| 1. |
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- 2019
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Tidskriftsartikel (refereegranskat)
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| 2. |
- Chen, Xue, et al.
(författare)
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Co-Doped Fe3S4Nanoflowers for Boosting Electrocatalytic Nitrogen Fixation to Ammonia under Mild Conditions
- 2022
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Ingår i: Inorganic Chemistry. - : American Chemical Society. - 0020-1669 .- 1520-510X. ; 61:49, s. 20123-20132
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Tidskriftsartikel (refereegranskat)abstract
- Compared with the Haber Bosch process, the electrochemical nitrogen reduction reaction (NRR) under mild conditions provides an alternative and promising route for ammonia synthesis due to its green and sustainable features. However, the great energy barrier to break the stable NN bond hinders the practical application of NRR. Though Fe is the only common metal element in all biological nitrogenases in nature, there is still a lack of study on developing highly efficient and low-cost Fe-based catalysts for N2fixation. Herein, Co-doped Fe3S4nanoflowers were fabricated as the intended catalyst for NRR. The results indicate that 4% Co-doped Fe3S4nanoflowers achieve a high Faradaic efficiency of 17% and a NH3yield rate of 37.5 μg·h-1·mg-1cat.at-0.55 V versus RHE potential in 0.1 M HCl, which is superior to most Fe-based catalysts. The introduction of Co atoms can not only shift the partial density states of Fe3S4toward the Fermi level but also serve as new active centers to promote N2absorption, lowering the energy barrier of the potential determination step to accelerate the catalytic process. This work paves a pathway of the morphology and doping engineering for Fe-based electrocatalysts to enhance ammonia synthesis.
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| 3. |
- Luo, Xiyu, et al.
(författare)
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Effects of local compositional heterogeneity in mixed halide perovskites on blue electroluminescence
- 2024
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Ingår i: Matter. - 2590-2393. ; 7:3, s. 1054-1070
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Tidskriftsartikel (refereegranskat)abstract
- Compositional heterogeneity is commonly observed in mixed bromide/iodide perovskite photoabsorbers, typically with minimal effects on charge carrier recombination and photovoltaic performance. Consistently, it has so far received very limited attention in bromide/chloride-mixed perovskites, which hold particular significance for blue light-emitting diodes. Here, we uncover that even a minor degree of localized halide heterogeneity leads to severe non-radiative losses in mixed bromide/chloride blue perovskite emitters, presenting a stark contrast to general observations in photovoltaics. We not only provide a visualization of the heterogeneity landscape spanning from micro-to sub-microscale but also identify that this issue mainly arises from the initially formed chloride-rich clusters during perovskite nucleation. Our work sheds light on a long-term neglected factor impeding the advancement of blue light-emitting diodes using mixed halide perovskites and provides a practical strategy to mitigate this issue.
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| 4. |
- Yuan, Chunyu, et al.
(författare)
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Defect and Donor Manipulated Highly Efficient Electron-Hole Separation in a 3D Nanoporous Schottky Heterojunction
- 2023
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Ingår i: JACS Au. - : American Chemical Society (ACS). - 2691-3704. ; 3:11, s. 3127-3140
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Tidskriftsartikel (refereegranskat)abstract
- Given the rapid recombination of photogenerated charge carriers and photocorrosion, transition metal sulfide photocatalysts usually suffer from modest photocatalytic performance. Herein, S-vacancy-rich ZnIn2S4 (VS-ZIS) nanosheets are integrated on 3D bicontinuous nitrogen-doped nanoporous graphene (N-npG), forming 3D heterostructures with well-fitted geometric configuration (VS-ZIS/N-npG) for highly efficient photocatalytic hydrogen production. The VS-ZIS/N-npG presents ultrafast interfacial photogenerated electrons captured by the S vacancies in VS-ZIS and holes neutralization behaviors by the extra free electrons in N-npG during photocatalysis, which are demonstrated by in situ XPS, femtosecond transient absorption (fs-TA) spectroscopy, and transient-state surface photovoltage (TS-SPV) spectra. The simulated interfacial charge rearrangement behaviors from DFT calculations also verify the separation tendency of photogenerated charge carriers. Thus, the optimized VS-ZIS/N-npG 3D hierarchical heterojunction with 1.0 wt % N-npG exhibits a comparably high hydrogen generation rate of 4222.4 μmol g–1 h–1, which is 5.6-fold higher than the bare VS-ZIS and 12.7-fold higher than the ZIS without S vacancies. This work sheds light on the rational design of photogenerated carrier transfer paths to facilitate charge separation and provides further hints for the design of hierarchical heterostructure photocatalysts.
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| 5. |
- Ba, Kun, et al.
(författare)
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Billiard Catalysis at Ti3C2 MXene/MAX Heterostructure for Efficient Nitrogen Fixation
- 2022
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 317, s. 121755-
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Tidskriftsartikel (refereegranskat)abstract
- Electrocatalytic ammonia (NH3) conversion under ambient atmosphere is crucial to mimic the nature's nitrogen cycle. But currently it is always interrupted by the HER process which is more competitive. Herein, we tactically cultivate a series of incompletely etched Ti3AlC2 MAX / Ti3C2 MXene based heterostructure catalysts whose composition can be finely tuned through regulation of the LiF percentage in mixed chemical etching agent. Notably, the surface potential difference between MAX and MXene is ~40 mV, indicating that the electron can be readily transferred from MAX to MXene across the interfaces, which is favorable for N2 fixation, yielding an outstanding Faradic efficiency of 36.9%. Furthermore, density functional theory calculations reveal the billiard-like catalysis mechanism, where the intermediates are alternatively adsorbed on MAX or MXene surfaces. Meanwhile, the rate-determining step of *NH → *NH2 possesses an energy barrier of 0.96 eV on the hetero-interface which follows associative distal mechanism. This work opens a new frontier of heterostructured catalyst for balancing electrical conductivity and catalytic activity in electrocatalysis.
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| 6. |
- Cheng, Qiaoyun, et al.
(författare)
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The conversion of nanocellulose into solvent-free nanoscale liquid crystals by attaching long side-arms for multi-responsive optical materials
- 2020
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Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 8:32, s. 11022-11031
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Tidskriftsartikel (refereegranskat)abstract
- Nanocellulose, with its unique optical and chemical properties, has received increasing attention as feedstock to fabricate sustainable materials. However, achieving a nanocellulose-based solvent-free liquid crystal with good responsiveness still remains a challenge. Herein, for the first time, solvent-free supramolecular liquid crystals were fabricated by attaching long side-arms on the fiber-like nanocellulose derived from tunicate (TCNC) with an average width of 20 nm and 400-3000 nm in length. The side-arms were grafted via surface condensation with a charged organosilane, followed by further functionalization with a counter-ion polyoxyethylene ether. The nanoscale liquid crystals consisted of the stiff TCNC as the core and flexible side-arms as the soft shells, forming the core-shell structure with an average width of 34-36 nm. The resulting solvent-free liquid crystal exhibited transparent and viscous liquid-like fluidity, as well as a bright birefringence between the crossed polarizers at room temperature. In our findings, the stiff core provided crystal-like ordering, whereas the soft shells induced the high mobility of the TCNCs as a result of the increased fractional free volume, as shown by positron annihilation lifetime spectra. The unique flowability enables the possibility of multi-responsiveness to temperature, deformation, and alternating electric fields. In addition, the thermo-responsiveness can be regulated by tailoring the canopy. This work provides a novel strategy for the conversion of solid nanocellulose into a solvent-free nanoscale liquid crystal, which is promising for use as a responsive optical material.
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| 7. |
- Gao, Hong, et al.
(författare)
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The landscape of tolerated genetic variation in humans and primates
- 2023
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 380:6648
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Tidskriftsartikel (refereegranskat)abstract
- Personalized genome sequencing has revealed millions of genetic differences between individuals, but our understanding of their clinical relevance remains largely incomplete. To systematically decipher the effects of human genetic variants, we obtained whole-genome sequencing data for 809 individuals from 233 primate species and identified 4.3 million common protein-altering variants with orthologs in humans. We show that these variants can be inferred to have nondeleterious effects in humans based on their presence at high allele frequencies in other primate populations. We use this resource to classify 6% of all possible human protein-altering variants as likely benign and impute the pathogenicity of the remaining 94% of variants with deep learning, achieving state-of-the-art accuracy for diagnosing pathogenic variants in patients with genetic diseases.
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| 8. |
- Kuderna, Lukas F. K., et al.
(författare)
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Identification of constrained sequence elements across 239 primate genomes
- 2024
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Ingår i: Nature. - : Springer Nature. - 0028-0836 .- 1476-4687. ; 625:7996, s. 735-742
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Tidskriftsartikel (refereegranskat)abstract
- Noncoding DNA is central to our understanding of human gene regulation and complex diseases1,2, and measuring the evolutionary sequence constraint can establish the functional relevance of putative regulatory elements in the human genome3,4,5,6,7,8,9. Identifying the genomic elements that have become constrained specifically in primates has been hampered by the faster evolution of noncoding DNA compared to protein-coding DNA10, the relatively short timescales separating primate species11, and the previously limited availability of whole-genome sequences12. Here we construct a whole-genome alignment of 239 species, representing nearly half of all extant species in the primate order. Using this resource, we identified human regulatory elements that are under selective constraint across primates and other mammals at a 5% false discovery rate. We detected 111,318 DNase I hypersensitivity sites and 267,410 transcription factor binding sites that are constrained specifically in primates but not across other placental mammals and validate their cis-regulatory effects on gene expression. These regulatory elements are enriched for human genetic variants that affect gene expression and complex traits and diseases. Our results highlight the important role of recent evolution in regulatory sequence elements differentiating primates, including humans, from other placental mammals.
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| 9. |
- Yu, Weibin, et al.
(författare)
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Facile preparation of sulfonated biochar for highly efficient removal of toxic Pb(II) and Cd(II) from wastewater
- 2021
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Ingår i: Science of the Total Environment. - : ELSEVIER. - 0048-9697 .- 1879-1026. ; 750
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Tidskriftsartikel (refereegranskat)abstract
- Biochar is deemed as the ideal material for the effective removal of heavy metals in wastewater treatment. Herein, we developed a facile one-step solvothermal method for the preparation of sulfonated biochar (SBC) from Axonopus compressus under a low-temperature condition. FTIR and XPS analysis demonstrate that plenty of -OH, -COOH and -SO3H moieties are generated on the surface of SBC during the sulfonation process. Due to high electronegativity and strong complexation of these moieties, SBC can rapidly adsorb Pb(II) and Cd(II) with capacities of 191.07 and 85.76 mg/g respectively within 5 min. SBC can be reused for 5 cycles with a negligible loss of adsorption capacity. In addition, different biomass-based biochars are prepared under the identical experimental conditions, and they are successfully applied in the treatments of Pb(II) and Cd(II). The satisfying results indicate that one-step low-temperature sulfonation could be a universalmethod, and various types of biomass waste could be the abundant, effective, economical material source for the treatment of environmental heavy metal pollution in future. (C) 2020 Elsevier B.V. All rights reserved.
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| 10. |
- Zhang, Helin, et al.
(författare)
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Complex nonmonotonic responses of biodiversity to habitat destruction
- 2023
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Ingår i: Ecology. - : WILEY. - 0012-9658 .- 1939-9170.
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Tidskriftsartikel (refereegranskat)abstract
- It has typically been assumed that habitat destruction, characterized by habitat loss and fragmentation, has consistently negative effects on biodiversity. While numerous empirical studies have shown the detrimental effects of habitat loss, debate continues as to whether habitat fragmentation has universally negative effects. To explore the effects of habitat fragmentation, we developed a simple model for site-occupancy dynamics in fragmented landscapes. With the model, we demonstrate that a competition-colonization trade-off can result in nonlinear oscillatory responses in biodiversity to both habitat loss and fragmentation. However, the overall pattern of habitat loss reducing species richness is still established, in line with empirical observations. Interestingly, the existence of localized oscillations in biodiversity can explain the mixed responses of species richness to habitat fragmentation per se observed in nature, thereby reconciling the debate on the fragmentation-diversity relationship. Therefore, this study offers a parsimonious mechanistic explanation for empirically observed biodiversity patterns in response to habitat destruction.
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| 11. |
- Zhou, Xuming, et al.
(författare)
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Research on Theory and Technology of Floor Heave Control in Semicoal Rock Roadway: Taking Longhu Coal Mine in Qitaihe Mining Area as an Example
- 2022
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Ingår i: Lithosphere. - : GeoScienceWorld. - 1941-8264 .- 1947-4253. ; 2022:Special 11
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Tidskriftsartikel (refereegranskat)abstract
- As one of the most common disasters in deep mine roadway, floor heave has caused serious obstacles to mine transportation and normal production activities. The third section winch roadway in the third mining area of Qitaihe Longhu coal mine has a serious floor heave due to the large buried depths of the roadway and the semicoal rock roadway, and the maximum floor heave is 750 mm. For the problem of floor stability, this paper establishes a mechanical model to analyze the stability of roadway floor heave by analogy with the basement heave of deep foundation pit. It provides a model reference for analyzing the problem of roadway floor heave. Aiming at the problem of roadway floor heave in Longhu coal mine, the roadway model is established by using FLAC3D, and the roadway model after support is established according to the on-site support measures. Through the analysis of the distribution of roadway plastic area, stress nephogram, and displacement field simulation results, the results show that the maximum displacement of roadway roof and floor after support is reduced by 15% and 23%, but the maximum floor heave is still 770 mm, which is close to the measured floor heave of roadway. In order to solve the problem of roadway floor heave and integrate economic factors, this paper puts forward three support optimization schemes, simulates the support effect of each scheme, and finally determines that scheme 3 is the best support optimization scheme. Compared with that under the original support, the amount of floor heave is reduced by 81%, and the final amount of floor heave is 150 mm, which can meet the requirements of roadway floor deformation. The results provide a scheme and guidance for roadway support optimization
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