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1.
Chemosphere ; 356: 141952, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38599329

RESUMEN

Photo-Fenton-like technology based on H2O2 is considered as an ideal strategy to generate reactive oxygen species (ROS) for antibiotic degradation, but O2 overflow in the process severely limits the utilization efficiency of H2O2. Herein, we fabricate Bi2MoO6 (BMO) photocatalyst modified with Frustrated Lewis pairs (FLPs) as a Fenton catalyst model for enhancing reuse of spilled O2. The FLPs created by the introduction of cerium and oxygen vacancy were found to contribute to regulate the electronic structure of BMO and further improve the acidic and basic properties of photocatalyst surface. More importantly, the frustrated acid and base sites can enhance the H2O2 and O2 interfacial adsorption process and provide an Ce4+-Ov-O2- active site on the surface of Ce-BMO nanosheets, which can promote O2/•O2-/1O2/H2O2 redox cycles to achieve high H2O2 utilization efficiency. Specifically, in the experiment using tetracycline as a photocatalytic degradation object, the degradation activity of Ce-BMO was 2.15 times higher than that of BMO pure phase. Quenching experiments and EPR assays also confirmed that 1O2 and •O2- were the dominant oxidative species. This study systematically reveals the design of Fenton photocatalytic active sites at the atomic scale and provides new insights into constructing FLPs photocatalysts with high H2O2 utilization efficiency.


Asunto(s)
Bismuto , Cerio , Peróxido de Hidrógeno , Fotólisis , Peróxido de Hidrógeno/química , Bismuto/química , Cerio/química , Catálisis , Molibdeno/química , Hierro/química , Especies Reactivas de Oxígeno/química , Oxidación-Reducción , Oxígeno/química
2.
Phys Chem Chem Phys ; 26(15): 11570-11581, 2024 Apr 17.
Artículo en Inglés | MEDLINE | ID: mdl-38533820

RESUMEN

The capture and separation of CF4 from CF4/N2 mixture gas is a crucial issue in the electronics industry, as CF4 is a commonly used etching gas and the ratio of CF4 to N2 directly affects process efficiency. Utilizing high-throughput computational screening techniques and grand canonical Monte Carlo (GCMC) simulations, we comprehensively screened and assessed 247 types of pure silicon zeolite materials to determine their adsorption and separation performance for CF4/N2 mixtures. Based on screening, the relationships between the structural parameters and adsorption and separation properties were meticulously investigated. Four indicators including adsorption selectivity, working capacity, adsorbent performance score (APS), and regenerability (R%) were used to evaluate the performance of adsorbents. Based on the evaluation, we selected the top three best-performing zeolite structures for vacuum swing adsorption (LEV, AWW and ESV) and pressure swing adsorption (AVL, ZON, and ERI) processes respectively. Also, we studied the preferable adsorption sites of CF4 and N2 in the selected zeolite structures through centroid density distributions at the molecule level. We expect the study may provide some valuable guidance for subsequent experimental investigations on adsorption and separation of CF4/N2.

3.
Small ; 19(36): e2302272, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37127855

RESUMEN

The large-scale hydrogen production and application through electrocatalytic water splitting depends crucially on the development of highly efficient, cost-effective electrocatalysts for oxygen evolution reaction (OER), which, however, remains challenging. Here, a new electrocatalyst of trimetallic Fe-Co-Ni hydroxide (denoted as FeCoNiOx Hy ) with a nanotubular structure is developed through an enhanced Kirkendall process under applied potential. The FeCoNiOx Hy features synergistic electronic interaction between Fe, Co, and Ni, which not only notably increases the intrinsic OER activity of FeCoNiOx Hy by facilitating the formation of *OOH intermediate, but also substantially improves the intrinsic conductivity of FeCoNiOx Hy to facilitate charge transfer and activate catalytic sites through electrocatalyst by promoting the formation of abundant Co3+ . Therefore, FeCoNiOx Hy delivers remarkably accelerated OER kinetics and superior apparent activity, indicated by an ultra-low overpotential potential of 257 mV at a high current density of 200 mA cm-2 . This work is of fundamental and practical significance for synergistic catalysis related to advanced energy conversion materials and technologies.

4.
Inorg Chem ; 61(21): 8283-8290, 2022 May 30.
Artículo en Inglés | MEDLINE | ID: mdl-35583467

RESUMEN

The rational design and synthesis of highly efficient electrocatalysts for oxygen evolution reaction (OER) is of critical importance to the large-scale production of hydrogen by water electrolysis. Here, we develop a bimetallic, synergistic, and highly efficient Co-Fe-P electrocatalyst for OER, by selecting a two-dimensional metal-organic framework (MOF) of Co-ZIF-L as the precursor. The Co-Fe-P electrocatalyst features pronounced synergistic effects induced by notable electron transfer from Co to Fe, and a large electrochemical active surface area achieved by organizing the synergistic Co-Fe-P into hierarchical nanosheet arrays with disordered grain boundaries. Such features facilitate the generation of abundant and efficiently exposed Co3+ sites for electrocatalytic OER and thus enable Co-Fe-P to deliver excellent activity (overpotential and Tafel slope as low as 240 mV and 36 mV dec-1, respectively, at a current density of 10 mA cm-2 in 1.0 M KOH solution). The Co-Fe-P electrocatalyst also shows great durability by steadily working for up to 24 h. Our work thus provides new insight into the development of highly efficient electrocatalysts based on nanoscale and/or electronic structure engineering.

5.
Med Sci Monit ; 27: e928637, 2021 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-33711006

RESUMEN

BACKGROUND Concerns have been raised among clinicians and patients about the cardiovascular risks of bisphosphonates used in the treatment of osteoporosis. The goal of this study was to investigate the acute effect of zoledronic acid (ZA) infusion on arrhythmia development using an electrocardiograph (ECG). MATERIAL AND METHODS This prospective study was a self-controlled case series study that recruited 116 female patients with osteoporosis. The patients underwent standard 12-lead electrocardiography before and 1 day after zoledronic acid intravenous infusion to evaluate cardiac adverse effects and the change in ECG parameters after the infusion. Heart rhythm, atrial and ventricular premature contractions, atrial fibrillation, P wave, and QTc parameters were measured using an ECG. A blood biochemical examination was performed for all patients before the ZA infusion. Body temperature was measured twice per day. RESULTS Before ZA administration, ECG findings were normal in 47 patients and abnormal in 69 patients. After ZA administration, ECG findings were normal in 35 patients and abnormal in 81 patients. New onsets of premature atrial contractions and atrial fibrillation were observed in 1 patient each, and new onsets of premature ventricular contractions were observed in 2 patients. The heart rate was obviously higher, and the QT interval was obviously shorter after ZA administration, compared with before administration. No significant differences in P wave and QTc parameters were found between the 2 ECG measurements. CONCLUSIONS During the acute phase, 116 women with osteoporosis who were treated with zoledronic acid infusion did not develop significantly abnormal ECG changes.


Asunto(s)
Arritmias Cardíacas/etiología , Ácido Zoledrónico/efectos adversos , Ácido Zoledrónico/uso terapéutico , Enfermedad Aguda , Anciano , Arritmias Cardíacas/fisiopatología , Pueblo Asiatico , Fibrilación Atrial/fisiopatología , Difosfonatos/efectos adversos , Electrocardiografía/métodos , Femenino , Atrios Cardíacos/fisiopatología , Frecuencia Cardíaca/efectos de los fármacos , Humanos , Persona de Mediana Edad , Monitoreo Fisiológico , Osteoporosis/tratamiento farmacológico , Estudios Prospectivos , Ácido Zoledrónico/metabolismo
6.
Inorg Chem ; 58(21): 14652-14659, 2019 Nov 04.
Artículo en Inglés | MEDLINE | ID: mdl-31603662

RESUMEN

The development of cost-effective, high-performance, and robust bifunctional electrocatalysts for overall water splitting remains highly desirable yet quite challenging. Here, by selecting appreciate precursors of dopamine and a Co-containing metal-organic framework of ZIF-67, we subtly couple their reaction processes to develop a facile approach for the synthesis of a hollow CoP nanostructure with N-doped carbon skeleton (H-CoP@NC). Benefiting from the highly porous nanostructure and conductive carbon skeleton, H-CoP@NC is capable of working as highly active and durable bifunctional electrocatalyst for both hydrogen and oxygen evolution reaction. When further used as the electrocatalyst for overall water splitting, H-CoP@NC delivers excellent activity (cell voltage of 1.72 V at a current density of 10 mA cm-2), close to that of the noble-metal-based benchmark catalyst couple of Pt/C||RuO2. Our work thus provides new insights into the development of transitional metal phosphides based hollow hybrid nanostructures, particularly those with multiple functionalities in sustainable energy conversion technologies and systems.

7.
Small ; 12(17): 2365-75, 2016 05.
Artículo en Inglés | MEDLINE | ID: mdl-26948965

RESUMEN

The capacity of anode materials plays a critical role in the performance of lithium-ion batteries. Using the nanocrystals of oxygen-free metal-organic framework ZIF-67 as precursor, a one-step calcination approach toward the controlled synthesis of CoO nanoparticle cookies with excellent anodic performances is developed in this work. The CoO nanoparticle cookies feature highly porous structure composed of small CoO nanoparticles (≈12 nm in diameter) and nitrogen-rich graphitic carbon matrix (≈18 at% in nitrogen content). Benefiting from such unique structure, the CoO nanoparticle cookies are capable of delivering superior specific capacity and cycling stability (1383 mA h g(-1) after 200 runs at 100 mA g(-1) ) over those of CoO and graphite.

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