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1.
J Am Chem Soc ; 146(37): 25824-25831, 2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39228089

ABSTRACT

Noble metal elements are ubiquitous in our everyday life, from medical applications to electronic devices and synthetic chemistry. Iridium is one of the least abundant elements, and despite its scarcity, it remains essential for efficient and active catalytic processes. Consequently, the development of heterogeneous catalysts with the presence of active iridium sites is of enormous interest as it leads to the improvement of their recyclability and reusability. Here, we demonstrate a strategy to incorporate iridium atoms into metal-organic frameworks (MOFs), as part of their secondary building units (SBUs), resulting in robust and reusable materials with heterogeneous photocatalytic activity.

2.
ACS Appl Electron Mater ; 6(6): 4709-4717, 2024 Jun 25.
Article in English | MEDLINE | ID: mdl-38947954

ABSTRACT

We report a semiconducting triindole-based discotic liquid crystal (TRISMe) functionalized with six p-methylthiophenyl groups at its periphery. While initially a crystalline solid at room temperature, TRISMe transitions to a columnar hexagonal mesophase upon heating and retains this supramolecular organization upon subsequent cooling, despite having only three flexible alkyl chains attached to the core's nitrogens. The incorporation of methylthio groups effectively hinders tight molecular packing, stabilizing the columnar arrangement of this disk-shaped molecule. Single crystal analysis confirmed the high tendency of this compound to organize into a columnar architecture and the role played by the methylthio groups in reinforcing such structure. The mesomorphic behavior of TRISMe provides an opportunity for processing from its molten state. Notably, our research reveals significant differences in charge transport depending on the processing method, whether solution drop-casting or melt-based. TRISMe shows hole mobility values averaging 3 × 10-1 cm2 V-1 s-1 when incorporated in diode-type devices from the isotropic melt and annealed at the mesophase temperature, estimated by SCLC (space-charge-limited current) measurements. However, when integrated into solution-processed organic field-effect transistors (OFETs), crystalline TRISMe exhibits a hole mobility of 3 × 10-4 cm2 V-1 s-1. The observed differences can be attributed to a beneficial supramolecular assembly achieved in the mesophase in spite of its lower order. These results emphasize the material's potential for applications in easy-to-process electronic devices and highlight the potential of methylthio moieties in promoting columnar mesophases.

4.
J Appl Microbiol ; 135(5)2024 May 01.
Article in English | MEDLINE | ID: mdl-38609348

ABSTRACT

AIM: Evaluate the efficacy of sponge wipe sampling at recovering potential bacterial surrogates for Category A and B non-spore-forming bacterial bioterrorism agents from hard, nonporous surfaces. METHODS: A literature survey identified seven nonpathogenic bacteria as potential surrogates for selected Category A and B non-spore-forming bacterial agents. Small (2 × 4 cm) and large (35.6 × 35.6 cm) coupons made from either stainless steel, plastic, or glass, were inoculated and utilized to assess persistence and surface sampling efficiency, respectively. Three commercially available premoistened sponge wipes (3M™, Sani-Stick®, and Solar-Cult®) were evaluated. RESULTS: Mean recoveries from persistence testing indicated that three microorganisms (Yersinia ruckeri, Escherichia coli, and Serratia marcescens) demonstrated sufficient persistence across all tested material types. Sampling of large inoculated (≥107 CFU per sample) coupons resulted in mean recoveries ranging from 6.6 to 3.4 Log10 CFU per sample. Mean recoveries for the Solar-Cult®, 3M™ sponge wipes, and Sani-Sticks® across all test organisms and all material types were ≥5.7, ≥3.7, and ≥3.4 Log10 CFU per sample, respectively. Mean recoveries for glass, stainless steel, and ABS plastic across all test organisms and all sponge types were ≥3.8, ≥3.7, and ≥3.4 Log10 CFU per sample, respectively. CONCLUSIONS: Recovery results suggest that sponge wipe sampling can effectively be used to recover non-spore-forming bacterial cells from hard, nonporous surfaces such as stainless steel, ABS plastic, and glass.


Subject(s)
Bioterrorism , Stainless Steel , Bacteria/isolation & purification , Plastics , Escherichia coli/isolation & purification , Serratia marcescens/isolation & purification , Glass , Colony Count, Microbial , Biological Warfare Agents
7.
Inorg Chem ; 62(48): 19741-19748, 2023 Dec 04.
Article in English | MEDLINE | ID: mdl-38044828

ABSTRACT

Magnetic refrigeration based on the magnetocaloric effect (MCE) in metal-organic frameworks (MOF) is regarded as an attractive approach to create more sustainable cooling systems with higher efficiency than traditional ones. Here, we report a study of the MCE in a series of rare-earth-based MOFs. We have considered the selection of the rare-earth cation by investigating materials belonging to the α-rare-earth polymeric framework-4 (α-RPF-4) MOF family, synthesized with different rare-earth cations, and observed that paramagnetic moment and saturation magnetization play an important role in enhancing the magnetic entropy change ΔSM. The effect of structural parameters has also been considered by investigating three classes of metal-organic Gd materials built up from different types of inorganic secondary building units, including clusters (as in Gd-UiO-66), one-dimensional (as in α-RPF-4), and layered (as in Gd-LRH) conformations. Moreover, the analysis of the hydrostatic pressure influence reveals a significant increase in the -ΔSM and relative cooling power (RCP) with values between 4.3 and 16.3 and 121-509 J/kg. Specifically, the RCPmax found was ∼683 J/kg for Gd-UiO-66, which is higher than the one recently observed for Gd2SiO5 (649.5 J/kg). The present study demonstrates that the engineering of metal-organic framework systems based on high Gd densities may favor enhancing of magnetocaloric responses even at low pressures, thus promoting a new design strategy for efficient cooling devices.

10.
J Investig Allergol Clin Immunol ; 33(6): 419-430, 2023 12 14.
Article in English | MEDLINE | ID: mdl-37669083

ABSTRACT

BACKGROUND: Impairment of smell is more commonly related to chronic rhinosinusitis with nasal polyps (CRSwNP) than without, especially when asthma and/or NSAID-exacerbated respiratory disease and type 2 inflammation are also present. Therapeutic options include intranasal and systemic corticosteroids, surgery, and, more recently, biological therapy. We summarize current knowledge on the effect of biologics on olfaction in patients with CRSwNP. METHODS: We performed a systematic search of the PubMed and Cochrane databases from January 2001 to June 2022. The inclusion criteria were as follows: adult patients with CRS treated with dupilumab, omalizumab, mepolizumab, benralizumab, or reslizumab; and studies published in English reporting outcomes for sense of smell based on psychophysical and/or subjective tools. We excluded reports that did not assess CRSwNP, loss of smell evaluated with a method other than those accepted in the inclusion criteria, review articles, and expert opinions. No funding was received. RESULTS: Dupilumab has demonstrated rapid and sustained long-term improvement in smell in clinical trials and in real life. Omalizumab improves smell at 24 weeks. This improvement is maintained in the long-term, although it is not clinically relevant. Mepolizumab and benralizumab improved smell in the long term based on a subjective scale. No studies examining the improvement in smell in patients with CRSwNP treated with reslizumab were found. Indirect comparisons by meta-analysis consistently conclude that dupilumab is the most effective biologic for improving impaired sense of smell. CONCLUSION: Dupilumab seems to be more efficacious for improving the sense of smell than omalizumab, mepolizumab, and benralizumab.


Subject(s)
Nasal Polyps , Rhinitis , Rhinosinusitis , Sinusitis , Adult , Humans , Antibodies, Monoclonal/therapeutic use , Nasal Polyps/drug therapy , Omalizumab/therapeutic use , Smell , Chronic Disease , Sinusitis/drug therapy , Rhinitis/drug therapy , Quality of Life
13.
J. investig. allergol. clin. immunol ; 33(6): 419-430, 2023. ilus, tab
Article in English | IBECS | ID: ibc-228624

ABSTRACT

Background: Impairment of smell is more commonly related to chronic rhinosinusitis with nasal polyps (CRSwNP) than without, especially when asthma and/or NSAID-exacerbated respiratory disease and type 2 inflammation are also present. Therapeutic options include intranasal and systemic corticosteroids, surgery, and, more recently, biological therapy. We summarize current knowledge on the effect of biologics on olfaction in patients with CRSwNP.Methods: We performed a systematic search of the PubMed and Cochrane databases from January 2001 to June 2022. The inclusion criteria were as follows: adult patients with CRS treated with dupilumab, omalizumab, mepolizumab, benralizumab, or reslizumab; and studies published in English reporting outcomes for sense of smell based on psychophysical and/or subjective tools. We excluded reports that did not assess CRSwNP, loss of smell evaluated with a method other than those accepted in the inclusion criteria, review articles, and expert opinions. No funding was received.Results: Dupilumab has demonstrated rapid and sustained long-term improvement in smell in clinical trials and in real life. Omalizumab improves smell at 24 weeks. This improvement is maintained in the long-term, although it is not clinically relevant. Mepolizumab and benralizumab improved smell in the long term based on a subjective scale. No studies examining the improvement in smell in patients with CRSwNP treated with reslizumab were found. Indirect comparisons by meta-analysis consistently conclude that dupilumab is the most effective biologic for improving impaired sense of smell.Conclusion: Dupilumab seems to be more efficacious for improving the sense of smell than omalizumab, mepolizumab, and benralizumab. (AU)


Antecedentes: La pérdida de olfato de la rinosinusitis crónica se relaciona principalmente con el fenotipo que presenta poliposis nasal (RSCcPN), especialmente si asocia asma y/o EREA, e inflamación tipo 2. Los corticoides intranasales y sistémicos, la cirugía y, de forma más reciente, los fármacos biológicos, constituyen las principales estrategias terapéuticas. Este documento contiene una revisión sistemática del efecto de los fármacos biológicos en el olfato de pacientes con RSCcPN. Métodos: Se realizó una búsqueda sistemática en las bases de datos PubMed y Cochrane desde enero de 2001 hasta junio de 2022. Los criterios de inclusión fueron: pacientes adultos con RSC tratados con dupilumab, omalizumab, mepolizumab, benralizumab o reslizumab; estudios publicados en inglés, con datos sobre la mejoría del olfato utilizando test psicofísicos y/o subjetivos. Los criterios de exclusión fueron: publicaciones que no incluían pacientes con poliposis nasal, la pérdida del olfato evaluada con un método diferente de los criterios de inclusión mencionados, los artículos de revisión y la opinión de expertos. No se empleó ningún recurso de financiación. Resultados: Dupilumab ha demostrado una mejora del olfato rápida y mantenida a largo plazo en ensayos clínicos y en la práctica clínica habitual. Omalizumab mejora el olfato en la 24ª semana y lo mantiene a largo plazo, pero no alcanza una mejoría clínicamente relevante. Mepolizumab y benralizumab mejoran el olfato a largo plazo, evaluado mediante un test subjetivo. No se encontraron estudios respecto a la mejoría del olfato en pacientes con RSCcPN tratados con reslizumab. Las comparaciones indirectas mediante metaanálisis concluyen de forma consistente que dupilumab es el biológico más eficaz para mejorar el sentido del olfato. Conclusión: Dupilumab es el biológico más eficaz en la mejoría del olfato en RSCcPN, en comparación con omalizumab, mepolizumab y benralizumab. (AU)


Subject(s)
Humans , Nasal Polyps/drug therapy , Rhinitis/drug therapy , Sinusitis/drug therapy , Antibodies, Monoclonal/therapeutic use , Omalizumab/therapeutic use , Quality of Life
19.
J Investig Allergol Clin Immunol ; 33(1): 37-44, 2023 Feb 17.
Article in English | MEDLINE | ID: mdl-35416154

ABSTRACT

BACKGROUND AND OBJECTIVES: Chronic rhinosinusitis with nasal polyps (CRSwNP), which is characterized by partial loss of smell (hyposmia) or total loss of smell (anosmia), is commonly associated with asthma and/or nonsteroidal anti-inflammatory drug-exacerbated respiratory disease (N-ERD). CRSwNP worsens disease severity and quality of life. The objective of this real-world study was to determine whether biological treatments prescribed for severe asthma can improve olfaction in patients with CRSwNP. A further objective was to compare the improvement in in olfaction in N-ERD and non-N-ERD subgroups. METHODS: We performed a multicenter, noninterventional, retrospective, observational study of 206 patients with severe asthma and CRSwNP undergoing biological treatment (omalizumab, mepolizumab, benralizumab, or reslizumab). RESULTS: Olfaction improved after treatment with all 4 monoclonal antibodies (omalizumab [35.8%], mepolizumab [35.4%], reslizumab [35.7%], and benralizumab [39.1%]), with no differences between the groups. Olfaction was more likely to improve in patients with atopy, more frequent use of short-course systemic corticosteroids, and larger polyp size. The proportion of patients whose olfaction improved was similar between the N-ERD (37%) and non-N-ERD (35.7%) groups. CONCLUSIONS: This is the first real-world study to compare improvement in olfaction among patients undergoing long-term treatment with omalizumab, mepolizumab, reslizumab, or benralizumab for severe asthma and associated CRSwNP. Approximately 4 out of 10 patients reported a subjective improvement in olfaction (with nonsignificant differences between biologic drugs). No differences were found for improved olfaction between the N-ERD and non-N-ERD groups.


Subject(s)
Asthma , Biological Products , Nasal Polyps , Rhinitis , Sinusitis , Humans , Omalizumab/therapeutic use , Nasal Polyps/complications , Nasal Polyps/drug therapy , Smell , Biological Products/therapeutic use , Anosmia/complications , Anosmia/drug therapy , Quality of Life , Retrospective Studies , Asthma/complications , Asthma/drug therapy , Immunosuppressive Agents/therapeutic use , Sinusitis/complications , Sinusitis/drug therapy , Chronic Disease , Rhinitis/complications , Rhinitis/drug therapy
20.
J Investig Allergol Clin Immunol ; 33(4): 281-288, 2023 Jul 27.
Article in English | MEDLINE | ID: mdl-35503227

ABSTRACT

BACKGROUND AND OBJECTIVE: Comorbidities can influence asthma control and promote asthma exacerbations (AEs). However, the impact of multimorbidity in AEs, assessed based on long-term follow-up of patients with asthma of different degrees of severity, has received little attention in real-life conditions. To describe the epidemiological and clinical characteristics and predictors of AEs in patients who had presented at least 1 AE in the previous year in the MEchanism of Genesis and Evolution of Asthma (MEGA) cohort. METHODS: The work-up included a detailed clinical examination, pulmonary function testing, fractional exhaled nitric oxide (FeNO), blood counts, induced sputum, skin prick-tests, asthma questionnaires, and assessment of multimorbidity. The number of moderate-severe AEs in the preceding year was registered for each patient. RESULTS: The study population comprised 486 patients with asthma (23.7% mild, 35% moderate, 41.3% severe). Disease remained uncontrolled in 41.9%, and 47.3% presented ≥1 moderate-severe AE, with a mean (SD) annual exacerbation rate of 0.47 (0.91) vs 2.11 (2.82) in mild and severe asthma, respectively. Comorbidity was detected in 56.4% (66.6% among those with severe asthma). Bronchiectasis, chronic rhinosinusitis with nasal polyps, atopy, psychiatric illnesses, hyperlipidemia, and hypertension were significantly associated with AEs. No associations were found for FeNO, blood eosinophils, or total serum IgE. Sputum eosinophilia and a high-T2 inflammatory pattern were significantly associated with AEs. Multivariable regression analysis showed a significant association with asthma severity, uncontrolled disease, and low prebronchodilator FEV1/FVC. CONCLUSION: Our study revealed a high frequency of AE in the MEGA cohort. This was strongly associated with multimorbidity, asthma severity, poor asthma control, airflow obstruction, higher sputum eosinophils, and a very high-T2 inflammatory pattern.


Subject(s)
Asthma , Eosinophilia , Humans , Nitric Oxide , Multimorbidity , Asthma/diagnosis , Asthma/epidemiology , Eosinophils
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