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1.
J Phys Chem Lett ; 15(19): 5259-5266, 2024 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-38721943

RESUMO

The inverted perovskite solar cells have drawn considerable attention owing to their low cost, good compatibility, and easy production processes. However, the device performance is still limited by some important factors, such as surface imperfections and interfacial nonradiative recombination losses. Here, N-acetylethylenediamine (N-AE) is introduced to bind to the surface of the perovskite film via an ammonia condensation reaction. This process creates a stable interfacial layer with n-type doping to enhance the open-circuit voltage (VOC). Moreover, during post-treatment, N-AE dissolves a portion of the perovskite on the surface, leading to perovskite recrystallization. This process enhances the surface quality of the perovskite film and reduces nonradiative recombination. As a result, the inverted perovskite solar cell exhibits a power conversion efficiency approaching 20%, with a rise in VOC from 0.96 to 1.05 V. More impressively, the unencapsulated devices display excellent stability at 85 °C annealing and retained 88% of the initial PCE for 816 h.

2.
Inorg Chem ; 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38776123

RESUMO

Metal halides have drawn great interest as luminescent materials and scintillators due to their outstanding optical properties. Exploring new types of phosphors with easy production processes, excellent photophysical properties, high light yields, and environmentally friendly compositions is crucial and quite challenging. Herein, a novel Mn(II)-based metal halide (4-BTP)2MnBr4 was produced using a facile solvent evaporation method, which exhibited a strong green emission peaking at 524 nm from the d-d transition of tetrahedral-coordinated Mn2+ ion and a near-unity quantum yield. The prepared white light-emitting diode device has a wide color gamut of 100.7% NTSC with CIE chromaticity coordinates of (0.32, 0.32). In addition, (4-BTP)2MnBr4 demonstrates excellent characteristics in X-ray scintillation, including a high light yield of 98 000 photons/MeV, a sensitive detection limit of 37.4 nGy/s, excellent resistance to radiation damage, and successful demonstration of X-ray imaging with high resolution at 21.3 lp/mm, revealing the potential for application in diagnostic X-ray medical imaging and industry radiation detection.

3.
Heliyon ; 10(7): e29062, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38601693

RESUMO

Background: The role of Ferroptosis in the course of sepsis-induced myopathy is yet unclear. The objective of our work is to identify key genes connected with Ferroptosis in sepsis-induced myopathy and investigate possible pharmaceutical targets related to this process. This research aims to provide new insights into the management of sepsis-induced myopathy. Methods: We got the GSE13205 dataset from the Gene Expression Omnibus (GEO) and extracted Ferroptosis-associated genes from the FerrDb database. After conducting a functional annotation analysis of these genes, we created a protein-protein interaction network using Cytoscape software to identify important genes. Subsequently, we employed CMap to investigate prospective pharmaceuticals that could target these crucial genes. Results: A total of 61 genes that are expressed differently (DEGs) have been found concerning Ferroptosis. These genes are involved in a wide range of biological functions, including reacting to signals from outside the cell and the availability of nutrients, programmed cell death, controlling apoptosis, and responding to peptides, chemical stressors, and hormones. The KEGG pathway study revealed that these pathways are involved in Ferroptosis, autophagy, P53 signaling, PI3K-Akt signaling, mTOR signaling, HIF-1 signaling, endocrine resistance, and different tumorigenic processes. In addition, we created a network that shows the simultaneous expression of important genes and determined the top 10 medications that have the potential to treat sepsis-induced myopathy. Conclusion: The bioinformatics research undertaken sheds insight into the probable role of Ferroptosis-associated genes in sepsis-induced myopathy. The identified critical genes show potential as therapeutic targets for treating sepsis-induced myopathy, offering opportunities for the development of tailored medicines.

4.
Small ; : e2309646, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38676330

RESUMO

The long-term stability of perovskite solar cells (PSCs) is still challenging for commercialization and mainly linked to the life span of perovskite films. Herein, a spontaneous compositional-interfacial co-modification strategy is developed based on the ion exchange reaction by introducing ammonium hexafluorophosphate (NH4PF6) into antisolvent to form gradient structures through a simple one-step solvent engineering. With the assistance of the ion exchange reaction, NH4PF6 forms a multifunctional structure to protect perovskite films from both internal and external factors for the exceptionally long-term stability of photovoltaics. The reason for this is linked to the high hydrophobicity of NH4PF6 for preventing H2O invasion, suppressing ion migration by forming hydrogen bonding, and reducing perovskite defects. The resulting unencapsulated devices show exceptionally long-term stability under standardized the International Summit on Organic Photovoltaic Stability (ISOS) protocols, with over 94%, 81%, and 83% retained power conversion efficiencies after aging tests under N2 (ISOS-D-1I), ambient air (ISOS-D-1), and 85 °C (ISOS-D-2I) for 14016, 2500, and 1248 h, respectively. These performances compare well with the state-of-the-art stability of inverted PSCs. Further investigations are conducted to study the evolution of macroscopic morphology and microscopic crystal structure in aged perovskite films, aiming to provide evidence supporting the aforementioned improvements in stability.

5.
Chem Sci ; 15(11): 3988-3995, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38487237

RESUMO

Na3Zr2Si2PO12 has been proven to be a promising electrolyte for solid-state sodium batteries. However, its poor conductivity prevents application, caused by the large ionic resistance created by the grain boundary. Herein, we propose an additional glass phase (Na-Ga-Si-P-O phase) to connect the grain boundary via Ga ion introduction, resulting in enhanced sodium-ion conduction and electrochemical performance. The optimized Na3Zr2Si2PO12-0.15Ga electrolyte exhibits Na+ conductivity of 1.65 mS cm-1 at room temperature and a low activation energy of 0.16 eV, with 20% newly formed glass phase enclosing the grain boundary. Temperature-dependent NMR line shapes and spin-lattice relaxation were used to estimate the Na self-diffusion and Na ion hopping. The dense glass-ceramic electrolyte design strategy and the structure-dynamics-property correlation from NMR, can be extended to the optimization of other materials.

6.
Sci Total Environ ; 918: 170689, 2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38320709

RESUMO

Gaseous carbon exchange at the water-air interface of rivers and lakes is an essential process for regional and global carbon cycle assessments. Many studies have shown that rivers surrounding urban landscapes can be hotspots for greenhouse gas (GHG) emissions. Here we investigated the variability of diffusive GHG (methane [CH4] and carbon dioxide [CO2]) emissions from rivers in different landscapes (i.e., urban, agricultural and mixed) and from lakes in Suzhou, a highly urbanized region in eastern China. GHG emissions in the Suzhou metropolitan water network followed a typical seasonal pattern, with the highest fluxes in summer, and were primarily influenced by temperature and dissolved oxygen concentration. Surprisingly, lakes were emission hotspots, with mean CH4 and CO2 fluxes of 2.80 and 128.89 mg m-2 h-1, respectively, translating to a total CO2-equivalent flux of 0.21 g CO2-eq m-2 d-1. The global warming potential of urban and mixed rivers (0.19 g CO2-eq m-2 d-1) was comparable to that for lakes, but about twice the value for agricultural rivers (0.10 g CO2-eq m-2 d-1). Factors related to the high GHG emissions in lakes included hypoxic water conditions and an adequate nutrient supply. Riverine CH4 emissions were primarily associated with the concentrations of total dissolved solids (TDS), ammonia­nitrogen and chlorophyll a. CO2 emissions in rivers were mainly closely related to TDS, with suitable conditions allowing rapid organic matter decomposition. Compared with other types of rivers, urban rivers had more available organic matter and therefore higher CO2 emissions. Overall, this study emphasizes the need for a deeper understanding of the impact of GHG emissions from different water types on global warming in rapidly urbanizing regions. Flexible management measures are urgently needed to mitigate CO2 and CH4 emissions more effectively in the context of the shrinking gap between urban and rural areas with growing socio-economic development.

7.
Intern Emerg Med ; 19(2): 511-521, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37740869

RESUMO

Acute gastrointestinal (GI) bleeding are potentially life-threatening conditions. Early risk stratification is important for triaging patients to the appropriate level of medical care and intervention. Patients admitted to intensive care unit (ICU) has a high mortality, but risk tool is scarce for these patients. This study aimed to develop and validate a risk score to improve the prognostication of death at the time of patient admission to ICU. We developed and internally validated a nomogram for mortality in patients with acute GI bleeding from the eICU Collaborative Research Database (eICU-CRD), and externally validated it in patients from the Medical Information Mart for Intensive Care III database (MIMIC-III) and Wuhan Tongji Hospital. The performance of the model was assessed by examining discrimination (C-index), calibration (calibration curves) and usefulness (decision curves). 4750 patients were included in the development cohort, with 1184 patients in the internal validation cohort, 1406 patients in the MIMIC-III validation cohort, and 342 patients in the Tongji validation cohort. The nomogram, which incorporated ten variables, showed good calibration and discrimination in the training and validation cohorts, yielded C-index ranged from 0.832 (95%CI 0.811-0.853) to 0.926 (95CI% 0.905-0.947). The nomogram-defined high-risk group had a higher mortality than the low-risk group (44.8% vs. 3.5%, P < 0.001; 41.4% vs 3.1%, P < 0.001;53.6% vs 7.5%, P < 0.001; 38.2% vs 4.2%, P < 0.001). The model performed better than the conventional Glasgow-Blatchford score, AIMS65 and the newer Oakland and Sengupta scores for mortality prediction in both the derivation and validation cohorts concerning discrimination and usefulness. Our nomogram is a reliable prognostic tool that might be useful to identify high-risk acute GI bleeding patients admitted to ICU.


Assuntos
Hemorragia Gastrointestinal , Hospitalização , Humanos , Prognóstico , Hemorragia Gastrointestinal/diagnóstico , Fatores de Risco , Unidades de Terapia Intensiva
8.
Front Optoelectron ; 16(1): 47, 2023 Dec 29.
Artigo em Inglês | MEDLINE | ID: mdl-38155231

RESUMO

Tin perovskites with exemplary optoelectronic properties offer potential application in lead-free perovskite solar cells. However, Sn vacancies and undercoordinated Sn ions on the tin perovskite surfaces can create deep-level traps, leading to non-radiative recombination and absorption of nucleophilic O2 molecules, impeding further device efficiency and stability. Here, in this study, a new additive of semicarbazide hydrochloride (SEM-HCl) with a N-C=O functional group was introduced into the perovskite precursor to fabricate high-quality films with a low concentration of deep-level trap densities. This, in turn, serves to prevent undesirable interaction between photogenerated carriers and adsorbed oxygen molecules in the device's operational environment, ultimately reducing the proliferation of superoxide entities. As the result, the SEM-HCl-derived devices show a peak efficiency of 10.9% with improved device stability. These unencapsulated devices maintain almost 100% of their initial efficiencies after working for 100 h under continuous AM1.5 illumination conditions.

9.
Adv Mater ; 35(47): e2301752, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37815114

RESUMO

Upscaling efficient and stable perovskite films is a challenging task in the industrialization of perovskite solar cells partly due to the lack of high-performance hole transport materials (HTMs), which can simultaneously promote hole transport and regulate the quality of perovskite films especially in inverted solar cells. Here, a novel HTM based on N-C = O resonance structure is designed for facilitating the modulation of the crystallization and bottom-surface defects of perovskite films. Benefiting from the resonance interconversion (N-C = O and N+ = C-O- ) in donor-resonance-donor (D-r-D) architecture and interactions with uncoordinated Pb2+ in perovskite, the resulting D-r-D HTM with two donor units exhibits not only excellent hole extraction and transport capacities, but also efficient crystallization modulation of perovskite for high-quality photovoltaic films in large area. The D-r-D HTM-based large-area (1.02 cm2 ) devices exhibit high power conversion efficiencies (PCEs) up to 21.0%. Moreover, the large-area devices have excellent photo-thermal stability, showing only a 2.6% reduction in PCE under continuous AM 1.5G light illumination at elevated temperature (≈65 °C) for over 1320 h without encapsulation.

10.
Inorg Chem ; 62(40): 16538-16546, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37737143

RESUMO

Organic-inorganic metal hybrid perovskites (OIHPs) have emerged as a promising class of materials for next-generation optoelectronic applications. However, the realization of red and near-infrared (NIR) room-temperature phosphorescence (RTP) in these materials remains limited. In this study, a very strong red RTP emission centered at 610 nm is achieved by doping Mn2+ ions into Cd-based 2D OIHPs. Notably, the optimized B-EACC:Mn2+ exhibited a high quantum yield of 44.11%, an ultralong lifetime of up to 378 ms, and excellent stability against high temperatures and various solvents, surpassing most reported counterparts of 2D OIHPs. Moreover, the B-EACC:Mn2+ can be used as a red emitter for coating an ultraviolet light-emitting diode chip, exhibiting an observable afterglow to the naked eye for approximately 4 s. In addition, the B-EACC:Mn2+ demonstrates interesting characteristics under X-ray excitation, exhibiting X-ray response at radiation doses in the range of 34.75-278 µGy s-1. This work suggests the infinite possibility of doping guest ions to realize red RTP in 2D OIHPs, promoting the development of long-persistent phosphorescent emitters for multifunctional light-emitting applications.

11.
Front Med (Lausanne) ; 10: 1249724, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37692780

RESUMO

Background: Persistent Inflammation, Immunosuppression, and Catabolism Syndrome (PIICS) is a significant contributor to adverse long-term outcomes in severe trauma patients. Objective: The objective of this study was to establish and validate a PIICS predictive model in severe trauma patients, providing a practical tool for early clinical prediction. Patients and methods: Adult severe trauma patients with an Injury Severity Score (ISS) of ≥16, admitted between October 2020 and December 2022, were randomly divided into a training set and a validation set in a 7:3 ratio. Patients were classified into PIICS and non-PIICS groups based on diagnostic criteria. LASSO regression was used to select appropriate variables for constructing the prognostic model. A logistic regression model was developed and presented in the form of a nomogram. The performance of the model was evaluated using calibration and ROC curves. Results: A total of 215 patients were included, consisting of 155 males (72.1%) and 60 females (27.9%), with a median age of 51 years (range: 38-59). NRS2002, ISS, APACHE II, and SOFA scores were selected using LASSO regression to construct the prognostic model. The AUC of the ROC analysis for the predictive model in the validation set was 0.84 (95% CI 0.72-0.95). The Hosmer-Lemeshow test in the validation set yielded a χ2 value of 14.74, with a value of p of 0.098. Conclusion: An accurate and easily implementable PIICS risk prediction model was established. It can enhance risk stratification during hospitalization for severe trauma patients, providing a novel approach for prognostic prediction.

12.
J Phys Chem Lett ; 14(38): 8638-8647, 2023 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-37728759

RESUMO

Two-dimensional (2D) metal halide perovskites with highly efficient ultralong room-temperature phosphorescence (URTP) are rare due to their uncertain structures and complicated intermolecular interactions. Herein, by varying the alkyl length of organic units, we synthesized two single-component 2D metal hybrid perovskites, i.e., B-MACC and B-EACC, with obvious URTP emission. In particular, B-EACC exhibits a green-yellow URTP emission with an ultralong lifetime (579 ms) and a high efficiency (14.86%). It is found that the molecular packing of B-EA+ cations because of the presence one more carbon in the alkyl chain affords strong hydrogen bonding and π-π stacking interactions, which immobilizes and reduces the triplet exciton quenching. Moreover, B-MACC and B-EACC with space-time dual-resolved characteristics can be utilized for dynamic information encryption and optical logic gate applications. This study is the first to disclose the relation between the characteristics of molecular packing and the resultant URTP of 2D metal hybrid perovskites, significantly advancing the development of next-generation URTP materials for versatile applications.

13.
Life Sci ; 330: 121948, 2023 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-37467885

RESUMO

AIMS: To identify N-acetyltransferase 10 (NAT10) and its downstream signaling pathways in myocytes and skeletal muscle, and to investigate its role in inflammation-induced muscle atrophy. MATERIALS AND METHODS: Cecal ligation and puncture models were used to induce sepsis in C57BL/6 mice, which were treated with either a NAT10 inhibitor or a control agent. The therapeutic effect of NAT10 inhibitor was investigated by evaluating the mass, morphology, and molecular characteristics of mouse skeletal muscle. C2C12 cells were stimulated with LPS, and the expression of the NAT10 gene, downstream protein content, and atrophy phenotype were analyzed using a NAT10 inhibitor, to further explore the atrophic effect of NAT10 on C2C12 differentiated myotubes. RESULTS: Gene set enrichment analysis revealed that NAT10 expression was elevated in the Lateral femoris muscle of patients with ICUAW. In vitro and in vivo experiments showed that sepsis or LPS induced the upregulation of NAT10 expression in skeletal muscles and C2C12 myotubes. Skeletal muscle mass, tissue morphology, gene expression, and protein content were associated with atrophic response in sepsis models. Remodelin ameliorated the LPS-induced skeletal muscle weight loss, as well as muscular atrophy, and improved survival. Remodelin reversed the atrophy program that was induced by inflammation through the downregulation of the ROS/NLRP3 pathway, along with the inhibition of the expression of MuRF1 and Atrogin-1. CONCLUSION: NAT10 is closely related to skeletal muscle atrophy during sepsis. Remodelin improves the survival rate of mice by improving the systemic inflammatory response and skeletal muscle atrophy by downregulating the ROS/NLRP3 signaling pathway.


Assuntos
Proteína 3 que Contém Domínio de Pirina da Família NLR , Sepse , Animais , Camundongos , Inflamação/patologia , Lipopolissacarídeos/farmacologia , Camundongos Endogâmicos C57BL , Fibras Musculares Esqueléticas/metabolismo , Músculo Esquelético/metabolismo , Atrofia Muscular/tratamento farmacológico , Atrofia Muscular/etiologia , Atrofia Muscular/prevenção & controle , Proteína 3 que Contém Domínio de Pirina da Família NLR/metabolismo , Espécies Reativas de Oxigênio/metabolismo , Sepse/metabolismo
14.
Biomed Pharmacother ; 163: 114837, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37156115

RESUMO

Sepsis is described as an immune response disorder of the host to infection in which microorganisms play a non-negligible role. Most survivors of sepsis experience ICU-acquired weakness, also known as septic myopathy, characterized by skeletal muscle atrophy, weakness, and irreparable damage/regenerated or dysfunctional. The mechanism of sepsis-induced myopathy is currently unclear. It has been believed that this state is triggered by circulating pathogens and their related harmful factors, leading to impaired muscle metabolism. Sepsis and its resulting alterations in the intestinal microbiota are associated with sepsis-related organ dysfunction, including skeletal muscle wasting. There are also some studies on interventions targeting the flora, including fecal microbiota transplants, the addition of dietary fiber and probiotics in enteral feeding products, etc., aiming to improve sepsis-related myopathy. In this review, we critically assess the potential mechanisms and therapeutic prospects of intestinal flora in the development of septic myopathy.


Assuntos
Microbioma Gastrointestinal , Doenças Musculares , Sepse , Humanos , Doenças Musculares/etiologia , Doenças Musculares/terapia , Músculo Esquelético/metabolismo , Atrofia Muscular/patologia , Sepse/metabolismo
15.
Biomed Pharmacother ; 158: 114209, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36916434

RESUMO

Septic myopathy, also known as ICU acquired weakness (ICU-AW), is a characteristic clinical symptom of patients with sepsis, mainly manifested as skeletal muscle weakness and muscular atrophy, which affects the respiratory and motor systems of patients, reduces the quality of life, and even threatens the survival of patients. Melatonin is one of the hormones secreted by the pineal gland. Previous studies have found that melatonin has anti-inflammatory, free radical scavenging, antioxidant stress, autophagic lysosome regulation, mitochondrial protection, and other multiple biological functions and plays a protective role in sepsis-related multiple organ dysfunction. Given the results of previous studies, we believe that melatonin may play an excellent regulatory role in the repair and regeneration of skeletal muscle atrophy in septic myopathy. Melatonin, as an over-the-counter drug, has the potential to be an early, complementary treatment for clinical trials. Based on previous research results, this article aims to critically discuss and review the effects of melatonin on sepsis and skeletal muscle depletion.


Assuntos
Melatonina , Doenças Musculares , Sepse , Humanos , Melatonina/uso terapêutico , Qualidade de Vida , Doenças Musculares/tratamento farmacológico , Músculo Esquelético/patologia , Sepse/tratamento farmacológico , Sepse/patologia , Atrofia Muscular/patologia
16.
Small ; 19(25): e2207226, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36929122

RESUMO

The improving intrinsic stability, determining the life span of devices, is a challenging task in the industrialization of inverted perovskite solar cells. The most important prerequisite for boosting intrinsic stability is high-quality perovskite films deposition. Here, a molecule, N-(2-pyridyl)pivalamide (NPP) is utilized, as a multifunctional resonance bridge between poly(triarylamine) (PTAA) and perovskite film to regulate the perovskite film quality and promote hole extraction for enhancing the device intrinsic stability. The pyridine groups in NPP couple with the phenyl groups in PTAA through π-π stacking to improve hole extraction capacities and minimize interfacial charge recombination, and the resonance linkages (NCO) in NPP dynamically modulate the perovskite buried defects through strong PbO bonds based on the fast self-adaptive tautomerization between resonance forms (NCO and N+ CO- ). Because of the combined effect of the reduction defect density and improved energy level in the perovskite buried interfaces as well as the optimized crystal orientation in perovskite film enabled by the NPP substrate, the devices based on NPP-grown perovskite films show an efficiency approaching 20% with negligible hysteresis. More impressively, the unencapsulated device displays start-of-the-art intrinsic photostability, operating under continuous 1-sun illumination for 2373 h at 65 °C without loss of PCE.

17.
Ren Fail ; 45(1): 2151468, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36645039

RESUMO

BACKGROUND: Although current guidelines didn't support the routine use of furosemide in oliguric acute kidney injury (AKI) management, some patients may benefit from furosemide administration at an early stage. We aimed to develop an explainable machine learning (ML) model to differentiate between furosemide-responsive (FR) and furosemide-unresponsive (FU) oliguric AKI. METHODS: From Medical Information Mart for Intensive Care-IV (MIMIC-IV) and eICU Collaborative Research Database (eICU-CRD), oliguric AKI patients with urine output (UO) < 0.5 ml/kg/h for the first 6 h after ICU admission and furosemide infusion ≥ 40 mg in the following 6 h were retrospectively selected. The MIMIC-IV cohort was used in training a XGBoost model to predict UO > 0.65 ml/kg/h during 6-24 h succeeding the initial 6 h for assessing oliguria, and it was validated in the eICU-CRD cohort. We compared the predictive performance of the XGBoost model with the traditional logistic regression and other ML models. RESULTS: 6897 patients were included in the MIMIC-IV training cohort, with 2235 patients in the eICU-CRD validation cohort. The XGBoost model showed an AUC of 0.97 (95% CI: 0.96-0.98) for differentiating FR and FU oliguric AKI. It outperformed the logistic regression and other ML models in correctly predicting furosemide diuretic response, achieved 92.43% sensitivity (95% CI: 90.88-93.73%) and 95.12% specificity (95% CI: 93.51-96.3%). CONCLUSION: A boosted ensemble algorithm can be used to accurately differentiate between patients who would and would not respond to furosemide in oliguric AKI. By making the model explainable, clinicians would be able to better understand the reasoning behind the prediction outcome and make individualized treatment.


Assuntos
Injúria Renal Aguda , Furosemida , Humanos , Estudos Retrospectivos , Oligúria/diagnóstico , Oligúria/tratamento farmacológico , Injúria Renal Aguda/diagnóstico , Injúria Renal Aguda/tratamento farmacológico , Aprendizado de Máquina
18.
Sci Total Environ ; 856(Pt 2): 158970, 2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36162570

RESUMO

Color dissolved organic matter (CDOM) plays a key role in lacustrine ecosystems and its composition is commonly mediated by the allochthonous input and autochthonous production. Deep lakes have a strong in-lake processing, which highly affects the sources, composition and cycle of CDOM. Here, the second deepest lake (Lake Fuxian) in China was selected to investigate the effects of allochthonous input and in-lake processing on lacustrine CDOM in deep lakes. Firstly, a detailed survey on CDOM composition across Lake Fuxian in the top water layer and inflowing rivers was carried out in the wet season representing the allochthonous input. In addition, CDOM in Lake Fuxian was compared with those in other lakes with distinct catchment characteristics and lake morphology. The results showed that compared to lacustrine CDOM in Lake Fuxian, the riverine CDOM contained much more humic-like substances, resulting in the humic-like fluorescence intensity peaked at the confluence of rivers into Lake Fuxian. In contrast, CDOM in Lake Fuxian was dominated by the protein-like substance. Comparison of CDOM composition among Lake Fuxian (well-vegetated catchment, deep lakes) with other diverse lakes in China (shallow/deep lakes with poor-vegetated catchment, and shallow lakes with well-vegetated catchment) showed similar CDOM quality in all type lakes, which were dominated by non-humified and autochthonous CDOM. Yet, CDOM quantity increased as the orders of deep lakes within poor-vegetated (Tibetan deep lakes) < the deep lake within well-vegetated catchment (Lake Fuxian) < shallow lakes within poorly-vegetated catchment (Tibetan shallow lakes) < shallow lakes within well-vegetated catchment (lakes along the middle and lower reaches of Yangtze River). Our results evidenced that the effect of allochthonous input on CDOM composition could be counteracted by in-lake processing in deep lakes. For deep lakes, a comprehensive understanding of in-lake processing of CDOM is critical for predicting lacustrine DOM composition and cycle.


Assuntos
Matéria Orgânica Dissolvida , Lagos , Ecossistema , Rios , Substâncias Húmicas/análise , China , Espectrometria de Fluorescência
19.
ACS Appl Mater Interfaces ; 14(41): 46801-46808, 2022 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-36215120

RESUMO

Tin perovskites have received great concern in solar cell research owing to their favorable optoelectronic performance and environmental friendliness. However, due to their poor crystallization and easy oxidation, the performance improvement for tin-based perovskite solar cells (TPSCs) is rather challenging. Herein, reductive 3-hydroxytyramine hydrochloride (DACl) with NH2·HCl and phenol groups as co-additives with SnF2 is added into the precursor to modulate perovskite crystallization and inhibit Sn2+ oxidation for high-performance TPSCs. The Lewis base group of NH2 HCl in DACl could bind to perovskite lattices to modulate the crystallization with suppressed defects in the bulk and grain boundary, whereas reductive phenol groups effectively constrain the Sn2+ oxidation. Moreover, the undissociated DACl decreases the supersaturated concentration of tin perovskite solution and creates a pre-nucleation site for rapid nucleation to further regulate crystallization. Consequently, the DACl-derived TPSCs achieve a high power-conversion efficiency (PCE) that reaches up to 11%. More impressively, the device remains at 84% of the initial PCE after full-sun illumination in N2 over 600 h without being encapsulated. This DACl-based synergistic modulation of a lead-free perovskite demonstrates a feasible approach using one molecule with different functional groups to manipulate crystallization, Sn2+ oxidation, and defect reparation of tin perovskite films, providing a critical guideline for constructing high-quality perovskites by multifunctional additives with high photovoltaic performance.

20.
Adv Sci (Weinh) ; 9(28): e2202028, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35975451

RESUMO

High-performance perovskite solar cells (PSCs) depend heavily on the quality of perovskite films, which is closely related to the lattice distortion, perovskite crystallization, and interfacial defects when being spin-coated and annealed on the substrate surface. Here, a dynamic strategy to modulate the perovskite film formation by using a soft perovskite-substrate interface constructed by employing amphiphilic soft molecules (ASMs) with long alkyl chains and Lewis base groups is proposed. The hydrophobic alkyl chains of ASMs interacted with poly(triarylamine) (PTAA) greatly improve the wettability of PTAA to facilitate the nucleation and growth of perovskite crystals, while the Lewis base groups bound to perovskite lattices significantly passivate the defects in situ. More importantly, this soft perovskite-substrate interface with ASMs between PTAA and perovskite film can dynamically match the lattice distortion with reduced interfacial residual strain upon perovskite crystallization and thermal annealing owing to the soft self-adaptive long-chains, leading to high-quality perovskite films. Thus, the inverted PSCs show a power conversion efficiency approaching 20% with good reproducibility and negligible hysteresis. More impressively, the unencapsulated device exhibits state-of-the-art photostability, retaining 84% of its initial efficiency under continuous simulated 1-sun illumination for more than 6200 h at elevated temperature (≈65 °C).

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