Lithium‐sulfur (Li‐S) batteries are one of the most promising candidates for high energy density rechargeable batteries beyond current Li‐ion batteries. However, severe corrosion of Li metal anode ...and low Coulombic efficiency (CE) induced by the unremitting shuttle of Li polysulfides immensely hinder the practical applications of Li‐S batteries. Herein, a compact inorganic layer (CIL) formed by ex situ reactions between Li anode and ionic liquid emerged as an effective strategy to block Li polysulfides and suppress shuttle effect. A CE of 96.7% was achieved in Li‐S batteries with CIL protected Li anode in contrast to 82.4% for bare Li anode while no lithium nitrate was employed. Furthermore, the corrosion of Li during cycling was effectively inhibited. While applied to working batteries, 80.6% of the initial capacity after 100 cycles was retained in Li‐S batteries with CIL‐protected ultrathin (33 μm) Li anode compared with 58.5% for bare Li anode, further demonstrating the potential of this strategy for practical applications. This study presents a feasible interfacial regulation strategy to protect Li anode with the presence of Li polysulfides and opens avenues for Li anode protection in Li‐S batteries under practical conditions.
A compact inorganic layer (CIL) that can block lithium polysulfides and shuttle effect in lithium‐sulfur batteries is constructed on lithium metal anode. The CIL renders much improved Coulombic efficiency without LiNO3 additive and ensures superior cycling performance of lithium‐sulfur batteries with ultrathin lithium metal anodes.
The persistent efforts to reveal the formation and evolution mechanisms of solid electrolyte interphase (SEI) are of fundamental significance for the rational regulation. In this work, through ...combined theoretical and experimental model investigations, we elucidate that the electric double layer (EDL) chemistry at the electrode/electrolyte interface beyond the thermodynamic stability of electrolyte components predominately controls the competitive reduction reactions during SEI construction on Li metal anode. Specifically, the negatively‐charged surface of Li metal will prompt substantial cation enrichment and anion deficiency within the EDL. Necessarily, only the species participating in the solvation shell of cations could be electrostatically accumulated in proximity of Li metal surface and thereafter be preferentially reduced during sustained dynamic cycling. Incorporating multi‐valent cation additives to more effectively drag the favorable anionic SEI enablers into EDL is validated as a promising strategy to upgrade the Li protection performance. The conclusions drawn herein afford deeper understandings to bridge the EDL principle, cation solvation, and SEI formation, shedding fresh light on the targeted regulation of reactive alkali metal interfaces.
The electric double layer chemistry and structure are identified to play a predominate role in governing the competitive reactions during solid electrolyte interphase formation on lithium‐metal anodes. This knowledge affords critical guidance on the targeted interface design to enable a stable working lithium anode.
AbstractThis study aims to develop a high-performance acrylate viscoelastic damper (HAVED), which is suitable for the low-frequency vibration control of building structures. To reveal the influence ...of ambient temperature, excitation frequency, and displacement amplitude on the dynamic mechanical performance and energy dissipation capacity of a HAVED, a series of dynamic mechanical performance tests were performed on a HAVED within the extensive temperature (10°C–50°C), frequency (0.1–3 Hz), and displacement (0.5–4 mm) range. The analysis results show that a HAVED has excellent energy dissipation capacity and good adaptability to the external environment. The loss factor of a HAVED can reach up to 1.85, and it remains above 0.28 even in a high-temperature environment of 50°C. The dynamic mechanical properties and energy dissipation capacity of a HAVED show strong dependences and obvious coupling effects on temperature, frequency, and displacement amplitude. Based on the experimental research of a HAVED, the micromechanical properties of viscoelastic materials are analyzed, and the high-order fractional derivative model is used to comprehensively describe the mechanical characterization of microscopic molecular chains. The Kraus theory is introduced to consider the influence of filler particles, and the high-order fractional derivative micro–macro cross-scale mathematical model is proposed by combining with the temperature-frequency equivalence principle. Through the experimental results, the prediction capabilities of the model that have been established have been verified. The analysis results show that the proposed model can comprehensively describe the influence of ambient temperature, excitation frequency, displacement amplitude, microscopic molecular chain structure, and filler particles on the mechanical properties of a HAVED.
In this study, a novel aggregation-induced emission supramolecular organic framework (AIE SOF) with ultrasensitive response, termed
FSOF
, was constructed using a tri-pillar5arene-based foldamer. ...Interestingly, benefiting from the noise signal shielding properties of
FSOF
as well as the competition between the cation π and π π interactions, the
FSOF
shows an ultrasensitive response for multi-analytes, such as Fe
3+
, Hg
2+
and Cr
3+
. The limits of detection (LODs) of the
FSOF
for Fe
3+
, Hg
2+
and Cr
3+
are in the range of 9.40 × 10
−10
-1.86 × 10
−9
. More importantly, the xerogel of
FSOF
exhibits porous mesh structures, which could effect high-efficiency separation above metal ions from their aqueous solution, with adsorption percentages in the range 92.39-99.99%. In addition, by introducing metal ions into the
FSOF
, a series of metal ions coordinated supramolecular organic frameworks (
MSOFs
) were successfully constructed. Moreover,
MSOFs
show selective fluorescence "turn on" ultrasensitive detection CN
−
(LOD = 2.12 × 10
−9
) and H
2
PO
4
−
(LOD = 1.78 × 10
−9
). This is a novel approach to construct SOFs through a tri-pillar5arene-based foldamer, and also provides a new way to achieve ultrasensitive detection and high-efficiency separation.
A novel aggregation-induced emission supramolecular organic framework (AIE SOF) constructed using tri-pillar5arene-based foldamer which could be used for the ultrasensitive detection of multi-analytes.
Lithium metal is among the most promising anode materials in next-generation energy-storage systems. However, Li dendrite growth and unstable solid electrolyte interphase have hindered its practical ...applications. Structured current collectors have been widely proposed to settle these issues, whereas the pre-filling of Li metal into structured anode is challenging. We proposed a coralloid silver-coated carbon fiber-based composite Li anode (CF/Ag-Li) through Ag electroplating and molten Li infusion. The molten Li can be infused into the carbon fiber framework due to the lithiophilic nature of Ag. In addition, a dendrite-free morphology and extraordinary electrochemical performance are achieved in Li-LiFePO4 and Li-sulfur cells. The CF/Ag-Li|Li symmetrical cells can cycle for 160 cycles at 10.0 mA cm−2 and 10.0 mAh cm−2. The CF/Ag-Li|S cells exhibited a high initial discharge capacity of 785 mAh g−1 and a large capacity retention rate after 400 cycles at 0.5C.
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•Coralloid carbon fibers were achieved by electroplating Ag onto their surface•Ag coating layer endows electrodes with lithiophilic nature to syphon molten Li•The composite Li electrode can cycle without dendrite growth or volume change•The composite Li can match Li-containing (LiFePO4) and Li-free (sulfur) cathodes
With the rapid development of electric vehicles and portable electronics such as mobile phones and laptops, the widely used lithium (Li)-ion batteries are having many difficulties in meeting the growing demands for high-energy-density energy-storage systems. Li metal, with an ultrahigh theoretical specific capacity of 3,860 mAh g−1 and the lowest negative electrochemical potential (−3.040 V versus standard hydrogen electrode), has become one of the most promising anode materials for next-generation batteries. Unfortunately, the practical application of Li metal anode has been hindered by its low cycling efficiency, short lifespan, and potential safety hazards. Herein we propose a Li-containing composite electrode based on coralloid carbon fibers that exhibited extraordinary electrochemical performance in full cells of Li-S and Li-LiFePO4 batteries. Such proof of concept on Li-infused structured electrodes sheds fresh light on the dendrite-free plating of Li metal anodes in working rechargeable batteries.
Lithium (Li) metal is among the most promising anode materials for next-generation high-energy-density batteries. However, both dendrite growth and unstable solid electrolyte interphases have hindered its practical applications. Herein, we propose a coralloid carbon fiber-based composite lithium anode, which is an initially Li-containing structured anode. Such electrode design renders dendrite-free morphology during repeated stripping/plating cycles and extraordinary electrochemical performance in Li-LiFePO4 and Li-sulfur cells.
The prognostic value and clinical relevance of tertiary lymphoid structures (TLSs) in intrahepatic cholangiocarcinoma (iCCA) remain unclear. Thus, we aimed to investigate the prognostic value and ...functional involvement of TLSs in iCCA.
We retrospectively included 962 patients from 3 cancer centers across China. The TLSs at different anatomic subregions were quantified and correlated with overall survival (OS) by Cox regression and Kaplan-Meier analyses. Multiplex immunohistochemistry (mIHC) was applied to characterize the composition of TLSs in 39 iCCA samples.
A quaternary TLS scoring system was established for the intra-tumor region (T score) and peri-tumor region (P score) respectively. T scores positively correlated with favorable prognosis (p <0.001), whereas a high P score signified worse survival (p <0.001). mIHC demonstrated that both T follicular helper and regulatory T cells were significantly increased in intra-tumoral TLSs compared to peri-tumoral counterparts (p <0.05), and regulatory T cell frequencies within intra-tumoral TLSs were positively associated with P score (p <0.05) rather than T score. Collectively, the combination of T and P scores stratified iCCAs into 4 immune classes with distinct prognoses (p <0.001) that differed in the abundance and distribution pattern of TLSs. Patients displaying an immune-active pattern had the lowest risk, with 5-year OS rates of 68.8%, whereas only 3.4% of patients with an immune-excluded pattern survived at 5 years (p <0.001). The C-index of the immune class was statistically higher than the TNM staging system (0.73 vs. 0.63, p <0.001). These results were validated in an internal and 2 external cohorts.
The spatial distribution and abundance of TLSs significantly correlated with prognosis and provided a useful immune classification for iCCA. T follicular helper and regulatory T cells may play a critical role in determining the functional orientation of spatially different TLSs.
Tertiary lymphoid structures (TLSs) are associated with favorable prognosis in a number of cancers. However, their role in intrahepatic cholangiocarcinoma (iCCA) remains unclear. Herein, we comprehensively evaluated the spatial distribution, abundance, and cellular composition of TLSs in iCCA, and revealed the opposite prognostic impacts of TLSs located within or outside the tumor. This difference could be mediated by the different immune cell subsets present within the spatially distinct TLSs. Based on our analysis, we were able to stratify iCCAs into 4 immune subclasses associated with varying prognoses.
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•Tertiary lymphoid structures (TLSs) within and outside the tumor have opposite prognostic impacts on patients with iCCA.•The heterogeneous distribution of Tfh and Treg cells within distinct TLSs might be a determinant of their functional state.•The geographic integration of TLSs stratified iCCAs into 4 immune subclasses with distinct clinical outcomes.
Cisplatin-based concurrent chemoradiotherapy is currently considered to be the standard treatment regimen for patients with advanced nasopharyngeal carcinoma, but has well known side-effects such as ...gastrointestinal reactions, nephrotoxicity, and ototoxicity. Nedaplatin was developed to decrease the toxic effects induced by cisplatin, and in this trial we assessed whether a nedaplatin-based concurrent chemoradiotherapy regimen was non-inferior to a cisplatin-based regimen in patients with locoregional, stage II–IVB nasopharyngeal carcinoma.
We did an open-label, non-inferiority, phase 3, randomised, controlled trial at two centres in China. Patients aged 18–65 years with non-keratinising stage II–IVB (T1–4N1–3 or T3–4N0) nasopharyngeal carcinoma, a Karnofsky score of at least 70, and adequate haematological, renal, and hepatic function were randomly assigned (1:1) to receive intravenously either nedaplatin 100 mg/m2 or cisplatin 100 mg/m2 on days 1, 22, and 43 for three cycles concurrently with intensity-modulated radiotherapy. Randomisation was done manually using a computer-generated random number code and patients were stratified by treatment centre and clinical stage. Patients and clinicians were not masked to treatment allocation. The primary endpoint was progression-free survival at 2 years; non-inferiority was shown if the upper limit of the 95% CI for the difference in 2-year progression-free survival between the two groups did not exceed 10%. Analyses were by both intention to treat and per protocol, including all patients who received at least one complete cycle of chemotherapy. This trial is registered with ClinicalTrials.gov, number NCT01540136, and is currently in follow-up.
Between Jan 16, 2012, and July 16, 2014, we randomly assigned 402 patients to nedaplatin-based (n=201) or cisplatin-based (n=201) concurrent chemoradiotherapy. In the intention-to-treat population, 2-year progression-free survival was 89·9% (95% CI 85·8–94·0) in the cisplatin group and 88·0% (83·5–94·5) in the nedaplatin group, with a difference of 1·9% (95% CI −4·2 to 8·0; pnon-inferiority=0·0048). In the per-protocol analysis (cisplatin group, n=197; nedaplatin group, n=196), 2-year progression-free survival was 89·7% (95% CI 85·4–94·0) in the cisplatin group and 88·7% (84·2–94·5) in the nedaplatin group, with a difference of 1·0% (95% CI −5·2 to 7·0; pnon-inferiority=0·0020). A significantly higher frequency of grade 3 or 4 vomiting (35 18% of 198 in the cisplatin group vs 12 6% of 200 in the nedaplatin group, p<0·0001), nausea (18 9% vs four 2%, p=0·0021), and anorexia (53 27% vs 26 13%, p=0·00070) was observed in the cisplatin group compared with the nedaplatin group. 11 (6%) patients in the nedaplatin group had grade 3 or 4 thrombocytopenia compared with four (2%) in the cisplatin group (p=0·065). Patients in the cisplatin group had a higher frequency of any grade or grade 3 or 4 late auditory or hearing toxicities than did patients in the nedaplatin group (grade 3 or 4: three 2% in the nedaplatin group vs 11 6% in the cisplatin group, p=0·030). No patients died from treatment-related causes.
Our findings show that nedaplatin-based concurrent chemoradiotherapy represents an alternative doublet treatment strategy to cisplatin-based concurrent chemoradiotherapy for patients with locoregional, advanced nasopharyngeal carcinoma. Further investigations are needed to explore the potential use of this treatment as induction or adjuvant chemotherapy or in combination with other agents.
National Key R&D Program of China, National Natural Science Foundation of China, Sun Yat-sen University Clinical Research 5010 Program, Sci-Tech Project Foundation of Guangzhou City, National Key Basic Research Program of China, Special Support Plan of Guangdong Province, Sci-Tech Project Foundation of Guangdong Province, Health & Medical Collaborative Innovation Project of Guangzhou City, National Science & Technology Pillar Program during the Twelfth Five-year Plan Period, PhD Start-up Fund of Natural Science Foundation of Guangdong Province, Cultivation Foundation for the Junior Teachers in Sun Yat-sen University, and Fundamental Research Funds for the Central Universities.
Graphene quantum dots (GQDs) have attracted tremendous research interest due to the unique properties associated with both graphene and quantum dots. Here, a new application of GQDs as ideal ...electrode materials for supercapacitors is reported. To this end, a GQDs//GQDs symmetric micro‐supercapacitor is prepared using a simple electro‐deposition approach, and its electrochemical properties in aqueous electrolyte and ionic liquid electrolyte are systematically investigated. The results show that the as‐made GQDs micro‐supercapacitor has superior rate capability up to 1000 V s−1, excellent power response with very short relaxation time constant (τ0 = 103.6 μs in aqueous electrolyte and τ0 = 53.8 μs in ionic liquid electrolyte), and excellent cycle stability. Additionally, another GQDs//MnO2 asymmetric supercapacitor is also built using MnO2 nanoneedles as the positive electrode and GQDs as the negative electrode in aqueous electrolyte. Its specific capacitance and energy density are both two times higher than those of GQDs//GQDs symmetric micro‐supercapacitor in the same electrolyte. The results presented here may pave the way for a new promising application of GQDs in micropower suppliers and microenergy storage devices.
Graphene quantum dots (GQDs)‐based micro‐supercapacitors are prepared using a simple eletrodeposition approach and their electrochemical properties in aqueous and ionic liquid electrolytes are studied. The GQDs‐based micro‐supercapacitors exhibit superior rate capability, high power response capability, and excellent cyclic stability
Abstract
In this work, commercial anatase TiO
2
powders were modified using ultrathin Fe
2
O
3
layer by atomic layer deposition (ALD). The ultrathin Fe
2
O
3
coating having small bandgap of 2.20 eV ...can increase the visible light absorption of TiO
2
supports, at the meantime, Fe
2
O
3
/TiO
2
heterojunction can effectively improve the lifetime of photogenerated electron–hole pairs. Results of ALD Fe
2
O
3
modified TiO
2
catalyst, therefore, showed great visible light driven catalytic degradation of methyl orange compared to pristine TiO
2
. A 400 cycles of ALD Fe
2
O
3
(~ 2.6 nm) coated TiO
2
powders exhibit the highest degradation efficiency of 97.4% in 90 min, much higher than pristine TiO
2
powders of only 12.5%. Moreover, an ultrathin ALD Al
2
O
3
(~ 2 nm) was able to improve the stability of Fe
2
O
3
-TiO
2
catalyst. These results demonstrate that ALD surface modification with ultrathin coating is an extremely powerful route for the applications in constructing efficient and stable photocatalysts.
The new shoots of the albino tea cultivar 'Anji Baicha' are yellow or white at low temperatures and turn green as the environmental temperatures increase during the early spring. 'Anji Baicha' ...metabolite profiles exhibit considerable variability over three color and developmental stages, especially regarding the carotenoid, chlorophyll, and theanine concentrations. Previous studies focused on physiological characteristics, gene expression differences, and variations in metabolite abundances in albino tea plant leaves at specific growth stages. However, the molecular mechanisms regulating metabolite biosynthesis in various color and developmental stages in albino tea leaves have not been fully characterized.
We used RNA-sequencing to analyze 'Anji Baicha' leaves at the yellow-green, albescent, and re-greening stages. The leaf transcriptomes differed considerably among the three stages. Functional classifications based on Gene Ontology enrichment and Kyoto Encyclopedia of Genes and Genomes enrichment analyses revealed that differentially expressed unigenes were mainly related to metabolic pathways, biosynthesis of secondary metabolites, phenylpropanoid biosynthesis, and carbon fixation in photosynthetic organisms. Chemical analyses revealed higher β-carotene and theanine levels, but lower chlorophyll a levels, in the albescent stage than in the green stage. Furthermore, unigenes involved in carotenoid, chlorophyll, and theanine biosyntheses were identified, and the expression patterns of the differentially expressed unigenes in these biosynthesis pathways were characterized. Through co-expression analyses, we identified the key genes in these pathways. These genes may be responsible for the metabolite biosynthesis differences among the different leaf color and developmental stages of 'Anji Baicha' tea plants.
Our study presents the results of transcriptomic and biochemical analyses of 'Anji Baicha' tea plants at various stages. The distinct transcriptome profiles for each color and developmental stage enabled us to identify changes to biosynthesis pathways and revealed the contributions of such variations to the albino phenotype of tea plants. Furthermore, comparisons of the transcriptomes and related metabolites helped clarify the molecular regulatory mechanisms underlying the secondary metabolic pathways in different stages.
Celotno besedilo
Dostopno za:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
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