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1.
Proc Natl Acad Sci U S A ; 119(34): e2206131119, 2022 08 23.
Artigo em Inglês | MEDLINE | ID: mdl-35969735

RESUMO

Split air conditioners (ACs) are the most used appliance for space cooling worldwide. The phase-down of refrigerants with high global warming potential (GWP) prescribed by the Kigali Amendment to the Montreal Protocol has triggered a major effort to find less harmful alternative refrigerants. HFC-32 is currently the most common refrigerant to replace HFC-410A in split ACs. The GWP of HFC-32 is about one-third that of HFC-410A but still considerably higher than that of a growing number of nonfluorinated alternatives like propane with a GWP of <1, which have recently become commercially available for split ACs. Here, we show that a switch to propane as an energy-efficient and commercially available low-GWP alternative in split ACs could avoid 0.09 (0.06 to 0.12) °C increase in global temperature by the end of the century. This is significantly more than the 0.03 (0.02 to 0.05) °C avoided warming from a complete switch to HFC-32 in split ACs.


Assuntos
Poluentes Atmosféricos/análise , Aquecimento Global , Hidrocarbonetos Fluorados/análise , Propano , Desenvolvimento Sustentável , Temperatura
2.
Nano Lett ; 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38837959

RESUMO

Propane dehydrogenation (PDH) serves as a pivotal intentional technique to produce propylene. The stability of PDH catalysts is generally restricted by the readsorption of propylene which can subsequently undergo side reactions for coke formation. Herein, we demonstrate an ultrastable PDH catalyst by encapsulating PtIn clusters within silicalite-1 which serves as an efficient promoter for olefin desorption. The mean lifetime of PtIn@S-1 (S-1, silicalite-1) was calculated as 37317 h with high propylene selectivity of >97% at 580 °C with a weight hourly space velocity (WHSV) of 4.7 h-1. With an ultrahigh WHSV of 1128 h-1, which pushed the catalyst away from the equilibrium conversion to 13.3%, PtIn@S-1 substantially outperformed other reported PDH catalysts in terms of mean lifetime (32058 h), reaction rates (3.42 molpropylene gcat-1 h-1 and 341.90 molpropylene gPt-1 h-1), and total turnover number (14387.30 kgpropylene gcat-1). The developed catalyst is likely to lead the way to scalable PDH applications.

3.
Small ; 20(32): e2309127, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38554016

RESUMO

Conventional separation technologies for valuable commodities require substantial energy, accounting for 10%-15% of global consumption. Mixed-matrix membranes (MMMs) offer a promising solution by combining processable polymers with selective inorganic fillers. Here, the potential of using ordered microporous structured materials is demonstrated as MMM fillers. The use of ordered macroporous ZIF-67 in combination with the well-known 6FDA-DAM polymer leads to superior performance in the important separation of propylene from propane. The enhanced performance can be rationalized with the help of advanced microscopy, which demonstrates that the polymer is able to penetrate the macroporous network around which the MOF (Metal-Organic Framework) is synthesized, resulting in a much better interphase between the two components and the homogeneous distribution of the filler, even at high loadings.

4.
Chemistry ; : e202402764, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39327774

RESUMO

Silicoaluminate zeolites have relatively strong Brönsted (B) acid properties that can easily lead to deep cracking reactions, making them less favourable as carriers for propane dehydrogenation. Here, we utilise zincosilicate zeolite with less B-acid produced by the introduction of the heteroatom Zn into the framework as a carrier, followed by simultaneous ion exchange (IE) of M monometallic or PtM bimetallic (M = Cu, Zn and Ga, etc.). The optimized PtZn/Zn-4 exhibits a superior propane dehydrogenation performance over PtCu/Zn-4 and PtGa/Zn-4, which can achieve a propane conversion of about 30% in a pure propane atmosphere at 550 °C and can be operated for at least 168 h without significant deactivation. Characterization techniques such as spherical aberration corrected transmission electron microscopy, in situ X-ray photoelectron spectroscopy, and in situ diffuse reflectance infrared fourier transform spectroscopy with different gas adsorptions are used to investigate these PtM@zeolite catalysts in order to deepen the understanding of acid site identification, promoter effect and catalysis.

5.
Environ Sci Technol ; 58(28): 12742-12753, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-38959431

RESUMO

Short carbon chain alkanes, as typical volatile organic compounds (VOCs), have molecular structural stability and low molecular polarity, leading to an enormous challenge in the catalytic oxidation of propane. Although Ru-based catalysts exhibit a surprisingly high activity for the catalytic oxidation of propane to CO2 and H2O, active RuOx species are partially oxidized and sintered during the oxidation reaction, leading to a decrease in catalytic activity and significantly inhibiting their application in industrial processes. Herein, the Ru/Ce@Co catalyst is synthesized with a specific structure, in which cerium dioxide is dispersed in a thin layer on the surface of Co3O4, and Ru nanoparticles fall preferentially on cerium oxide with high dispersity. Compared with the Ru/CeO2 and Ru/Co3O4 catalysts, the Ru/Ce@Co catalyst demonstrates excellent catalytic activity and stability for the oxidation of propane, even under severe operating conditions, such as recycling reaction, high space velocity, a certain degree of moisture, and high temperature. Benefiting from this particular structure, the Ru/Ce@Co (5:95) catalyst with more Ce3+ species leads to the Ru species being anchored more firmly on the CeO2 surface with a low-valent state and has a strong potential for adsorption and activation of propane and oxygen, which is beneficial for RuOx species with high activity and stability. This work provides a novel strategy for designing high-efficiency Ru-based catalysts for the catalytic combustion of short carbon alkanes.


Assuntos
Oxirredução , Catálise , Cério/química , Propano/química , Propano/análogos & derivados , Rutênio/química
6.
Environ Sci Technol ; 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38319875

RESUMO

Light alkanes (LAs), typical VOCs existing in both stationary and mobile sources, pose significant environmental concerns. Although noble metal catalysts demonstrate strong C-H bond activation, their effectiveness in degrading LAs is hindered by inherent challenges, including poor chemical stability and water resistance. Here, from a new perspective, we propose a feasible strategy that adjusting the metal bond lengths within Pd clusters through partial substitution of smaller radius 3d transition metals (3dTMs) to prioritize the activation of low-energy C-C bonds within LAs. Benefiting from this, PdCo/CeO2 exhibits exceptional catalytic performance in propane degradation due to their high capacity for C-C cleavage stemming from the shorter Pd-Co length (2.51 Å) and lower coordination number (1.73), boosting the activation of α-H and ß-H of propane simultaneously and accelerating the mobility of postactivated oxygen species to prevent Pd center deep oxidation. The presence of 3dTMs on Pd clusters improves the redox and charge transfer ability of catalysts, resulting in an amplified generation of oxygen vacancies and facilitating the adsorption and activation of reactants. Mechanistic studies and DFT calculations suggest that the substitution of 3dTMs significantly accelerate C-C bond cleavage within C3 intermediates to generate the subsequent C2 and C1 intermediates, suppressing the generation of harmful byproducts.

7.
Int J Toxicol ; : 10915818241260280, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38872413

RESUMO

The Expert Panel for Cosmetic Ingredient Safety (Panel) first published the Final Report of the safety of Isobutane, Isopentane, Butane, and Propane in 1982. The Panel previously concluded that these ingredients are considered safe as cosmetic ingredients under the present conditions of concentration and use, as described in that safety assessment. Upon re-review in 2002, the Panel reaffirmed the original conclusion, as published in 2005. The Panel reviewed update frequency and concentration of use data again in 2023, in addition to newly available, relevant safety data. Considering this information, as well as the information provided in the original safety assessment and the prior re-review document, the Panel reaffirmed the 1982 conclusion for Isobutane, Isopentane, Butane, and Propane.

8.
Molecules ; 29(6)2024 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-38542849

RESUMO

Compared to the currently widely used propane dehydrogenation process for propylene production, propane oxidative dehydrogenation (ODHP) offers the advantage of no thermodynamic limitations and lower energy consumption. However, a major challenge in ODHP is the occurrence of undesired over-oxidation reactions of propylene, which reduce selectivity and hinder industrialization. MOFs possess a large number of metal sites that can serve as catalytic centers, which facilitates the easier access of reactants to the catalytic centers for reaction. Additionally, their flexible framework structure allows for easier adjustment of their pores compared to metal oxides and molecular sieves, which is advantageous for the diffusion of products within the framework. This property reduces the likelihood of prolonged contact between the generated propylene and the catalytic centers, thus minimizing the possibility of over-oxidation. The research on MOF catalyzed oxidative dehydrogenation of propane (ODHP) mainly focuses on the catalytic properties of MOFs with cobalt oxygen sites and boron oxygen sites. The advantages of cobalt oxygen site MOFs include significantly reduced energy consumption, enabling catalytic reactions at temperatures of 230 °C and below, while boron oxygen site MOFs exhibit high conversion rates and selectivity, albeit requiring higher temperatures. The explicit structure of MOFs facilitates the mechanistic study of these sites, enabling further optimization of catalysts. This paper provides an overview of the recent progress in utilizing MOFs as catalysts for ODHP and explores how they promote progress in ODHP catalysis. Finally, the challenges and future prospects of MOFs in the field of ODHP reactions are discussed.

9.
Molecules ; 29(13)2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38999013

RESUMO

Propane dehydrogenation (PDH) is a crucial approach for propylene production. However, commonly used CrOx-based catalysts have issues including easy sintering at elevated reaction temperatures and relying on high acidity supports. In this work, we develop a strategy, to strongly anchor and isolate active sites against their commonly observed aggregation during reactions, by taking advantage of the net trap effect in chromate intercalated Zn-Cr layered hydroxides as precursors. Furthermore, the intercalated chromate overcomes the collapse of traditional layered hydroxides during their transformation to metal oxide, thus exposing more available active sites. A joint fine modulation including crystal structure, surface acidity, specific surface area, and active sites dispersion is performed on the final mixed metal oxides for propane dehydrogenation. As a result, Zn1Cr2-CrO42--MMO delivers attractive propane conversion (~27%) and propylene selectivity (>90%) as compared to other non-noble-metal-based catalysts.

10.
Environ Monit Assess ; 196(10): 935, 2024 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-39278887

RESUMO

There is growing global concern regarding the detrimental health impacts of PM2.5 emissions from traditional stoves that utilize polluting fuels. Conventional methods for estimating daily personal PM2.5 exposure involve personal air samplers and measuring devices placed in a waist pouch, but these instruments are cumbersome and inconvenient. To address this issue, we developed a novel neck-mounted PM2.5 monitoring device (Pocket PM2.5 Logger) that is compact, lightweight, and can operate continuously for 1 week without recharging. Twelve participants who utilized charcoal, firewood, or propane gas for cooking in rural regions of Rwanda wore the Pocket PM2.5 Logger continuously for 1 week, and time-series variations in personal PM2.5 exposure were recorded at 5-min intervals. Individual daily exposure concentrations during cooking differed significantly among users of the different fuel types, and PM2.5 exposure was at least 2.6 and 3.4 times higher for charcoal and firewood users, respectively, than for propane gas users. Therefore, switching from biomass fuels to propane gas would reduce daily individual exposure by at least one-third. An analysis of cooking times showed that the median cooking time per meal was 30 min; however, half the participants cooked for 1.5 h per meal, and one-third cooked for over 4.5 h per meal. Reducing these extremely long cooking times would reduce exposure with all fuel types. The Pocket PM2.5 Logger facilitates the comprehensive assessment of personal PM2.5 exposure dynamics and is beneficial for the development of intervention strategies targeting household air pollution.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Culinária , Monitoramento Ambiental , Material Particulado , População Rural , Ruanda , Material Particulado/análise , Humanos , Culinária/instrumentação , Monitoramento Ambiental/métodos , Monitoramento Ambiental/instrumentação , Poluição do Ar em Ambientes Fechados/análise , Poluição do Ar em Ambientes Fechados/estatística & dados numéricos , Poluentes Atmosféricos/análise , Adulto , Masculino , Feminino , Exposição Ambiental/estatística & dados numéricos , Exposição Ambiental/análise , Carvão Vegetal , Pessoa de Meia-Idade
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