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1.
Nature ; 633(8028): 77-82, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39198652

RESUMO

Numerous correlated many-body phases, both conventional and exotic, have been reported in magic-angle twisted bilayer graphene (MATBG)1-24. However, the dynamics associated with these correlated states, crucial for understanding the underlying physics, remain unexplored. Here we combine exciton sensing and optical pump-probe spectroscopy to investigate the dynamics of isospin orders in MATBG with WSe2 substrate across the entire flat band, achieving sub-picosecond resolution. We observe remarkably slow isospin dynamics in a broad filling range around ν = 2 and between ν = -3 and -2, with lifetimes of up to 300 ps that decouple from the much faster cooling of electronic temperature (about 10 ps). This non-thermal behaviour demonstrates the presence of abnormally long-lived modes in the isospin degrees of freedom. This observation, not anticipated by theory, implies the existence of long-range propagating collective modes, strong isospin fluctuations and memory effects and is probably associated with an intervalley coherent or incommensurate Kekulé spiral ground state. We further demonstrate non-equilibrium control of the isospin orders previously found around integer fillings. Specifically, through ultrafast manipulation, it can be transiently shifted away from integer fillings. Our study demonstrates a unique probe of collective excitations in MATBG and paves the way for actively controlling non-equilibrium phenomena in moiré systems.

2.
Proc Natl Acad Sci U S A ; 120(39): e2305943120, 2023 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-37738298

RESUMO

Different superconducting pairing mechanisms are markedly distinct in the underlying Cooper pair kinematics. Quantum-critical soft modes drive pairing interactions in which the pair scattering processes are highly collinear and can be classified into two categories: forward scattering and backscattering. Conversely, in conventional phonon mechanisms, Cooper pair scattering is of a generic noncollinear character. In this study, we present a method to discern the kinematic type by observing the evolution of superconductivity while adjusting the Fermi surface geometry. To demonstrate our approach, we utilize the recently reported phase diagrams of untwisted graphene multilayers. Our analysis connects the emergence of superconductivity at "ghost crossings" of Fermi surfaces in distinct valleys to the pair kinematics of a backscattering type. Together with the observed nonmonotonic behavior of superconductivity near its onset (sharp rise followed by a drop), it lends strong support to a particular quantum-critical superconductivity scenario in which pairing is driven by intervalley coherence fluctuations. These findings offer direct insights into the genesis of pairing in these systems, providing compelling evidence for the electron-electron interactions driving superconductivity. More broadly, our work highlights the potential of tuning bands via ghost crossings as a promising means of boosting superconductivity.

3.
Phys Rev Lett ; 133(6): 066301, 2024 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-39178453

RESUMO

Bernal bilayer graphene has recently been discovered to exhibit a wide range of unique ordered phases resulting from interaction-driven effects and encompassing spin and valley magnetism, correlated insulators, correlated metals, and superconductivity. This Letter reports on a novel family of correlated phases characterized by spin and valley ordering, distinct from those reported previously. These phases emerge in electron-doped bilayer graphene where the energy bands are exceptionally flat, manifested through an intriguing nonlinear current-bias behavior that occurs at the onset of the phases and is accompanied by an insulating temperature dependence. These characteristics align with the presence of charge- or spin-density-wave states that open a gap on a portion of the Fermi surface or fully gapped Wigner crystals, resulting in an exceptionally intricate phase diagram.

4.
Phys Rev Lett ; 130(20): 206701, 2023 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-37267555

RESUMO

We argue that spin- and valley-polarized metallic phases recently observed in graphene bilayers and trilayers support chiral edge modes that allow spin waves to propagate ballistically along system boundaries without backscattering. The chiral edge behavior originates from the interplay between the momentum-space Berry curvature in Dirac bands and the geometric phase of a spin texture in position space. The edge modes are weakly confined to the edge, featuring dispersion that is robust and insensitive to the detailed profile of magnetization at the edge. This unique character of edge modes reduces their overlap with edge disorder and enhances the mode lifetime. The mode propagation direction reverses upon reversing valley polarization, an effect that provides a clear testable signature of geometric interactions in isospin-polarized Dirac bands.

5.
J Clin Gastroenterol ; 2023 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-37732730

RESUMO

BACKGROUND AND AIMS: Recently, the location-based resect-and-discard (LBRD) strategy, which does not depend on optical diagnosis, was developed and demonstrated different surveillance interval agreement with the pathology-based reference in several researches. We aimed to evaluate the performance of LBRD in our first-time colonoscopy cohort, and improve the LBRD. METHODS: The first-time colonoscopy with complete pathologic information were enrolled. The accuracy of LBRD strategy applied in diminutive polyps in different colonic segments was used as indicator to develop modified LBRD (mLBRD) strategy. Surveillance interval agreement with pathology-based reference was compared between LBRD and mLBRD. The ≥ 90% agreement with pathology was used as benchmark. RESULTS: The polyps in sigmoid colon were significantly associated with higher proportion of neoplastic compared with polyps in rectum. The accuracy of LBRD applied in polyps in sigmoid colon were only 53.5%, which was significantly lower than that applied in polyps in other colonic segments. Thus, we hypothesized that mLBRD requiring pathology examination of diminutive polyps in sigmoid colon was more efficient in clinical use. The mLBRD significantly outperformed LBRD in surveillance interval agreement with pathology-based reference (90.2% vs. 83.4%, P<0.001), had lower proportion of patients assigned a longer surveillance interval (3.6% vs. 10.5%, P<0.001) and reached the benchmark, although the proportion of patients with an immediate surveillance interval recommendations and pathology examination avoided decreased. CONCLUSIONS: The mLBRD, but not LBRD, achieved sufficient surveillance interval agreement with pathology-based surveillance interval assignment and reduced over 30% of pathology examinations.

6.
Phys Rev Lett ; 126(25): 256803, 2021 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-34241524

RESUMO

Achieving Bloch oscillations of free carriers under a direct current, a long-sought-after collective many-body behavior, has been challenging due to stringent constraints on the band properties. We argue that the flat bands in moiré graphene fulfill the basic requirements for observing Bloch oscillations, offering an appealing alternative to the stacked quantum wells used in previous work aiming to access this regime. Bloch-oscillating moiré superlattices emit a comblike spectrum of incommensurate frequencies, a property of interest for converting direct currents into high-frequency currents and developing broadband amplifiers in terahertz domain. The oscillations can be synchronized through coupling to an oscillator mode in a photonic or plasmonic resonator. Phase-coherent collective oscillations in the resonant regime provide a realization of current-pumped terahertz lasing.

7.
J Gastroenterol Hepatol ; 36(6): 1649-1655, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33105040

RESUMO

BACKGROUND AND AIM: The number of colonoscopies required to reach satisfactory adenoma detection rate (ADR) is not well established. The aim of this study was to identify the appropriate number of procedures required to attain satisfactory ADR for those well-trained endoscopists who have a cecal intubation rate (CIR) ≥ 90% and start to perform colonoscopy independently. METHODS: All endoscopists with compelete independent colonoscopy data during career in our database were enrolled. The number of procedures required to achieve ADR ≥ 20% was identified by cumulative summation (Cusum), learning curve Cusum (LC-Cusum), and moving average method. Mixed effect logistic regression model was developed to determine the relationship between endoscopist as well as patient-related factors and adenoma detection. RESULTS: A total of 24 943 procedures and 14 endoscopists were enrolled. By Cusum analysis, the interest point was at 207 procedures. By LC-Cusum analysis, 71% (10/14) and 86% (12/14) of endoscopists had attained satisfactory ADR after 200 and 300 procedures, respectively. By moving average method, endoscopists reached a mean ADR of 20% at 216 and 261 procedures over blocks of 50 and 100 procedures, respectively. The total number of procedures, number of daily procedures, patient age and gender, bowel preparation, sedation, and diverticulosis were significantly associated with adenoma detection. CONCLUSIONS: This is the first study to investigate the learning curve of ADR for those well-trained endoscopists who have a CIR ≥ 90% and start to perform colonoscopy independently. Two hundred procedures might be an optimal number required to reach an ADR ≥ 20%.


Assuntos
Adenoma/diagnóstico , Competência Clínica , Colonoscopia/educação , Colonoscopia/estatística & dados numéricos , Neoplasias Colorretais/diagnóstico , Curva de Aprendizado , Fatores Etários , Sedação Consciente , Divertículo , Humanos , Modelos Logísticos , Fatores Sexuais
8.
Microbiol Spectr ; 12(3): e0384623, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38299831

RESUMO

Acidovorax citrulli is the main pathogen causing bacterial fruit blotch, which seriously threatens the global watermelon industry. At present, rapid, sensitive, and low-cost detection methods are urgently needed. The established CRISPR/LbCas12a visual detection method can specifically detect A. citrulli and does not cross-react with other pathogenic bacteria such as Erwinia tracheiphila, Pseudomonas syringae, and Xanthomonas campestris. The sensitivity of this method for genomic DNA detection is as low as 0.7 copies/µL, which is higher than conventional PCR and real-time PCR. In addition, this method only takes 2.5 h from DNA extraction to quantitative detection and does not require complex operation and sample treatment. Additionally, the technique was applied to test real watermelon seed samples for A. citrulli, and the results were contrasted with those of real-time fluorescence quantitative PCR and conventional PCR. The high sensitivity and specificity have broad application prospects in the rapid detection of bacterial fruit blotch bacterial pathogens of watermelon.IMPORTANCEBacterial fruit blotch, Acidovorax citrulli, is an important seed-borne bacterial disease of watermelon, melon, and other cucurbits. The lack of rapid, sensitive, and reliable pathogen detection methods has hampered research on fruit spot disease prevention and control. Here, we demonstrate the CRISPR/Cas12a system to analyze aspects of the specificity and sensitivity of A. citrulli and to test actual watermelon seed samples. The results showed that the CRISPR/Cas12a-based free-amplification method for detecting bacterial fruit blotch pathogens of watermelons was specific for A. citrulli target genes and 100-fold more sensitive than conventional PCR with quantitative real-time PCR. This method provides a new technical tool for the detection of A. citrulli.


Assuntos
Citrullus , Comamonadaceae , Citrullus/genética , Citrullus/microbiologia , Frutas/microbiologia , Doenças das Plantas/microbiologia , Comamonadaceae/genética , DNA
9.
ACS Appl Mater Interfaces ; 16(27): 35303-35314, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38934377

RESUMO

Self-powered ultraviolet photodetectors with bipolar photoresponse have great potential in the fields of ultraviolet optical communication, all-optical controlled artificial synapses, high-resolution ultraviolet imaging equipment, and multiband photoelectric detection. However, the current low optoelectronic performance limits the development of such polar switching devices. Here, we construct a self-powered ultraviolet photodetector based on GaN and In/Sn-doped Ga2O3 (IGTO) nanowires (NWs) pn junction structure. This unique nanowire/thin film structure allows GaN and IGTO to dominate the absorption of light at different wavelengths, resulting in a highly bipolar photoresponse. The device has a responsivity of 2.04 A/W and a normalized detectivity of 7.18 × 1013 Jones at 254 nm and a responsivity of -2.09 A/W and a normalized detectivity of -7 × 1013 Jones at 365 nm, both at zero bias. In addition, it has an extremely high Ilight/Idark ratio of 1.05 × 105 and ultrafast response times of 2.4/1.9 ms (at 254 nm) and 5.7/5.2 ms (at 365 nm). These excellent properties are attributed to the high specific surface area of the one-dimensional nanowire structure and the abundant voids generated by the nanowire network to enhance the absorption of light, and the p-n junction structure enables the rapid separation and transfer of photogenerated electron-hole pairs. Our findings provide a feasible strategy for high-performance wavelength-controlled polarity switching devices.

10.
RSC Adv ; 14(32): 22847-22857, 2024 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-39035720

RESUMO

Ga2O3 is a kind of wide-band gap semiconductor, which has great potential in deep ultraviolet detection because of its high efficiency and fast response. Doping can improve the photoelectric properties of Ga2O3 materials. In this paper, In and Al elements alloyed Ga2O3 nanowires (InAl-Ga2O3 NWs) were successfully grown on p-GaN using a cost-effective chemical vapor deposition method and a vertical structure. The GaN/InAl-Ga2O3 NWs p-n self-powered wide-gap UV photodetector (PD) was constructed based on sputtered gold film as the bottom and top electrodes, and spin coated with polymethyl methacrylate as the insulating layer in the vertical direction. The GaN/InAl-Ga2O3 UV PD exhibits excellent performances, including an extremely low dark current of 0.015 nA, a maximum photocurrent of about 16 nA at zero-bias voltage under 265 nm illumination, and a light-to-dark current ratio greater than 103. The responsivity is 0.94 mA W-1, the specific detectivity is 9.63 × 109 jones, and the good fast response/attenuation time is 31.2/69.6 ms. The self-powered characteristics are derived from the internal electric field formed between p-type GaN and n-type InAl-Ga2O3 NWs, which is conducive to the rapid separation and transfer of photogenerated carriers. This work provides an innovative mechanism of high-performance metal oxide nanowires for the application of p-n junction photodetectors, which can operate without any external bias.

11.
Nat Commun ; 15(1): 3133, 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38605052

RESUMO

Bernal bilayer graphene (BLG) offers a highly flexible platform for tuning the band structure, featuring two distinct regimes. One is a tunable band gap induced by large displacement fields. Another is a gapless metallic band occurring at low fields, featuring rich fine structure consisting of four linearly dispersing Dirac cones and van Hove singularities. Even though BLG has been extensively studied experimentally, the evidence of this band structure is still elusive, likely due to insufficient energy resolution. Here, we use Landau levels as markers of the energy dispersion and analyze the Landau level spectrum in a regime where the cyclotron orbits of electrons or holes in momentum space are small enough to resolve the distinct mini Dirac cones. We identify the presence of four Dirac cones and map out topological transitions induced by displacement field. By clarifying the low-energy properties of BLG bands, these findings provide a valuable addition to the toolkit for graphene electronics.

12.
Biomaterials ; 314: 122809, 2024 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-39303415

RESUMO

Targeted therapies have revolutionized traditional cancer treatments by precisely targeting tumor cells, enhancing efficacy and safety. Despite this advancement, the proportion of cancer patients eligible for such therapies remains low due to the absence of suitable targets. Here, we investigate whether the translocation of the immunogenic cell death (ICD) marker calreticulin (CALR) from the endoplasmic reticulum (ER) to the cell surface following ICD induction can serve as a target for targeted therapies. To target CALR, a nanobody Nb215 identified from a naïve VHH phage library with high binding affinity to both human and mouse CALR was employed to engineer probiotic EcN 1917. Our results demonstrated that CALR nanobody-modified EcN-215 coupled with the photothermal dye indocyanine green (ICG) was able to exert NIR-II imaging-guide photothermal therapy (PTT). Moreover, PTT with EcN-215/ICG can reshape the tumor microenvironment by enhancing the infiltration of CD45+CD3+ T cells and CD11b+F4/80+ macrophages. Furthermore, the antitumor activity of CALR-targeted EcN-215/ICG is synergistically enhanced by blocking CD47-SIRPα axis. Collectively, our study provides a proof of concept for CALR-targeted therapy. Given that CALR translocation can be induced by various anticancer therapies across numerous tumor cell lines, CALR-targeted therapies hold promise as a novel approach for treating multiple types of cancers.

13.
J Immunother Cancer ; 12(7)2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38964787

RESUMO

BACKGROUND: Chimeric antigen receptor natural killer (CAR-NK) therapy holds great promise for treating hematologic tumors, but its efficacy in solid tumors is limited owing to the lack of suitable targets and poor infiltration of engineered NK cells. Here, we explore whether immunogenic cell death (ICD) marker ERp57 translocated from endoplasmic reticulum to cell surface after drug treatment could be used as a target for CAR-NK therapy. METHODS: To target ERp57, a VHH phage display library was used for screening ERp57-targeted nanobodies (Nbs). A candidate Nb with high binding affinity to both human and mouse ERp57 was used for constructing CAR-NK cells. Various in vitro and in vivo studies were performed to assess the antitumor efficacy of the constructed CAR-NK cells. RESULTS: We demonstrate that the translocation of ERp57 can not only be induced by low-dose oxaliplatin (OXP) treatment but also is spontaneously expressed on the surface of various types of tumor cell lines. Our results show that G6-CAR-NK92 cells can effectively kill various tumor cell lines in vitro on which ERp57 is induced or intrinsically expressed, and also exhibit potent antitumor effects in cancer cell-derived xenograft and patient-derived xenograft mouse models. Additionally, the antitumor activity of G6-CAR-NK92 cells is synergistically enhanced by the low-dose ICD-inducible drug OXP. CONCLUSION: Collectively, our findings suggest that ERp57 can be leveraged as a new tumor antigen for CAR-NK targeting, and the resultant CAR-NK cells have the potential to be applied as a broad-spectrum immune cell therapy for various cancers by combining with ICD inducer drugs.


Assuntos
Morte Celular Imunogênica , Células Matadoras Naturais , Oxaliplatina , Isomerases de Dissulfetos de Proteínas , Humanos , Animais , Camundongos , Oxaliplatina/farmacologia , Oxaliplatina/uso terapêutico , Células Matadoras Naturais/imunologia , Células Matadoras Naturais/efeitos dos fármacos , Morte Celular Imunogênica/efeitos dos fármacos , Isomerases de Dissulfetos de Proteínas/metabolismo , Imunoterapia Adotiva/métodos , Receptores de Antígenos Quiméricos/imunologia , Receptores de Antígenos Quiméricos/metabolismo , Linhagem Celular Tumoral , Antineoplásicos/farmacologia , Antineoplásicos/uso terapêutico , Ensaios Antitumorais Modelo de Xenoenxerto , Neoplasias/imunologia , Neoplasias/tratamento farmacológico , Neoplasias/terapia , Feminino
14.
Science ; 383(6678): 42-48, 2024 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-38175887

RESUMO

Quantum oscillations originating from the quantization of electron cyclotron orbits provide sensitive diagnostics of electron bands and interactions. We report on nanoscale imaging of the thermodynamic magnetization oscillations caused by the de Haas-van Alphen effect in moiré graphene. Scanning by means of superconducting quantum interference device (SQUID)-on-tip in Bernal bilayer graphene crystal axis-aligned to hexagonal boron nitride reveals large magnetization oscillations with amplitudes reaching 500 Bohr magneton per electron in weak magnetic fields, unexpectedly low frequencies, and high sensitivity to superlattice filling fraction. The oscillations allow us to reconstruct the complex band structure, revealing narrow moiré bands with multiple overlapping Fermi surfaces separated by unusually small momentum gaps. We identified sets of oscillations that violate the textbook Onsager Fermi surface sum rule, signaling formation of broad-band particle-hole superposition states induced by coherent magnetic breakdown.

15.
CNS Neurosci Ther ; 30(2): e14611, 2024 02.
Artigo em Inglês | MEDLINE | ID: mdl-38353051

RESUMO

AIMS: Basolateral amygdala (BLA), as a center for stress responses and emotional regulation, is involved in visceral hypersensitivity of irritable bowel syndrome (IBS) induced by stress. In the present study, we aimed to investigate the role of EphB2 receptor (EphB2) in BLA and explore the underlying mechanisms in this process. METHODS: Visceral hypersensitivity was induced by water avoidance stress (WAS). Elevated plus maze test, forced swimming test, and sucrose preference test were applied to assess anxiety- and depression-like behaviors. Ibotenic acid or lentivirus was used to inactivate BLA in either the induction or maintenance stage of visceral hypersensitivity. The expression of protein was determined by quantitative PCR, immunofluorescence, and western blot. RESULTS: EphB2 expression was increased in BLA in WAS rats. Inactivation of BLA or downregulation of EphB2 in BLA failed to induce visceral hypersensitivity as well as anxiety-like behaviors. However, during the maintenance stage of visceral pain, visceral hypersensitivity was only partially relieved but anxiety-like behaviors were abolished by inactivation of BLA or downregulation of EphB2 in BLA. Chronic WAS increased the expression of EphB2, N-methyl-D-aspartate receptors (NMDARs), and postsynaptic density protein (PSD95) in BLA. Downregulation of EphB2 in BLA reduced NMDARs and PSD95 expression in WAS rats. However, activation of NMDARs after the knockdown of EphB2 expression still triggered visceral hypersensitivity and anxiety-like behaviors. CONCLUSIONS: Taken together, the results suggest that EphB2 in BLA plays an essential role in inducing visceral hypersensitivity. In the maintenance stage, the involvement of EphB2 is crucial but not sufficient. The increase in EphB2 induced by WAS may enhance synaptic plasticity in BLA through upregulating NMDARs, which results in IBS-like symptoms. These findings may give insight into the treatment of IBS and related psychological distress.


Assuntos
Complexo Nuclear Basolateral da Amígdala , Síndrome do Intestino Irritável , Dor Visceral , Animais , Ratos , Complexo Nuclear Basolateral da Amígdala/metabolismo , Síndrome do Intestino Irritável/metabolismo , Síndrome do Intestino Irritável/psicologia , Ratos Sprague-Dawley , Receptor EphB2/metabolismo , Estresse Psicológico/psicologia , Dor Visceral/metabolismo , Água/metabolismo
16.
Biomater Res ; 28: 0041, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38911825

RESUMO

Surgery and targeted therapy are of equal importance for colorectal cancer (CRC) treatment. However, complete CRC tumor resection remains challenging, and new targeted agents are also needed for efficient CRC treatment. Cadherin 17 (CDH17) is a membrane protein that is highly expressed in CRC and, therefore, is an ideal target for imaging-guided surgery and therapeutics. This study utilizes CDH17 nanobody (E8-Nb) with the near-infrared (NIR) fluorescent dye IRDye800CW to construct a NIR-II fluorescent probe, E8-Nb-IR800CW, and a Pseudomonas exotoxin (PE)-based immunotoxin, E8-Nb-PE38, to evaluate their performance for CRC imaging, imaging-guided precise tumor excision, and antitumor effects. Our results show that E8-Nb-IR800CW efficiently recognizes CDH17 in CRC cells and tumor tissues, produces high-quality NIR-II images for CRC tumors, and enables precise tumor removal guided by NIR-II imaging. Additionally, fluorescent imaging confirms the targeting ability and specificity of the immunotoxin toward CDH17-positive tumors, providing the direct visible evidence for immunotoxin therapy. E8-Nb-PE38 immunotoxin markedly delays the growth of CRC through the induction of apoptosis and immunogenic cell death (ICD) in multiple CRC tumor models. Furthermore, E8-Nb-PE38 combined with 5-FU exerts synergistically antitumor effects and extends survival. This study highlights CDH17 as a promising target for CRC imaging, imaging-guided surgery, and drug delivery. Nanobodies targeting CDH17 hold great potential to construct NIR-II fluorescent probes for surgery navigation, and PE-based toxins fused with CDH17 nanobodies represent a novel therapeutic strategy for CRC treatment. Further investigation is warranted to validate these findings for potential clinical translation.

17.
ACS Omega ; 8(9): 8683-8694, 2023 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-36910988

RESUMO

A FeMnCe-activated semi-coke catalyst (FeMnCe/ASC) was prepared by the co-precipitation method using semi-coke as the raw material. The structure and morphology were characterized by X-ray diffraction, Brunauer-Emmett-Teller, scanning electron microscopy, and transmission electron microscopy analyses. The catalytic activity and stability of the FeMnCe/ASC catalyst were investigated with piperazine as the target degradation pollutant and ammonia nitrogen and chemical oxygen demand (COD) as the evaluation indexes. The results showed that the average pore size of FeMnCe/ASC mesopores was 6.68 nm, and the active components were uniformly dispersed on the carrier surface. Under the optimum conditions of piperazine solution including a mass concentration of 100 mg/L, a catalyst mass concentration of 4.0 g/L, a reaction temperature of 240 °C, an oxygen partial pressure of 1.2 MPa, a stirring speed of 500 rpm, and a reaction time of 120 min, the degradation rates of both ammonia nitrogen and COD reached 100%. After the catalyst was recycled five times, the degradation rates of ammonia nitrogen and COD still reached more than 90%. The elemental valence changes before and after the reaction were analyzed by X-ray photoelectron spectroscopy, and the intermediate products generated from piperazine degradation were analyzed by gas chromatography-mass spectroscopy to evaluate the mechanism of piperazine degradation and speculate about the degradation pathway of piperazine.

18.
ACS Omega ; 8(1): 1476-1485, 2023 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-36643557

RESUMO

The threshold dilution ratio of acetaldehyde is much larger than those of other odor compounds generated during the spontaneous combustion process and so it is the most important odorant. Studying the mechanism by which acetaldehyde is generated can provide the necessary theoretical support for acetaldehyde-based odor analysis. In the present work, the release of acetaldehyde was monitored while heating lignite, long-flame coal, and coking coal specimens under either air or nitrogen. The data show that acetaldehyde was primarily produced by the oxidation of active sites in the coal rather than by the pyrolysis of oxygen-containing functional groups. Based on quantum chemistry and coal-oxygen reaction theory, the transition state approach was used to further study the formation of acetaldehyde during the low-temperature oxidation of coal. Using density functional theory, three different coal molecule structures were modeled and optimized structures for acetaldehyde formation and the energies, bond lengths, and virtual frequencies of each reaction stagnation point were obtained at the B3LYP-D3/6-311G** and M062X-D3/Def2-TZVP levels. The results indicate that the low-temperature oxidation of coal to generate acetaldehyde involves the capture of H atoms from aliphatic side chains to generate peroxy radicals. These radicals then attack unsaturated C atoms through complex inversions to generate peroxides. In the third step of this process, the O-O single bonds in the peroxides break in response to thermal energy to form carbonyl groups. Finally, specific C-C or C-O bonds on the aliphatic side chains are thermally cleaved to generate acetaldehyde.

19.
J Environ Radioact ; 270: 107284, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37634424

RESUMO

The surface isotope radon measurement method (SIRMM) is widely used in fire source detection in abandoned mines. However, studies on the long-distance migration of radon during coal spontaneous combustion are lacking, which hinders the further popularization of this technology in coal fire prevention and control. For this reason, the migration law of radon in overlying strata in fire areas was studied through experiments and numerical simulation. The radon exhalation concentration of coal was found to increase at first and then decrease in the range of 30-350 °C through experiments. The radon concentration reaches the maximum value (557.1 Bq/m3) at 150 °C, which is 6.3 times higher than that at 30 °C. Based on the radon source term obtained by fitting the experimental data, the radon migration model of coal spontaneous combustion in abandoned goaf was constructed, and the dynamic distribution characteristics of the airflow, temperature, and radon concentration fields in the overlying strata area were analyzed. The internal relationship between surface radon and underground fire source was discussed. The simulation results revealed the sharp change in the porosity of the overlying rock causes radon concentration at the interface between the caving and fissure zones to increase continually with the process of spontaneous combustion, providing material and energy support for the long-distance radon migration. When the maximum temperature of the coal pile reaches 70 °C, the concentration of radon released from the coal pile increases rapidly to 13696 Bq/m3, and the radon from the underground space appears on the surface at this temperature. In the range of 70-150 °C, with rapid increase in radon released from coal piles, the surface concentration of radon also increased rapidly to 225 Bq/m3. At the high-temperature stage exceeding 150 °C, the concentration of radon released from coal piles exhibited a downward trend, resulting in a decrease in the rate of increase of radon concentration on the surface. A close relationship between the surface radon concentration and underground fire source temperature in the process of coal spontaneous combustion was observed. In the spatial position, the peak position of radon on the surface was highly consistent with that of the fire source longitudinally, which ensures the accuracy of the SIRMM to determine the location of the hidden fire source. This suggests that the SIRMM can accurately evaluate the fire source's temperature and fire area's development trend.


Assuntos
Minas de Carvão , Incêndios , Monitoramento de Radiação , Radônio , Radônio/análise , Combustão Espontânea , Carvão Mineral/análise , Monitoramento de Radiação/métodos , Incêndios/prevenção & controle
20.
Ther Clin Risk Manag ; 18: 561-569, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35602262

RESUMO

Purpose: To identify pathology discrepancy between forceps biopsies and polypectomy specimens in colorectal polyps, as well as the reliability of biopsy-based treatment strategy. Methods: All endoscopic polypectomy cases with forceps biopsies performed within 6 months were included in the study. The biopsies were compared with polypectomy specimens in terms of concordance of histological diagnosis. A logistic regression model was used to investigate the independent predictors of upgrade in histological diagnosis compared with concordance in histological diagnosis. Results: A total of 1686 paired screening-therapeutic colonoscopies and 1739 paired biopsy-polypectomy specimens were enrolled in the study. The grade of dysplasia in 84.5% of biopsy specimens were concordant to polypectomy specimens, but this proportion decreased to 75.4% when the specimens were classified using tubular or villousness structure. 10.1% and 5.4% of biopsy specimens were upgraded and downgraded in assessing grade of dysplasia, respectively, while 14.3% and 10.3% of biopsy specimens were upgraded and downgraded in assessing tubular or villousness structure, respectively. In subgroup analysis stratified by size of polyps, 9.0% and 10.6% of biopsies obtained from polyps smaller than 10 mm were upgraded in assessing dysplasia and tubular or villousness structure, respectively. This proportion increased to 10.7% and 21.3%, respectively, in biopsies obtained from polyps larger than 10 mm. Larger size of polyps and pedunculated polyps were associated with a higher incidence of upgrade in histological diagnosis. Nearly 25% of biopsy specimens with high-grade dysplasia were identified as adenocarcinoma in polypectomy specimens. Conclusion: The concordance between biopsy and polypectomy specimens is not adequate. The biopsy-based treatment strategy is not reliable and should not be considered as an indicator for further treatment, particularly in large or pedunculated polyps.

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