ABSTRACT
Quasi-2D perovskites have attracted much attention in perovskite photovoltaics due to their excellent stability. However, their photoelectric conversion efficiency (PCE) still lags 3D counterparts, particularly with high short-circuit current (JSC) loss. The quantum confinement effect is pointed out to be the sole reason, which introduces widened bandgap and poor exciton dissociation, and undermines the light capture and charge transport. Here, the gradient incorporation of formamidinium (FA) cations into quasi-2D perovskite is proposed to address this issue. It is observed that FA prefers to incorporate into the larger n value phases near the film surface compared to the smaller n value phases in the bulk, resulting in a narrow bandgap and gradient structure within the film. Through charge dynamic analysis using in situ light-dark Kelvin probe force microscopy and transient absorption spectroscopy, it is demonstrated that incorporating 10% FA significantly facilitates efficient charge transfer between low n-value phases in the bulk and high n-value nearby film surface, leading to reduced charge accumulation. Ultimately, the device based on (AA)2(MA0.9FA0.1)4Pb5I16, where AA represents n-amylamine renowned for its exceptional environmental stability as a bulky organic ligand, achieves an impressive power conversion efficiency (PCE) of 18.58% and demonstrates enhanced illumination and thermal stability.
ABSTRACT
Dopant-free hole transporting materials (HTMs) is significant to the stability of perovskite solar cells (PSCs). Here, we developed a novel star-shape arylamine HTM, termed Py-DB, with a pyrene core and carbon-carbon double bonds as the bridge units. Compared to the reference HTM (termed Py-C), the extension of the planar conjugation backbone endows Py-DB with typical intermolecular π-π stacking interactions and excellent solubility, resulting in improved hole mobility and film morphology. In addition, the lower HOMO energy level of the Py-DB HTM provides efficient hole extraction with reduced energy loss at the perovskite/HTM interface. Consequently, an impressive power conversion efficiency (PCE) of 24.33 % was achieved for dopant-free Py-DB-based PSCs, which is the highest PCE for dopant-free small molecular HTMs in n-i-p configured PSCs. The dopant-free Py-DB-based device also exhibits improved long-term stability, retaining over 90 % of its initial efficiency after 1000â h exposure to 25 % humidity at 60 °C. These findings provide valuable insights and approaches for the further development of dopant-free HTMs for efficient and reliable PSCs.
ABSTRACT
The development of novel polymer dielectrics with enhanced dielectric performance is a great challenge for application of film capacitors in modern electronics and electrical systems. Herein, an innovative approach of chemical vapor deposition polymerization technology is proposed to prepare the all-organic sandwich structured parylene/polyimide/parylene (Py/PI/Py) composite films by employing poly(chloro-para-xylylene) (parylene C) as the outer layers and polyimide (PI) as the inner layer. The Py/PI/Py composites exhibit superior thermal resistance and outstanding mechanical properties. Moreover, thanks to the interfacial effect which contributes to reinforcing the dielectric response and the thickness effect which facilitates improving the breakdown strength, the dielectric performance of Py/PI/Py composites has been enhanced significantly. Accordingly, dielectric constant of 4.52-5.09, dissipation factor of 0.21-1.01%, and breakdown strength of 307-460 MV m-1 are achieved. Besides, notable energy storage performance is also obtained in Py/PI/Py composite dielectrics. Consequently, this novel application of chemical vapor deposition polymerization method in preparing all-organic multilayered polymer composite films with sandwich structure shows promising potential in film capacitor applications in harsh conditions.
Subject(s)
Polymers , Xylenes , Electricity , Electronics , GasesABSTRACT
BACKGROUND: Anxiety is common in older patients suffering from lumbar disc herniation. Postoperative delirium is related to poor prognosis. But the relationship between preoperative anxiety and postoperative delirium among older patients undergoing elective surgery for lumbar disc herniation is not clear. AIMS: The study aimed to investigate if preoperative anxiety is an independent risk factor of postoperative delirium among older patients undergoing elective surgery for lumbar disc herniation. METHODS: The medical records of 1290 patients undergoing elective surgery for lumbar disc herniation at a single institution from 2016 through 2021 were reviewed. Of 863 eligible patients, 225 (26.1%) patients had been diagnosed with anxiety by a board-certified psychiatrist and constituted the Anxiety group; the remaining 638 patients constituted the no-anxiety group. The demographics, baseline, operative variable and postoperative complications were collected and compared between the two groups. The primary outcome of this study was the incidence of delirium, according to the Diagnostic and Statistical Manual of Mental Disorders-Fifth Edition, during a hospital stay after surgery for lumbar disc herniation. The relationship between anxiety and postoperative delirium was determined through multivariate logistic regression analysis. RESULTS: The demographics and comorbidity were similar between the two groups, except for age, sex, alcohol use and cerebrovascular disease. The operative variables were different between the two groups. The incidence of postoperative complications other than postoperative delirium was also similar between the two groups. In total, 86 patients (9.97%) had an episode of postoperative delirium, with anxiety group patients experiencing approximately a twofold higher rate (15.6% vs 7.99%). In a multivariate logistic regression analysis, anxiety was an independent predictor of postoperative delirium in older patients undergoing elective surgery for lumbar disc herniation (OR 2.228, 95% CI 1.494-3.416, p = 0.009). CONCLUSION: This study suggests that anxiety is an independent risk factor of postoperative delirium among older patients undergoing elective surgery for lumbar disc herniation. Preoperative anxiety assessment can help to identify older patients at high risk of postoperative delirium and facilitate perioperative management of older patients undergoing elective surgery for lumbar disc herniation.
Subject(s)
Emergence Delirium , Intervertebral Disc Displacement , Humans , Aged , Intervertebral Disc Displacement/complications , Intervertebral Disc Displacement/surgery , Intervertebral Disc Displacement/epidemiology , Lumbar Vertebrae/surgery , Anxiety , Postoperative Complications/epidemiology , Postoperative Complications/etiology , Risk FactorsABSTRACT
Hole transport materials (HTMs) are a key component of perovskite solar cells (PSCs). The small molecular 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenyl)-amine-9,9'-spirobifluorene (spiro-OMeTAD, termed "Spiro") is the most successful HTM used in PSCs, but its versatility is imperfect. To improve its performance, we developed a novel spiro-type HTM (termed "DP") by substituting four anisole units on Spiro with 4-methoxybiphenyl moieties. By extending the π-conjugation of Spiro in this way, the HOMO level of the HTM matches well with the perovskite valence band, enhancing hole mobility and increasing the glass transition temperature. DP-based PSC achieves high power conversion efficiencies (PCEs) of 25.24 % for small-area (0.06â cm2 ) devices and 21.86 % for modules (designated area of 27.56â cm2 ), along with the certified efficiency of 21.78 % on a designated area of 27.86â cm2 . The encapsulated DP-based devices maintain 95.1 % of the initial performance under ISOS-L-1 conditions after 2560â hours and 87 % at the ISOS-L-3 conditions over 600â hours.
ABSTRACT
We used UV-guided method to isolate and identify 12 secondary metabolites from Meehania fargesii var. Radicans for the first time, including eight triterpenoids (1-8), two phenylpropanoid derivatives (9-10) and two flavone glycosides (11-12). Their structures were identified by NMR spectroscopic methods, as well as literature comparison. The identified compounds and positive drugs (amoxicillin, omeprazole and clarithromycin) were further analyzed for their in silico docking interactions with HtrA using igemdock. Docking studies revealed the high binding affinity of phytochemicals at significant sites with HtrA, compounds 11 and 12 exhibiting stronger binding ability than standard drug, 1 and 3-10 demonstrating comparable docking capacity to standard drugs. The chemotaxonomic relationships were carried out to exploring the possibilities of other medicinal plants against Hp-induced gastric carcinoma. The results demonstrated there are closely chemotaxonomic similarity among several genera of the Lamiaceae family as well as among Lamiaceae, Actinidiaceae and Rosaceae families, indicating a similar chemical compositions and anti-Hp-induces gastric carcinoma activity among them.
Subject(s)
Carcinoma , Helicobacter Infections , Helicobacter pylori , Lamiaceae , Anti-Bacterial Agents/pharmacology , Carcinoma/drug therapy , Helicobacter Infections/drug therapy , Humans , Molecular Docking Simulation , Phytochemicals/pharmacologyABSTRACT
Using a gravity-like approach, we study how COVID-19 deaths and lockdown policies affected countries' imports from China during 2020. We find that a country's own COVID-19 deaths and lockdowns significantly reduced its imports from China, suggesting that the negative demand effects prevailed over the negative supply effects of the pandemic. On the contrary, COVID-19 deaths in the main trading partners of a country (excluding China) induce more imports from China, partially offsetting countries' own effects. The net effect of moving from the pre-pandemic situation to another where the main variables are evaluated at their 2020 mean is, on average, a reduction of nearly 10% in imports from China. There is also significant heterogeneity. For example, the negative own effects of the pandemic vanish when we restrict the sample to medical goods and are significantly mitigated for products with a high 'work-from-home' share or a high contract intensity for products exported under processing trade and for capital goods. We also find that deaths and lockdowns in previous months tend to increase current imports from China, partially offsetting the contemporaneous trade loss, suggesting that trade is not simply 'destroyed,' but partially 'postponed'.
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Atomistic molecular dynamics simulations are performed to explore the interaction between two alkylthiol-capped tetrahedral gold nanocrystals (NCs) in a vacuum. The results highlight the influential role of the effective softness of the ligated NCs, i.e. the ratio of the ligand length to the core size. For sufficiently large softness, the relatively long ligand molecules round the shape of the NCs, causing their interaction to be nearly isotropic. For small effective softness, the relative shortness of the ligand molecules leads to a geometrically asymmetric morphology of the NCs, so that the interaction is orientation-dependent and is the strongest when the two NCs face each other with (111) facets. These findings are helpful for the understanding of interaction and structure formation in superlattices self-assembled from non-spherical ligand-capped NCs.
ABSTRACT
Topological defect nucleation and boundary branching in crystal growth on a curved surface are two typical elastic instabilities driven by curvature induced stress, and have usually been discussed separately in the past. In this work they are simultaneously considered during crystal growth on a sphere. Phase diagrams with respect to sphere radius, size, edge energy and stiffness of the crystal for the equilibrium crystal morphologies are achieved by theoretical analysis and validated by Brownian dynamics simulations. The simulation results further demonstrate the detail of morphological evolution governed by these two different stress relaxation modes. Topological defect nucleation and boundary branching not only compete with each other but also coexist in a range of combinations of factors. Clarification of the interaction mechanism provides a better understanding of various curved crystal morphologies for their potential applications.
ABSTRACT
Atomistic molecular dynamics simulations are performed to study the thermal stability of bulk superlattices consisting of alkylthiol-coated gold nanocrystals. Using nanocrystals passivated by dodecanethiol chains, we show that the gold superlattice possesses a remarkable high-temperature stability, in agreement with experiment. When heated from room temperature, the superlattice expands slightly at lower temperature (<500 K) and then exhibits a considerable lattice contraction above 500 K, while maintaining the intact crystal structure up to 710 K. Once the temperature increases above 720 K, the gold superlattice becomes structurally unstable due to the local sintering of adjacent nanocrystals. Continuous heating to 750 K drives a large number of gold nanocrystals to coalesce and finally results in a tremendous destruction of the superstructure. The structural change and instability of superlattice are mainly attributed to the ligand desorption from nanocrystal surface induced by the variation in temperature. Furthermore, longer ligand length can effectively improve the thermal stability of gold superlattices. These findings are expected to provide a deep microscopic understanding of the thermal stability of superlattice materials.
ABSTRACT
Atomistic molecular dynamics simulations are performed to study the potential of mean force (PMF) between two asymmetric gold nanocrystals (NCs) capped by alkylthiols in a vacuum. We systematically investigate the dependence of the PMF on the sizes and capping ligand lengths of two NCs. The results show that the potential well depth scales linearly with increasing total length of two capping ligands on asymmetric dimers, but it hardly depends on the NC size. The predicted equilibrium distance between two asymmetric NCs grows significantly and linearly with the total size of two NCs and exhibits only a slight increase with increasing total ligand length. These findings are explained in terms of the amount of ligand interdigitation between NC surfaces as well as its alterations caused by the change in ligand length and NC size. Furthermore, we introduce a simple formula to estimate the equilibrium distance of two asymmetric NCs. On the basis of the computed PMFs, we propose an empirical two-body potential between asymmetric capped gold NCs.
ABSTRACT
Three heteroleptic ruthenium complexes, RC-15, RC-16 and RC-22, with sulfur- or oxygen-containing electron-donor, phenylpyridine-based ancillary ligands, are synthesized. The influence of the different electron donors-the acyclic electron donors methylthio and methoxyl, and the cyclic electron donor methylenedioxy-on the photophysical and electrochemical behavior in dye sensitizers and photovoltaic performance in DSSCs are investigated. Compared to the conventional dye N3, all the dyes demonstrate superior performance in the form of molar absorptivity, photocurrent density (J(SC)) and conversion efficiency (η). The DSSCs based on RC-15 and RC-16, with only a two-atom change in the acyclic electron donor, exhibit analogous photovoltaic performance (9.28% for RC-15 and 9.32% for RC-16). The highest photocurrent density (19.06 mA cm(-2)) and conversion efficiency (9.74%) are recorded for RC-22, which contains the cyclic electron donor. Transient absorption (TAS) and time-resolved photoluminescence (TRPL) measurements are carried out to investigate the sensitizers' regeneration and the behavior of excited electron decay kinetics. Furthermore, electrochemical impedance spectroscopy (EIS) is operated to explain the charge recombination and the electron lifetime. These consequences reveal substantial dependences on the different configurations of the electron-donor ancillary ligands.
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Isotopic signatures offer new methods, approaches, and perspectives for exploring the ecological adaptability and functions of plants. We examined pattern differences in the isotopic signatures (δ 13C, δ 15N, δ 34S) of Spartina alterniflora across varying plant life-death status along geographic clines. We extracted 539 sets of isotopic data from 57 publications covering 267 sites across a latitude range of over 23.8° along coastal wetlands. Responses of isotopic signatures to climate drivers (MAT and MAP) and the internal relationships between isotopic signatures were also detected. Results showed that the δ 13C, δ 15N, and δ 34S of S. alterniflora were -13.52 ± 0.83, 6.16 ± 0.14, and 4.01 ± 6.96, with a range of -17.44 to -11.00, -2.40 to 15.30, and -9.60 to 15.80, respectively. The latitudinal patterns of δ 13C, δ 15N, and δ 34S in S. alterniflora were shaped as a convex curve, a concave curve, and an increasing straight line, respectively. A decreasing straight line for δ 13C within the ranges of MAT was identified under plant life status. Plant life-death status shaped two nearly parallel decreasing straight lines for δ 34S in response to MAT, resulting in a concave curve of δ 34S for live S. alterniflora in response to MAP. The δ 15N of S. alterniflora significantly decreased with increasing δ 13C of S. alterniflora, except for plant death status. The δ 13C, δ 15N, and δ 34S of S. alterniflora are consistent with plant height, stem diameter, leaf traits, etc, showing general latitudinal patterns closely related to MAT. Plant life-death status altered the δ 15N (live: 6.55 ± 2.23; dead: -2.76 ± 2.72), latitudinal patterns of S. alterniflora and their responses to MAT, demonstrating strong ecological plasticity and adaptability across the geographic clines. The findings help in understanding the responses of latitudinal patterns of the δ 13C, δ 15N, and δ 34S isotope signatures of S. alterniflora in response plant life-death status, and provide evidence of robust ecological plasticity and adaptability across geographic clines.
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The top surface of the perovskite layer and the interface with the electron transporting layer play a key role in influencing the performance and operational stability of inverted perovskite solar cells (PSCs). A deficient or ineffective surface passivation strategy at the perovskite/electron transport layer interface can significantly impact the efficiency and scalability of PSCs. This study introduces phenyl dimethylammonium iodide (PDMAI2) as a passivation ligand that exhibits improved chemical and field-effect passivation at the perovskite/C60 interface. It was found that PDMAI2 not only passivates surface defects and suppresses recombination through robust coordination but also repels minority carriers and reduces contact-induced interface recombination. The approach leads to a twofold reduction in defect densities and photoluminescence quantum yield loss. This approach enabled high power conversion efficiencies (PCEs) of 25.3% for small-area (0.1 cm2) and 23.8% for large-area (1 cm2) inverted PSCs. Additionally, PDMAI2 passivation enabled PSCs to demonstrate steady operation at 65 °C for >1200 hours in an ambient environment.
ABSTRACT
In perovskite solar cells (PSCs), defects in the interface and mismatched energy levels can damage the device performance. Improving the interface quality is an effective way to achieve efficient and stable PSCs. In this work, a multifunctional dye molecule, named ThPCyAc, was designed and synthesized to be introduced in the perovskite/HTM interface. On one hand, various functional groups on the acceptor unit can act as Lewis base to reduce defect density and suppress nonradiative combinations. On the other hand, the stepwise energy-level alignment caused by ThPCyAc decreases the accumulation of interface carriers for facilitating charge extraction and transmission. Therefore, based on the ThPCyAc molecule, the devices exhibit elevated open-circuit voltage and fill factor, resulting in the best power conversion efficiency (PCE) of 23.16%, outperforming the control sample lacking the interface layer (PCE = 21.49%). Excitingly, when attempting to apply it as a self-assembled layer in inverted devices, ThPCyAc still exhibits attractive behavior. It is worth noting that these results indicate that dye molecules have great potential in developing multifunctional interface materials to obtain higher-performance PSCs.
ABSTRACT
The orthogonal structure of the widely used hole transporting material (HTM) 2,2',7,7'-tetrakis(N, N-di-p-methoxyphenylamino)-9,9'-spirobifluorene (Spiro-OMeTAD) imparts isotropic conductivity and excellent film-forming capability. However, inherently weak intra- and inter-molecular π-π interactions result in low intrinsic hole mobility. Herein, a novel HTM, termed FTPE-ST, with a twist conjugated dibenzo(g,p)chrysene core and coplanar 3,4-ethylenedioxythiophene (EDOT) as extended donor units, is designed to enhance π-π interactions, without compromising on solubility. The three-dimensional (3D) configuration provides the material multi-direction charge transport as well as excellent solubility even in 2-methylanisole, and its large conjugated backbone endows the HTM with a high hole mobility. Moreover, the sulfur donors in EDOT units coordinate with lead ions on the perovskite surface, leading to stronger interfacial interactions and the suppression of defects at the perovskite/HTM interface. As a result, perovskite solar cells (PSCs) employing FTPE-ST achieve a champion power conversion efficiency (PCE) of 25.21% with excellent long-time stability, one of the highest PCEs for non-spiro HTMs in n-i-p PSCs. In addition, the excellent film-forming capacity of the HTM enables the fabrication of FTPE-ST-based large-scale PSCs (1.0 cm2) and modules (29.0 cm2), which achieve PCEs of 24.21% (certificated 24.17%) and 21.27%, respectively.
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Compared with the aquatic ecosystem destruction caused by rapid urban development, substantial ecological restoration usually requires long periods and is a challenging process. Although river ecological restoration has been successful in different regions, the relationship between biodiversity, water quality, and effective measures applicable to developing countries remains poorly understood. This study was conducted in the Dasha River in Shenzhen city, one of the fastest-growing cities in China. The rehabilitation measures were sorted out in four phases to study the impact on water quality and biodiversity. In response, three campaigns were carried out to take phytoplankton, zooplankton, and benthos samples within the last three engineering stages, in 2007, 2012, and 2021. Synchronized investigations of water quality were conducted monthly from 2006 to 2021. Our analysis showed that the biodiversity of benthos has improved in recent years, which marks a turnaround for the aquatic ecological environment. According to the Hilsenhoff family biotic index (FBI), the water quality level in the 2021 campaign was promoted to "Good" in the downstream and "Fair" in the upper and middle streams. By analyzing Pearson's correlations between response ratios of water quality parameters and the Shannon-Wiener index of phytoplankton, zooplankton, and benthos, we concluded that biodiversity is significantly related to water quality. Specifically, the biodiversity of zooplankton is associated with ammonia nitrogen (NH3-N) (R2 = - 0.77, P < 0.05), and benthos diversity is strongly negatively correlated with NH3-N, total nitrogen, chemical oxygen demand, and biochemical oxygen demand (R2 ≥ -0.82, P < 0.01). Despite the temporary negative impact of along-river interception on aquatic organisms in the campaign of 2012, the measures quickly and effectively improved water quality, which is the foundation for biodiversity improvement in 2021. This study provides insights into relationships among biodiversity, water quality, and regulation projects and can offer a reference for selecting aquatic ecosystem restoration measures in developing areas.
Subject(s)
Ecosystem , Zooplankton , Animals , Hong Kong , Macau , Cities , China , Phytoplankton , Nitrogen/analysisABSTRACT
17ß-estradiol is abused in the food industry. Excess 17ß-estradiol can disturb the endocrine system or cause many diseases including obesity, diabetes, cardiac-cerebral vascular disease, and cancers in the human body. A "turn-on" fluorescence resonance energy transfer (FRET) aptasensor based on carbon dots (CDs) and gold nanoparticles (AuNPs) was developed for the detection of 17ß-estradiol. A thiol-modified oligonucleotide was conjugated to AuNPs and amino modified oligonucleotide was linked to CDs. The 17ß-estradiol aptamer was hybridized with the two oligonucleotides, shortening the distance between CDs and AuNPs. With 360 nm UV light excitation, FRET occurred between CDs and AuNPs. The system was "turn-off". When 17ß-estradiol was detected, the aptamer specifically bound to 17ß-estradiol, and the FRET system was destroyed, leading to the "turn-on" phenomenon. The fluorescence intensity recovery was detected in the concentration range of 400 pM to 5.5 µM. The limit of detection (LOD) was 245 pM. The FRET aptasensor demonstrated good selectivity for 17ß-estradiol detection. Reasonable spiked recoveries were obtained in sea salt samples. It showed the potential for estrogen detection in food safety and environmental applications.
ABSTRACT
Dielectrics of the polymer-matrix composite are considered to present combined advantages from both the polymer matrix and inorganic fillers. However, the breakdown strength, as well as energy density, is not effectively enhanced due to the poor compatibility between the organic and inorganic components. Herein, polymer composites derived from polystyrene (PS) and barium titanate (BTO) are proposed and beneficial interface modification by poly(styrene-co-maleic anhydride) (PS-co-mah) is conducted to improve compatibility between the inorganic filler and polymer matrix. The results show that the BTO@PS-co-mah/PS composites, in which the interfacial layer of PS-co-mah would undergo chemical reactions with the aminated BTO and blend PS matrix with excellent physical compatibility, exhibit enhanced breakdown strength and declined dielectric loss compared with both pure PS and BTO/PS without interfacial modulation. Particularly, the BTO@PS-co-mah/PS composite with 5 wt% filler content indicates optimized performance with an E b of 507 MV m-1 and tan δ of 0.085%. It is deduced that the deep energy traps introduced by the PS-co-mah layer would weaken the local electric field and suppress the space charge transporting so as to optimize the performance of composites. Consequently, the interfacial-modified BTO@PS-co-mah/PS would present great potential for applications, such as film capacitors.
ABSTRACT
Organizational resilience is vital to the survival and thriving of enterprises, especially during the COVID-19 pandemic. Although there has been an increasing interest in organizational resilience, the effects from the entrepreneur perspective receive scant attention. Based on upper echelons theory (UET) and personality psychology, we propose a model in which entrepreneurial mindfulness and entrepreneurial resilience could influence organizational resilience of SMEs. We empirically analyzed a sample of 180 entrepreneurs managing small- and medium-sized enterprises (SMEs) in China during the COVID-19 pandemic, using SmartPLS software. The research findings indicated that entrepreneurial mindfulness is positively associated with organizational resilience and such relationship is partially mediated by entrepreneurial resilience. These findings convey important theoretical implications in this field of research as well as practical implications for SMEs in China or other countries with similar nature.