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1.
J Am Chem Soc ; 146(21): 14528-14538, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38742912

RESUMO

Composite oxides have been widely applied in the hydrogenation of CO/CO2 to methanol or as the component of bifunctional oxide-zeolite for the synthesis of hydrocarbon chemicals. However, it is still challenging to disentangle the stepwise formation mechanism of CH3OH at working conditions and selectively convert CO2 to hydrocarbon chemicals with narrow distribution. Here, we investigate the reaction network of the hydrogenation of CO2 to methanol over a series of spinel oxides (AB2O4), among which the Zn-based nanostructures offer superior performance in methanol synthesis. Through a series of (quasi) in situ spectroscopic characterizations, we evidence that the dissociation of H2 tends to follow a heterolytic pathway and that hydrogenation ability can be regulated by the combination of Zn with Ga or Al. The coordinatively unsaturated metal sites over ZnAl2Ox and ZnGa2Ox originating from oxygen vacancies (OVs) are evidenced to be responsible for the dissociative adsorption and activation of CO2. The evolution of the reaction intermediates, including both carbonaceous and hydrogen species at high temperatures and pressures over the spinel oxides, has been experimentally elaborated at the atomic level. With the integration of a series of zeolites or zeotypes, high selectivities of hydrocarbon chemicals with narrow distributions can be directly produced from CO2 and H2, offering a promising route for CO2 utilization.

2.
Small ; : e2402655, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38949408

RESUMO

Solution Gated Graphene Field-Effect Transistors (SGGT) are eagerly anticipated as an amplification platform for fabricating advanced ultra-sensitive sensors, allowing significant modulation of the drain current with minimal gate voltage. However, few studies have focused on light-matter interplay gating control for SGGT. Herein, this challenge is addressed by creating an innovative photoelectrochemical solution-gated graphene field-effect transistor (PEC-SGGT) functionalized with enzyme cascade reactions (ECR) for Organophosphorus (OPs) detection. The ECR system, consisting of acetylcholinesterase (AChE) and CuBTC nanomimetic enzymes, selectively recognizes OPs and forms o-phenylenediamine (oPD) oligomers sediment on the PEC electrode, with layer thickness related to the OPs concentration, demonstrating time-integrated amplification. Under light stimulation, the additional photovoltage generated on the PEC gate electrode is influenced by the oPD oligomers sediment layer, creating a differentiated voltage distribution along the gate path. PEC-SGGT, inherently equipped with built-in amplification circuits, sensitively captures gate voltage changes and delivers output with an impressive thousandfold current gain. The seamless integration of these three amplification modes in this advanced sensor allows a good linear range and highly sensitive detection of OPs, with a detection limit as low as 0.05 pm. This work provides a proof-of-concept for the feasibility of light-assisted functionalized gate-controlled PEC-SGGT for small molecule detection.

3.
Neuroradiology ; 66(3): 443-455, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38183426

RESUMO

BACKGROUND: Optimal lumbar puncture segment selection remains controversial. This study aims to analyze anatomical differences among L3-4, L4-5, and L5-S1 segments across age groups and provide quantitative evidence for optimized selection. METHODS: 80 cases of CT images were collected with patients aged 10-80 years old. Threedimensional models containing L3-S1 vertebrae, dural sac, and nerve roots were reconstructed. Computer simulation determined the optimal puncture angles for the L3-4, L4-5, and L5-S1 segments. The effective dural sac area (ALDS), traversing nerve root area (ATNR), and area of the lumbar inter-laminar space (ALILS) were measured. Puncture efficacy ratio (ALDS/ALILS) and nerve injury risk ratio (ATNR/ALILS) were calculated. Cases were divided into four groups: A (10-20 years), B (21-40 years), C (41-60 years), and D (61-80 years). Statistical analysis was performed using SPSS. RESULTS: 1) ALDS was similar among segments; 2) ATNR was greatest at L5-S1; 3) ALILS was greatest at L5-S1; 4) Puncture efficacy ratio was highest at L3-4 and lowest at L5-S1; 5) Nerve injury risk was highest at L5-S1. In group D, L5-S1 ALDS was larger than L3-4 and L4-5. ALDS decreased after age 40. Age variations were minimal across parameters. CONCLUSION: The comprehensive analysis demonstrated L3-4 as the optimal first-choice segment for ages 10-60 years, conferring maximal efficacy and safety. L5-S1 can serve as an alternative option for ages 61-80 years when upper interspaces narrow. This study provides quantitative imaging evidence supporting age-specific, optimized lumbar puncture segment selection.


Assuntos
Vértebras Lombares , Punção Espinal , Humanos , Criança , Adolescente , Adulto Jovem , Adulto , Pessoa de Meia-Idade , Idoso , Idoso de 80 Anos ou mais , Simulação por Computador , Vértebras Lombares/diagnóstico por imagem , Região Lombossacral , Tomografia Computadorizada por Raios X
4.
Front Med (Lausanne) ; 10: 1293689, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38317755

RESUMO

Background: The conventional midline approach for lumbar puncture (MAT-LP) has a relatively low success rate of 70%. The paramedian approach can increase the effective puncture area and success rate but lacks standardized guidelines. This study evaluated a computer-modified paramedian approach technique (CMPAT) to optimize lumbar puncture using computational techniques. Methods: In this prospective study, 120 patients underwent CMPAT-LP (n = 60) or MAT-LP (n = 60). Puncture failure was defined after 6 attempts. Failure rate, number of attempts, pain score, and complications were compared. Subgroup analysis was conducted for age (≥ 50 years). Results: No significant demographic differences existed between groups. Failure rates were 3.3% for CMPAT vs. 13.3% for MAT. Puncture attempts averaged 2.0 vs. 3.5 and pain scores were 2.7 vs. 4.1 for CMPAT and MAT, respectively. All outcomes were significantly improved with CMPAT, especially in elderly patients. No significant difference in complications was observed. Conclusion: Compared to MAT, CMPAT-LP demonstrated lower failure rates, fewer puncture attempts, and less pain, without compromising safety. CMPAT may be superior and should be more widely implemented in clinical practice.

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