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1.
J Chem Phys ; 159(23)2023 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-38099551

RESUMO

The development of robust and efficient photocatalytic constructs for boosting the water oxidation reaction (WOR) is needed for establishing a sunlight-driven renewable energy infrastructure. Here, we synthesized plasmonic core-shell nanoconstructs consisting of triangular gold nanoprism (AuTNP) core with mixed manganese oxide (MnOx) shell for photoelectrocatalytic WOR. These constructs show electrocatalytic WOR with a low onset overpotential requirement of 270 mV at pH 10. Photoexcitation showed further enhancement of their catalytic activity resulting in ∼15% decrease of the onset overpotential requirement along with the generation of photocurrent density of up to 300 µA/cm2. We showed that such light-driven enhancement of AuTNP@MnOx dyad's catalytic activity toward the WOR process includes contributions from both photocatalytic (hot carriers driven) and photothermal effects with photothermal effect playing the major role for wavelength between 532 and 808 nm. The contribution from the photocatalytic effect is appreciable only for high-energy excitations near the interband region, while the photothermal effect largely dominates for lower energy excitations near the LSPR wavelengths of the dyad.

2.
Nanoscale ; 15(41): 16552-16560, 2023 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-37811748

RESUMO

Photoexcitation of noble metal nanoparticles creates surface plasmons which further decay to form energetic charge carriers. These charge carriers can initiate and/or accelerate various chemical processes at nanoparticle surfaces, although the efficiency of such processes remains low as a large fraction of these carriers recombine before they can reach the reaction sites. Thus efficient utilization of these charge carriers requires designing nanostructures that promote the separation of charges and their transport toward the reaction sites. Here we demonstrate that covalently bound surface-coating ligands with suitable orbital alignment can provide electron transport channels boosting hot electron extraction from a gold nanostructure leading to a huge enhancement in the rate of hydrogen evolution reaction (HER) under NIR excitation. A (p)Br-Ph-SH substituted gold nanoprism (AuTP) substrate produced ∼4500 fold more hydrogen compared to a pristine AuTP substrate under 808 nm excitation. Further experimental and theoretical studies on a series of substituted benzene-thiol bound AuTP substrates showed that the extent of the ligand-mediated HER enhancement depends not only on the polarity of the ligand but on the interfacial orbitals interactions.

4.
ACS Appl Mater Interfaces ; 14(34): 38815-38823, 2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-35980736

RESUMO

Near-infrared (NIR) photon-driven H2 production from water is regarded as one of the best routes for establishing a sustainable hydrogen-based energy economy. Here, we have developed a gold nanoprism-based photocatalytic assembly, rationally capped with an amine and a silane ligand pair, which exhibited an excellent H2 production rate (146 µL mg-1 h-1) in neutral water while achieving an absolute incident photon-to-hydrogen conversion efficiency of 0.53%. An array of spectroscopic and microscopic experiments unravel that the amine ligand scavenges the hot hole while the silane aids the H2 production via hydrolysis during the photocatalysis on the plasmon surface. This photocatalytic H2 production reactivity can be retained for multiple cycles following the replenishment of amine and silane. Hence, this photocatalytic assembly can set up the template for a large-scale NIR-driven H2 production unit.

5.
Radiographics ; 41(1): 58-74, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-33245670

RESUMO

Traumatic injuries of the pancreas are uncommon and often difficult to diagnose owing to subtle imaging findings, confounding multiorgan injuries, and nonspecific clinical signs. Nonetheless, early diagnosis and treatment are critical, as delays increase morbidity and mortality. Imaging has a vital role in diagnosis and management. A high index of suspicion, as well as knowledge of the anatomy, mechanism of injury, injury grade, and role of available imaging modalities, is required for prompt accurate diagnosis. CT is the initial imaging modality of choice, although the severity of injury can be underestimated and assessment of the pancreatic duct is limited with this modality. The time from injury to definitive diagnosis and the treatment of potential pancreatic duct injury are the primary factors that determine outcome following pancreatic trauma. Disruption of the main pancreatic duct (MPD) is associated with higher rates of complications, such as abscess, fistula, and pseudoaneurysm, and is the primary cause of pancreatic injury-related mortality. Although CT findings can suggest pancreatic duct disruption according to the depth of parenchymal injury, MR cholangiopancreatography and endoscopic retrograde cholangiopancreatography facilitate direct assessment of the MPD. Management of traumatic pancreatic injury depends on multiple factors, including mechanism of injury, injury grade, presence (or absence) of vascular injury, hemodynamic status of the patient, and associated organ damage. ©RSNA, 2020 See discussion on this article by Patlas.


Assuntos
Traumatismos Abdominais , Ferimentos não Penetrantes , Colangiopancreatografia Retrógrada Endoscópica , Diagnóstico por Imagem , Humanos , Pâncreas/diagnóstico por imagem , Ductos Pancreáticos
6.
Langmuir ; 36(33): 9894-9899, 2020 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-32787063

RESUMO

End-to-end dimers of gold nanorods are predicted to be excellent substrates for surface-enhanced spectroscopy. However, the synthesis of solution-stable end-to-end dimers remains challenging. We exploit the pH-dependent configurational change of polyelectrolytes to initiate and terminate the gold nanorod assembly formation to produce end-to-end linked dimers in high yield. The gold nanorods are first overcoated with a polyelectrolyte, and the end-to-end attachment is initiated by adding a thiol linker in acidic medium. The assembly formation is then terminated at the dimer stage by changing the pH of the medium by the addition of an appropriate amount of 1,4-diazabicyclo[2.2.2]octane (DABCO).The nanorod dimers synthesized here are stable in solution for a week without any additional surface encapsulation.

7.
J Thorac Imaging ; 35(2): W51-W59, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31584478

RESUMO

Ballistic injuries are a major cause of morbidity and mortality in the United States. Unstable patients have high mortality, and only a small subset arrive at the hospital alive. Many patients undergo emergent surgery upon arrival, but a small subset undergo imaging with plain film, computed tomography, and echocardiography. We present a pictorial essay of ballistic and penetrating injuries and their complications with a focus on lung, cardiac, and vascular injury.


Assuntos
Ecocardiografia/métodos , Radiografia/métodos , Traumatismos Torácicos/diagnóstico por imagem , Ferimentos por Arma de Fogo/diagnóstico por imagem , Ferimentos Penetrantes/diagnóstico por imagem , Humanos , Tomografia Computadorizada por Raios X/métodos
8.
Radiographics ; 39(5): 1327-1355, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31498742

RESUMO

The kidney is the most commonly transplanted solid organ. Advances in surgical techniques, immunosuppression regimens, surveillance imaging, and histopathologic diagnosis of rejection have allowed prolonged graft survival times. However, the demand for kidneys continues to outgrow the available supply, and there are efforts to increase use of donor kidneys with moderate- or high-risk profiles. This highlights the importance of evaluating the renal transplant patient in the context of both donor and recipient risk factors. Radiologists play an integral role within the multidisciplinary team in care of the transplant patient at every stage of the transplant process. In the immediate postoperative period, duplex US is the modality of choice for evaluating the renal allograft. It is useful for establishing a baseline examination for comparison at future surveillance imaging. In the setting of allograft dysfunction, advanced imaging techniques including MRI or contrast-enhanced US may be useful for providing a more specific diagnosis and excluding nonrejection causes of renal dysfunction. When a pathologic diagnosis is deemed necessary to guide therapy, US-guided biopsy is a relatively low-risk, safe procedure. The range of complications of renal transplantation can be organized temporally in relation to the time since surgery and/or according to disease categories, including immunologic (rejection), surgical or iatrogenic, vascular, urinary, infectious, and neoplastic complications. The unique heterotopic location of the renal allograft in the iliac fossa predisposes it to a specific set of complications. As imaging features of infection or malignancy may be nonspecific, awareness of the patient's risk profile and time since transplantation can be used to assign the probability of a certain diagnosis and thus guide more specific diagnostic workup. It is critical to understand variations in vascular anatomy, surgical technique, and independent donor and recipient risk factors to make an accurate diagnosis and initiate appropriate treatment.©RSNA, 2019.


Assuntos
Transplante de Rim , Imagem Multimodal , Complicações Pós-Operatórias/diagnóstico por imagem , Seleção do Doador , Humanos
9.
Radiol Clin North Am ; 57(3): 563-583, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30928078

RESUMO

In the context of chronic liver disease (CLD), sonographic features of hepatic steatosis, cirrhosis, and portal hypertension are discussed and examples are provided. The impact of CLD and hepatocellular carcinoma (HCC) is introduced, providing the rationale for a robust HCC screening and surveillance program for at-risk patients. The American College of Radiology Liver Imaging Reporting and Data System algorithms for screening and surveillance by ultrasound and for the definitive diagnosis of HCC by contrast-enhanced ultrasound are explained, with imaging examples provided. Contrast-enhanced ultrasound technique, limitations, and pitfalls also are introduced.


Assuntos
Carcinoma Hepatocelular/diagnóstico por imagem , Neoplasias Hepáticas/diagnóstico por imagem , Ultrassonografia/métodos , Algoritmos , Carcinoma Hepatocelular/patologia , Meios de Contraste , Diagnóstico Diferencial , Humanos , Neoplasias Hepáticas/patologia , Fatores de Risco , Sensibilidade e Especificidade
10.
Radiographics ; 38(3): 766-793, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-29757718

RESUMO

Acute cholecystitis is the most common diagnosable cause for right upper quadrant abdominal (RUQ) pain in patients who present to the emergency department (ED). However, over one-third of patients initially thought to have acute cholecystitis actually have RUQ pain attributable to other causes. Ultrasonography (US) is the primary imaging modality of choice for initial imaging assessment and serves as a fast, cost-effective, and dynamic modality to provide a definitive diagnosis or a considerably narrowed list of differential possibilities. Multiple organ systems are included at standard RUQ US, and a variety of ultrasonographically diagnosable disease processes can be identified, including conditions of hepatic, pancreatic, adrenal, renal, gastrointestinal, vascular, and thoracic origin, all of which may result in RUQ pain. In certain cases, subsequent computed tomography, magnetic resonance (MR) imaging, MR cholangiopancreatography, or cholescintigraphy may be considered, depending on the clinical situation and US findings. Familiarity with the spectrum of disease processes outside of the gallbladder and biliary tree that may manifest with RUQ pain and recognition at US of these alternative conditions is pivotal for early diagnosis and appropriate management. Diagnosis at the time of initial US can reduce unnecessary imaging and its consequences, including excess cost, radiation exposure, nephrotoxic contrast medium use, and time to diagnosis, thereby translating into improved patient care and outcome. This article (a) reviews the causes of RUQ pain identifiable at US using an organ-system approach, (b) illustrates the US appearance of select conditions from each organ system with multimodality imaging correlates, and (c) discusses the relevant pathophysiology and treatment of these entities to aid in efficient direction of management. Online supplemental material is available for this article. ©RSNA, 2018.


Assuntos
Dor Abdominal/diagnóstico por imagem , Dor Abdominal/etiologia , Serviço Hospitalar de Emergência , Ultrassonografia/métodos , Meios de Contraste , Diagnóstico Diferencial , Doenças do Sistema Digestório/diagnóstico por imagem , Humanos , Doenças Torácicas/diagnóstico por imagem , Doenças Urológicas/diagnóstico por imagem , Doenças Vasculares/diagnóstico por imagem
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