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1.
Nat Commun ; 15(1): 3115, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38600102

RESUMO

Nickel is the most widely used inexpensive active metal center of the heterogeneous catalysts for CO2 hydrogenation to methane. However, Ni-based catalysts suffer from severe deactivation in CO2 methanation reaction due to the irreversible sintering and coke deposition caused by the inevitable localized hotspots generated during the vigorously exothermic reaction. Herein, we demonstrate the inverse CeAlOx/Ni composite constructed on the Ni-foam structure support realizes remarkable CO2 methanation catalytic activity and stability in a wide operation temperature range from 240 to 600 °C. Significantly, CeAlOx/Ni/Ni-foam catalyst maintains its initial activity after seven drastic heating-cooling cycles from RT to 240 to 600 °C. Meanwhile, the structure catalyst also shows water resistance and long-term stability under reaction condition. The promising thermal stability and water-resistance of CeAlOx/Ni/Ni-foam originate from the excellent heat and mass transport efficiency which eliminates local hotspots and the formation of Ni-foam stabilized CeAlOx/Ni inverse composites which effectively anchored the active species and prevents carbon deposition from CH4 decomposition.

2.
Acta Obstet Gynecol Scand ; 102(12): 1661-1673, 2023 12.
Artigo em Inglês | MEDLINE | ID: mdl-37632276

RESUMO

INTRODUCTION: Stress urinary incontinence (SUI) occurs due to disruption of the pelvic floor anatomy; however, the complexity of the pelvic floor support structures and individual patient differences make it difficult to identify the weak points in the pelvic floor support that cause SUI to occur, develop, and recur. This study aimed to analyze the pelvic floor anatomy, structural features, and biomechanics of cystoceles to develop more effective treatment plans with individualized and precise healthcare. MATERIAL AND METHODS: In this observational case-controlled study (clinical trial identifier BOJI201855L), 102 women with normal pelvic floor function and 273 patients diagnosed with cystocele degrees I-III were identified at Shanghai General Hospital from October 2016 to December 2019. We combined ultrasound and vaginal tactile imaging (VTI) to assess the anatomy and biomechanical functions of the anterior and posterior vaginal walls. Both examinations included relaxation and muscle tension tests. RESULTS: Of the 42 VTI parameters, 13 were associated with the degree of cystocele, six with an increase in the urethral rotation angle (pointing to the mobility of the urethra), and six with a decrease in the retrovesical angle (pointing to hypsokinesis and decrease in bladder position). According to these data, the strength of tissues, especially the muscles in both the anterior and posterior compartments, contributes to the stability of the pelvic floor structure. The strength of the levator ani muscle (LAM) is important for the degree of cystocele, mobility of the urethra, hypsokinesis, and decrease in bladder position. CONCLUSIONS: In general, the biomechanical status of the pelvic floor in patients with cystocele is complex and involves various muscles, ligaments, tendons, and fascia. Of these, repair and exercise of the LAM have not received much attention in the treatment of patients with cystoceles, which may be an important risk factor for the high recurrence rate.


Assuntos
Cistocele , Incontinência Urinária por Estresse , Feminino , Humanos , China , Cistocele/diagnóstico por imagem , Cistocele/complicações , Diafragma da Pelve/diagnóstico por imagem , Bexiga Urinária , Incontinência Urinária por Estresse/diagnóstico por imagem , Incontinência Urinária por Estresse/etiologia , Estudos de Casos e Controles
3.
Int J Mol Sci ; 24(4)2023 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-36835639

RESUMO

Decarbonization has become an urgent affair to restrain global warming. CO2 hydrogenation coupled with H2 derived from water electrolysis is considered a promising route to mitigate the negative impact of carbon emission and also promote the application of hydrogen. It is of great significance to develop catalysts with excellent performance and large-scale implementation. In the past decades, metal-organic frameworks (MOFs) have been widely involved in the rational design of catalysts for CO2 hydrogenation due to their high surface areas, tunable porosities, well-ordered pore structures, and diversities in metals and functional groups. Confinement effects in MOFs or MOF-derived materials have been reported to promote the stability of CO2 hydrogenation catalysts, such as molecular complexes of immobilization effect, active sites in size effect, stabilization in the encapsulation effect, and electron transfer and interfacial catalysis in the synergistic effect. This review attempts to summarize the progress of MOF-based CO2 hydrogenation catalysts up to now, and demonstrate the synthetic strategies, unique features, and enhancement mechanisms compared with traditionally supported catalysts. Great emphasis will be placed on various confinement effects in CO2 hydrogenation. The challenges and opportunities in precise design, synthesis, and applications of MOF-confined catalysis for CO2 hydrogenation are also summarized.


Assuntos
Dióxido de Carbono , Estruturas Metalorgânicas , Hidrogenação , Hidrogênio , Carbono
4.
Nat Commun ; 13(1): 4404, 2022 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-35906219

RESUMO

Hydrogen storage by means of catalytic hydrogenation of suitable organic substrates helps to elevate the volumetric density of hydrogen energy. In this regard, utilizing cheaper industrial crude hydrogen to fulfill the goal of hydrogen storage would show economic attraction. However, because CO impurities in crude hydrogen can easily deactivate metal active sites even in trace amounts such a process has not yet been realized. Here, we develop a robust RuNi/TiO2 catalyst that enables the efficient hydrogenation of toluene to methyl-cyclohexane under simulated crude hydrogen feeds with 1000-5000 ppm CO impurity at around 180 °C under atmospheric pressure. We show that the co-localization of Ru and Ni species during reduction facilitated the formation of tightly coupled metallic Ru-Ni clusters. During the catalytic hydrogenation process, due to the distinct bonding properties, Ru and Ni served as the active sites for CO methanation and toluene hydrogenation respectively. Our work provides fresh insight into the effective utilization and purification of crude hydrogen for the future hydrogen economy.

5.
Nat Commun ; 10(1): 4348, 2019 09 25.
Artigo em Inglês | MEDLINE | ID: mdl-31554786

RESUMO

The shape-selective catalysis enabled by zeolite micropore's molecular-sized sieving is an efficient way to reduce the cost of chemical separation in the chemical industry. Although well studied since its discovery, HZSM-5's shape-selective capability has never been fully exploited due to the co-existence of its different-sized straight channels and sinusoidal channels, which makes the shape-selective p-xylene production from toluene alkylation with the least m-xylene and o-xylene continue to be one of the few industrial challenges in the chemical industry. Rather than modifications which promote zeolite shape-selectivity at the cost of stability and reactivity loss, here inverse Al zoned HZSM-5 with sinusoidal channels predominantly opened to their external surfaces is constructed to maximize the shape-selectivity of HZSM-5 sinusoidal channels and reach > 99 % p-xylene selectivity, while keeping a very high activity and good stability ( > 220 h) in toluene methylation reactions. The strategy shows good prospects for shape-selective control of molecules with tiny differences in size.

6.
Angew Chem Int Ed Engl ; 58(42): 15089-15097, 2019 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-31444841

RESUMO

The development of highly efficient metal-free carbon electrocatalysts for the oxygen reduction reaction (ORR) is one very promising strategy for the exploitation and commercialization of renewable and clean energy, but this still remains a significant challenge. Herein, we demonstrate a facile approach to prepare three-dimensional (3D) N-doped carbon with a sp3 /sp2 carbon interface derived from ionic liquids via a simple pyrolysis process. The tunable hybrid sp3 and sp2 carbon composition and pore structures stem from the transformation of ionic liquids to polymerized organics and introduction of a Co metal salt. Through tuning both composition and pores, the 3D N-doped nanocarbon with a high sp3 /sp2 carbon ratio on the surface exhibits a superior electrocatalytic performance for the ORR compared to that of the commercial Pt/C in Zn-air batteries. Density functional theory calculations suggest that the improved ORR performance can be ascribed to the existence of N dopants at the sp3 /sp2 carbon interface, which can lower the theoretical overpotential of the ORR.

7.
Adv Mater ; 31(50): e1901796, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31328318

RESUMO

Catalytic transformation of COx (x = 1, 2) with renewable H2 into valuable fuels and chemicals provides practical processes to mitigate the worldwide energy crisis. Fe-based catalytic materials are widely used for those reactions due to their abundance and low cost. Novel iron carbides are particularly promising catalytic materials among the reported ferrous catalysts. Recently, a series of strategies has been developed for the preparation of iron carbide nanoparticles and their nanocomposites. Control synthesis of FeCx -based nanomaterials and their catalytic applications in COx hydrogenation and electrochemical hydrogen evolution reaction (HER) are reviewed. The discussion is focused on the unique catalytic activities of iron carbides in COx hydrogenation and HER and the correlation between structure and catalytic performance. Future synthesis and potential catalytic applications of iron carbides are also summarized.

8.
J Am Chem Soc ; 140(3): 864-867, 2018 01 24.
Artigo em Inglês | MEDLINE | ID: mdl-29301395

RESUMO

Herein, we report the successful application of hybrid Au-Ag nanoparticles (NPs) and nanochains (NCs) in the harvesting of visible light energy for selective hydrogenation reactions. For individual Au@Ag NPs with Au25 cores, the conversion and turnover frequency (TOF) are approximately 8 and 10 times higher than those of Au25 NPs, respectively. Notably, after the self-assembly of the Au@Ag NPs, the conversion and TOF of 1D NCs were approximately 2.5 and 2 times higher than those of isolated Au@Ag NPs, respectively, owing to the coupling of surface plasmon and the increase in the rate at which hot (energetic) electrons are generated with the formation of plasmonic hot spots between NPs. Furthermore, the surface-enhanced Raman scattering (SERS) activity of 1D Au@Ag NCs was strengthened by nearly 2 orders of magnitude.

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