha' martensite at an Nb content of 5 wt.%. Among the alloys, the Ti-3Nb-13Ta-2Zr alloy shows the highest compressive strength (2270 +/- 10 MPa) and compressive strain (74.3% +/- 0.4%). This superior performance is due to the combination of alpha+beta dual-phase microstructure and stress-induced alpha '' martensite. Besides, lattice distortion caused by Ta element also contributes to the compressive properties. Nb and Ta contents of the alloys strongly affect Young's modulus and tensile properties after rolling. The as-rolled Ti-3Nb-13Ta-2Zr alloy exhibits much lower modulus due to lower Nb content as well as more alpha '' martensite and beta phase with a good combination of low modulus and high strength among all the designed alloys. Atom probe tomography analysis reveals the element partitioning between the a and beta phases in which Ta concentration is higher than Nb in the alpha phase. Also, the concentration of Ta is lower than that of Nb in the beta phase, indicating that the beta-stability of Nb is higher than that of Ta. This work proposes modern alpha+beta dual-phase Ti-xNb-yTa-2Zr alloys as a new concept to design novel biomedical Ti alloys with high performance.
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| 9. |
- Bennett, Kochise, et al.
(författare)
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Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
- 2016
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Ingår i: Physica Scripta. - : IOP PUBLISHING LTD. - 0031-8949 .- 1402-4896. ; T169
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Tidskriftsartikel (refereegranskat)abstract
- New x-ray free electron laser (XFEL) and high harmonic generation (HHG) light sources are capable of generating short and intense pulses that make x-ray nonlinear spectroscopy possible. Multidimensional spectroscopic techniques, which have long been used in the nuclear magnetic resonance, infrared, and optical regimes to probe the electronic structure and nuclear dynamics of molecules by sequences of short pulses with variable delays, can thus be extended to the attosecond x-ray regime. This opens up the possibility of probing core-electronic structure and couplings, the real-time tracking of impulsively created valence-electronic wavepackets and electronic coherences, and monitoring ultrafast processes such as nonadiabatic electron-nuclear dynamics near conical-intersection crossings. We survey various possible types of multidimensional x-ray spectroscopy techniques and demonstrate the novel information they can provide about molecules.
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| 10. |
- Feng, Junlong, et al.
(författare)
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Two-sided Discrimination in an Entrepreneurial Financing Setting : Experimental and Theoretical Evidence
- 2022
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Ingår i: SSRN Electronic Journal. - : SSRN. - 1556-5068 .- 1556-5068.
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Women's participation rate in the high-growth entrepreneurship has been consistently lower than in other high-skilled jobs for previous decades. This paper aims to explain this unique persistent gender gap in both the US venture capital industry and the US entrepreneurial activities from the point of view of gender discrimination on both sides of a two-sided matching market (i.e., the US entrepreneurial financing market). We invite real US startup founders to evaluate multiple randomly generated venture capitalists' and angel investors' profiles. Despite knowing all investor profiles are hypothetical, startup founders are willing to provide truthful evaluations to receive a data-driven investor recommendation list. This experiment provides the following findings. (i) Male entrepreneurs have implicit gender discrimination against female investors, who are perceived as lower quality and with fewer investment intentions. However, gender discrimination does not exist among female entrepreneurs. (ii) Implicit gender discrimination mainly exists among attractive investors and senior investors, suggesting the existence of a glass ceiling for women in the financial industry. (iii) The magnitude of implicit gender discrimination is stronger when startup founders' internal thresholds are higher, and investors need to compete for great deals. Together with Zhang(2020), this paper completes an experimental system that identifies gender discrimination on both the investor side and startup side in the US entrepreneurial finance system. Built on this experimental evidences, we provide a theoretical framework to explain several novel findings in recent experiments and how this two-sided gender discrimination can lead to a long-lasting low participation rate for women in the US entrepreneurial community
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| 11. |
- Guo, Shilong, et al.
(författare)
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Investigation on bluff-body and swirl stabilized flames near lean blowoff with PIV/PLIF measurements and LES modelling
- 2019
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Ingår i: Applied Thermal Engineering. - : Elsevier BV. - 1359-4311. ; 160
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Tidskriftsartikel (refereegranskat)abstract
- Lean premixed combustion (LPC) is a promising technology for low-NOx emission, while it increases the risk of blowoff at the same time. Experiments and Large Eddy Simulations (LES) on swirl stratified lean-premixed CH4/air flames were performed to study the differences between the stable and near blowoff flame. The flow fields and instantaneous flame structures were measured by simultaneous Particle Image Velocimetry (PIV) and Planar Laser Induced Fluorescence (OH-PLIF). The Thickened Flame (TF) model coupled with a two-step reduced chemical mechanism was used in LES modelling. The non-dynamic formulation of sub-grid flame wrinkling model is performed well for stable condition while it cannot predict the near lean blowoff flame reasonable. Compared with the stable flame, several significant differences can be observed in the near lean blowoff flame. The height of high-temperature-zone is relatively low and the heat loss of flame attachment can be easily enhanced by the low temperature spot induced by flame-vortex interaction. The flame attachment is subject to higher excess strain rate and turbulence fluctuation. Meanwhile, a Processing Vortex Core (PVC) appears downstream of the centerline. It is concluded that lean blowoff is the result of interactions between the fuel/air mixture ignition, PVC instability and flame attachment lift-off.
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| 12. |
- Hu, Kaibo, et al.
(författare)
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Highly selective recovery of rare earth elements from mine wastewater by modifying kaolin with phosphoric acid
- 2023
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Ingår i: Separation and Purification Technology. - : Elsevier. - 1383-5866 .- 1873-3794. ; 309
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Tidskriftsartikel (refereegranskat)abstract
- Recovery of rare earth elements (REEs) from mine wastewater is essential for maintaining rare earth reserves and sustainable application of REEs. In the present study, we prepared a phosphoric acid modified kaolin (P-K) adsorbent by a simple mechanochemical process for the selective recovery of REEs from rare earth wastewater. The impacts of phosphoric acid dosage, milling duration, initial pH, temperature, initial ion concentration, and adsorbent dosage on the selective adsorption of REEs were investigated. The findings demonstrate that the adsorption of REEs by P-K follows pseudo-second-order kinetic model and the Langmuir isotherm model, and is dominated by chemical adsorption, with a maximum adsorption capacity of 19.82 mg/g at 50 ℃. Additionally, in an original mine wastewater, the recovery rate of REEs can reach more than 90%, whereas the adsorption rates of calcium, magnesium and, ammonia nitrogen (whose concentration is 18 times that of REEs) are nearly zero, indicating that P-K has extremely high selectivity for REEs. Furthermore, the feedstock solution containing 40 mg/L of REEs may be concentrated to 3510 mg/L following enrichment treatment, and 99.9% of the REEs are eluted using a low concentration of hydrochloric acid. The findings illustrate that P-K has a wide range of potential applications in the treatment of rare earth industrial effluents.
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| 13. |
- Hua, Weijie, et al.
(författare)
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Study of double core hole excitations in molecules by X-ray double-quantum-coherence signals : a multi-configuration simulation
- 2016
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Ingår i: Chemical Science. - : Royal Society of Chemistry. - 2041-6520 .- 2041-6539. ; 7:9, s. 5922-5933
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Tidskriftsartikel (refereegranskat)abstract
- The multi-configurational self-consistent field method is employed to simulate the two-dimensional all-X-ray double-quantum-coherence (XDQC) spectroscopy, a four-wave mixing signal that provides direct signatures of double core hole (DCH) states. The valence electronic structure is probed by capturing the correlation between the single (SCH) and double core hole states. The state-averaged restricted-activespace self-consistent field (SA-RASSCF) approach is used which can treat the valence, SCH, and DCH states at the same theoretical level, and applies to all types of DCHs (located on one or two atoms, K-edge or L-edge), with both accuracy and efficiency. Orbital relaxation introduced by the core hole(s) and the static electron correlation is properly accounted for. The XDQC process can take place via different intermediate DCH state channels by tuning the pulse frequencies. We simulate the XDQC signals for the three isomers of aminophenol at 8 pulse frequency configurations, covering all DCH pathways involving the N1s and O1s core hole (N1sN1s, O1sO1s and N1sO1s), which reveal different patterns of valence excitations.
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| 14. |
- Huang, Yuting, et al.
(författare)
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Host-Guest Strategy Enabling Nonhalogenated Solvent Processing for High-Performance All-Polymer Hosted Solar Cells
- 2023
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Ingår i: Chinese journal of chemistry. - : WILEY-V C H VERLAG GMBH. - 1001-604X .- 1614-7065. ; 41:9, s. 1066-1074
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Tidskriftsartikel (refereegranskat)abstract
- The power conversion efficiencies (PCEs) of all-polymer solar cells (all-PSCs), usually processed from low-boiling-point and toxic solvents, have reached high values of 18%. However, poor miscibility and uncontrollable crystallinity in polymer blends lead to a notable drop in the PCEs when using green solvents, limiting the practical development of all-PSCs. Herein, a third component (guest) BTO was employed to optimize the miscibility and enhance the crystallinity of PM6/PY2Se-F host film processed from green solvent toluene (TL), which can effectively suppress the excessive aggregation of PY2Se-F and facilitate a nano-scale interpenetrating network morphology for exciton dissociation and charge transport. As a result, TL-processed all-polymer hosted solar cells (all-PHSCs) exhibited an impressive PCE of 17.01%. Moreover, the strong molecular interaction between the host and guest molecules also enhances the thermal stability of the devices. Our host-guest strategy provides a unique approach to developing high-efficiency and stable all-PHSCs processed from green solvents, paving the way for the industrial development of all-PHSCs.
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| 15. |
- Ji, Longjuan, et al.
(författare)
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Structure and thermoacoustic instability of turbulent swirling lean premixed methane/hydrogen/air flames in a model combustor
- 2024
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Ingår i: International Journal of Hydrogen Energy. - 0360-3199. ; 60, s. 890-901
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Tidskriftsartikel (refereegranskat)abstract
- The structure and thermoacoustic instability (TI) of premixed CH4/H2/air swirling flames were experimentally investigated for a range of hydrogen fraction (ηH2) up to 80% under different equivalence ratio (Φ) and swirl number (S) conditions. It is shown that the onset of TI is enhanced when increasing either ηH2, S, or Φ. The dominant frequency of TI increases dramatically with ηH2. The higher dominant frequency in the hydrogen-enriched flames can be attributed to a shorter flame length which results in a reduced flame convection time. It is observed that the unstable flames are always accompanied by the appearance of outer recirculation zone (ORZ) flame. Therefore, the flame kernel residing in the ORZ can be an indicator of the occurrence of TI. The flame front of thermoacoustic unstable flames was observed to be more wrinkled, e.g., with larger mean absolute curvature (κ abs) and local flame surface area ratio (δΣmax). Importantly, the phase-locked analysis shows that κ abs and δΣmax can be modified at different oscillation phases, and their maximum and minimum values are simultaneously achieved at phase angles θ of about 0° and 180°, respectively. Variations of κ abs and δΣmax are in phase with the heat release rate, indicating a strong correlation between the TI and flame structure modification; however, they show a phase lag of about 72° behind the pressure in this work. These results are vital when understanding and predicting the TI based on the flame structure, especially when adopting a visual detection method of the instability.
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| 16. |
- Qin, Ning, et al.
(författare)
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Increased CO 2 fixation enables high carbon-yield production of 3-hydroxypropionic acid in yeast
- 2024
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Ingår i: Nature Communications. - 2041-1723 .- 2041-1723. ; 15:1
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Tidskriftsartikel (refereegranskat)abstract
- CO2 fixation plays a key role to make biobased production cost competitive. Here, we use 3-hydroxypropionic acid (3-HP) to showcase how CO2 fixation enables approaching theoretical-yield production. Using genome-scale metabolic models to calculate the production envelope, we demonstrate that the provision of bicarbonate, formed from CO2, restricts previous attempts for high yield production of 3-HP. We thus develop multiple strategies for bicarbonate uptake, including the identification of Sul1 as a potential bicarbonate transporter, domain swapping of malonyl-CoA reductase, identification of Esbp6 as a potential 3-HP exporter, and deletion of Uga1 to prevent 3-HP degradation. The combined rational engineering increases 3-HP production from 0.14 g/L to 11.25 g/L in shake flask using 20 g/L glucose, approaching the maximum theoretical yield with concurrent biomass formation. The engineered yeast forms the basis for commercialization of bio-acrylic acid, while our CO2 fixation strategies pave the way for CO2 being used as the sole carbon source.
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| 17. |
- Wang, Sheng-Yu, et al.
(författare)
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Interpreting the Cu-O2 Antibonding Nature in Two Cu-O2 Complexes from Cu L-Edge X-ray Absorption Spectra
- 2023
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 62:42, s. 17115-17125
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Tidskriftsartikel (refereegranskat)abstract
- Cu–O2 structures play important roles in bioinorganic chemistry and enzyme catalysis, where the bonding between the Cu and O2 parts serves as a fundamental research concern. Here, we performed a multiconfigurational study on the copper L2,3-edge X-ray absorption spectra (XAS) of two copper enzyme model complexes to gain a better understanding of the antibonding nature from the clearly interpreted structure–spectroscopy relation. We obtained spectra in good agreement with the experiments by using the restricted active space second-order perturbation theory (RASPT2) method, which facilitated reliable chemical analysis. Spectral feature interpretations were supported by computing the spin–orbit natural transition orbitals. All major features were assigned to be mainly from Cu 2p to antibonding orbitals between Cu 3d and O2 π*, Cu 3d−πO–O* (type A), and a few also to mixed antibonding/bonding orbitals between Cu 3d and O2 π, Cu 3d ± πO–O (type M). Our calculations provided a clear illustration of the interactions between Cu 3d and O2 π*/π orbitals that are carried in the metal L-edge XAS.
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| 18. |
- Yang, Heyi, et al.
(författare)
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Composition-Conditioning Agent for Doped Spiro-OMeTAD to Realize Highly Efficient and Stable Perovskite Solar Cells
- 2022
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Ingår i: Advanced Energy Materials. - : WILEY-V C H VERLAG GMBH. - 1614-6832 .- 1614-6840. ; 12:44
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Tidskriftsartikel (refereegranskat)abstract
- The doped Spiro-OMeTAD hole transport layer (HTL) formed using the lithium bis(trifluoromethane) sulfonimide salt and 4-tert-butylpyridine with phenethylammonium iodide surface treatment on a perovskite film has continuously dominated the record power conversion efficiencies (PCEs) of perovskite solar cells (pero-SCs). However, unstable HTL compositions and iodide salts can cause severe device degradation. In this study, an HTL composition-conditioning agent (CCA), Spiro-BD-2OEG, is designed, which contains a Spiro-OMeTAD-like backbone, functional pyridine units, and oligo (ethylene glycol) chains. This finely designed CCA presents good miscibility with Spiro-OMeTAD and its dopants and acts as a conditioning agent through weak bond interactions. As a result, the CCA-regulated HTL shows a pinhole-free and smooth morphology with enhanced Spiro-OMeTAD ordering and improves dopant stability. In addition, the gradient-distributed CCA in the HTL can narrow the energy level offset with the valence band of the perovskite. The resultant pero-SCs exhibit an excellent PCE of 24.19% without any interface treatment and weak size dependence. A remarkable PCE of 22.63% is obtained even for a 1.004-cm(2) device. Importantly, the strategy shows good universality and significantly promotes the long-term stability of the pero-SCs based on the classical doped Spiro-OMeTAD.
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| 19. |
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| 20. |
- Zhang, Jun-Rong, et al.
(författare)
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Accurate K-edge X-ray photoelectron and absorption spectra of g-C3N4 nanosheets by first-principles simulations and reinterpretations
- 2019
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : ROYAL SOC CHEMISTRY. - 1463-9076 .- 1463-9084. ; 21:41, s. 22819-22830
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Tidskriftsartikel (refereegranskat)abstract
- We performed a density functional theory (DFT) study on X-ray photoelectron (XPS) and absorption (XAS) spectra of graphitic carbon nitride (g-C3N4) nanosheets at the N and C K-edges. A combined cluster-periodic approach was employed to calculate XPS spectra, in which the core ionic potential (IP) of the solid 2D material was computed by subtracting the work function (obtained with periodic conditions) from the gas phase IP (obtained with large cluster models). With amino-terminated supermolecules of different sizes, we obtained convergent spectra and provide new assignments for 5 nitrogen [1 sp(2); 4 sp(3) (bridging, tertiary, and primary/secondary amino nitrogens)] and 4 carbon (all bonded with three nitrogens) local structures. A good agreement with experiments was obtained, with the N1s (C1s) main peak position differing by 0.1-0.2 eV (0.5-0.8 eV). Our simulations show that N1s XPS of pure g-C3N4 contains only two major features at 398.6 and 401.2 eV, contributed from sp(2)-N and sp(3)-N, respectively. The chemical shifts of all sp(3)-N are so close (deviating by 0.3-0.6 eV) that terminal amino groups -NHx (x = 1, 2) will only be distinguished in high-resolution measurements. In C1s XPS, all carbons show similar (deviation < 0.2 eV) IPs, as determined by the same nearest neighbors. We further excluded the effect of shake-up satellites that may change our XPS interpretations by equivalent core hole time-dependent DFT (ECH-TDDFT) simulations. The effect of vibronic coupling is small (redistribution is only 0.1-0.3 eV to the higher-energy region) in the N1s edge as estimated from the asymmetric main peak shape, and negligible in the C1s edge. Quicker size convergence was found in XAS than XPS. In N1s XAS, we identified a weak pi* spectral feature at 400-401 eV for both -NHx and tertiary nitrogens. Our study provides a clear theoretical reference for X-ray spectral fingerprints of different local structures, which is useful for analysis of g-C3N4 based materials with various designed or unavoidable structural modifications. We also highlight our combined cluster-periodic approach in calculating the K-edge XPS spectra of general 2D materials which predicts accurate absolute values.
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| 21. |
- Zhang, Weijie, et al.
(författare)
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The effect of relative humidity on eddy covariance latent heat flux measurements and its implication for partitioning into transpiration and evaporation
- 2023
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Ingår i: Agricultural and Forest Meteorology. - : Elsevier BV. - 0168-1923. ; 330
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Tidskriftsartikel (refereegranskat)abstract
- While the eddy covariance (EC) technique is a well-established method for measuring water fluxes (i.e., evaporation or 'evapotranspiration’, ET), the measurement is susceptible to many uncertainties. One such issue is the potential underestimation of ET when relative humidity (RH) is high (>70%), due to low-pass filtering with some EC systems. Yet, this underestimation for different types of EC systems (e.g. open-path or closed-path sensors) has not been characterized for synthesis datasets such as the widely used FLUXNET2015 dataset. Here, we assess the RH-associated underestimation of latent heat fluxes (LE, or ET) from different EC systems for 163 sites in the FLUXNET2015 dataset. We found that the LE underestimation is most apparent during hours when RH is higher than 70%, predominantly observed at sites using closed-path EC systems, but the extent of the LE underestimation is highly site-specific. We then propose a machine learning based method to correct for this underestimation, and compare it to two energy balance closure based LE correction approaches (Bowen ratio correction, BRC, and attributing all errors to LE). Our correction increases LE by 189% for closed-path sites at high RH (>90%), while BRC increases LE by around 30% for all RH conditions. Additionally, we assess the influence of these corrections on ET-based transpiration (T) estimates using two different ET partitioning methods. Results show opposite responses (increasing vs. slightly decreasing T-to-ET ratios, T/ET) between the two methods when comparing T based on corrected and uncorrected LE. Overall, our results demonstrate the existence of a high RH bias in water fluxes in the FLUXNET2015 dataset and suggest that this bias is a pronounced source of uncertainty in ET measurements to be considered when estimating ecosystem T/ET and WUE.
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