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1.
Inorg Chem ; 63(33): 15516-15526, 2024 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-39102647

RESUMO

Water vapor inevitably exists in the environment, which causes adverse impacts on many crucial chemical reactions. However, high water vapor of up to 10 vol %─relevant to a broad spectrum of industrial practices-for catalytic implications has been less investigated or neglected. As such, we explored an industry-relevant, humidity-highly sensitive benzene oxidation only in the presence of 10 vol % water vapor using the well-established Pt/Co3O4 catalysts, to bring such an important yet ignored topic to the forefront. Results revealed that Pt/Co3O4 catalysts possessing higher contents of Pt nanoparticles exhibited marked tolerance to water vapor interference. Under an incomplete benzene conversion condition, the input of 10 vol % water vapor indeed impaired the catalytic performance of Pt/Co3O4 catalyst significantly, which, in fact, was caused by the unfavorable formation of carboxylate species covering the catalyst's surface engendering irrecoverable activity loss, instead of the well-accepted water competitive adsorption. While such activity loss can be restored by elevating the reaction to a higher temperature. This study helps us to understand the compromised catalytic activity caused by high humidity, urging the systematic evaluation of well-established catalyst systems in high water vapor-contained conditions and pressing the development of water-tolerant catalysts for real-life application consideration.

2.
Glob Chall ; 8(5): 2300304, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38745562

RESUMO

The acute water and electricity shortages in Gaza necessitate comprehensive solutions that recognize the interconnected nature of these vital resources. This article presents pragmatic solutions to align supply with fundamental needs in both domains, offering viable pathways for achieving strategic water-energy security in Gaza. Baseline data reveals a deficit in the current water supply, falling below the international minimum of 100 L per capita per day, while the reported 137-189 MW per day electricity supply significantly lags behind the estimated 390 MW per day peak demand. To meet projected 2024 residential, commercial, and industrial demands, this study proposes actionable measures including expanding wastewater treatment to enable over 150 MCM per year tertiary effluents for agricultural reuse and adopting energy-efficient forward osmosis-reverse osmosis and osmotically assisted reverse osmosis desalination methods to increase potable water supply to 150 MCM per year. Electricity supply strategies include scaling renewable capacity towards 110 MW per day, exploring regional cooperation to unlock over 360 MW of power per day, and potentially recovering up to 60 MW per day through system efficiencies. These recommendations aim to prevent exacerbated scarcity and alleviate hardships in Gaza.

3.
Ultrason Sonochem ; 101: 106669, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37925913

RESUMO

Overexposure to antibiotics originating in wastewater has profound environmental and health implications. Conventional treatment methods are not fully effective in removing certain antibiotics, such as the commonly used antibiotic, tetracycline, leading to its accumulation in water catchments. Alternative antibiotic removal strategies are garnering attention, including sonocatalytic oxidative processes. In this work, we investigated the degradation of tetracycline using a combination of TiO2 fractured nanoshells (TFNs) and an advanced sonochemical reactor design. The study encompassed an examination of multiple process parameters to understand their effects on the degradation of tetracycline. These included tetracycline adsorption on TFNs, reaction time, initial tetracycline concentration, solvent pH, acoustic pressure amplitude, number of acoustic cycles, catalyst dosage, TFNs' reusability, and the impact of adjuvants such as light and H2O2. Though TFNs adsorbed tetracycline, the addition of ultrasound was able to degrade tetracycline completely (with 100% degradation) within six minutes. Under the optimal operating conditions, the proposed sonocatalytic system consumed 80% less energy compared to the values reported in recently published sonocatalytic research. It also had the lowest CO2 footprint when compared to the other sono-/photo-based technologies. This study suggests that optimizing the reaction system and operating the reaction under low power and at a lower duty cycle are effective in achieving efficient cavitation for sonocatalytic reactions.


Assuntos
Nanoconchas , Peróxido de Hidrogênio , Tetraciclina , Antibacterianos , Águas Residuárias , Catálise
4.
Phys Chem Chem Phys ; 25(36): 24377-24385, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37681280

RESUMO

Cu/SiO2 is one of the most promising catalysts for the furfural (FF) hydrogenation reaction but suffers from the difficulty of tailoring the microstructure and surface properties. Herein, we developed a MOF-derived Cu/SiO2 catalyst (Cu/SiO2-MOF) for FF hydrogenation to 2-methyl furan (2-MF). In comparison with Cu/SiO2 catalysts prepared from ammonia evaporation (Cu/SiO2-AE) and traditional impregnation (Cu/SiO2-TI), the copper species in Cu/SiO2-MOF could not only be anchored on the silica surface via forming Cu-O-Si bonds but also exposed many more active sites. In this way, a higher ratio of Cu+/(Cu+ + Cu0) and richer oxygen defects were constructed via strong metal-support interactions, which were responsible for the superior catalytic performance. In addition, it was found that the solvent effect on product distribution played an important role in adjusting the selectivity to 2-MF and cyclopentanone (CPO). The present work not only provides a deep insight into the catalytic mechanism of Cu/SiO2-MOF for the FF hydrogenation reaction but also sheds light on the design and synthesis of highly efficient catalysts for other heterogeneous catalysis fields.

5.
Ultrason Sonochem ; 99: 106559, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37643498

RESUMO

Sonochemistry is the use of ultrasound to generate highly reactive radical species through the inertial collapse of a gas/vapour cavity and is a green alternative for hydrogen production, wastewater treatment, and chemical synthesis and modifications. Yet, current sonochemical reactors often are limited by their design, resulting in low efficacy and yields with slow reaction kinetics. Here, we constructed a novel sonochemical reactor design that creates cylindrically converging ultrasound waves to create an intense localised region of high acoustic pressure amplitudes (15 MPaPKPK) capable of spontaneously nucleating cavitation. Using a novel dosimetry technique, we determined the effect of acoustic parameters on the yield of hydroxyl radicals (HO), HO production rate, and ultimately the sonochemical efficiency (SE) of our reactor. Our reactor design had a significantly higher HO production rate and SE compared to other conventional reactors and across literature.

6.
Phys Chem Chem Phys ; 25(27): 18215-18223, 2023 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-37394949

RESUMO

The efficient production of γ-valerolactone (GVL) from renewable lignocellulose that is synthesized in plants by photosynthesis to replace the declining fossil resources conforms to the principles of circular economy. Compared to direct hydrogenation by H2 molecules, catalytic transfer hydrogenation (CTH) of levulinic acid (LA) and/or its esters to GVL with organic alcohols as a hydrogen source is a much milder route. The synergistic catalysis between Lewis and Brønsted acids is indispensable in the CTH process. Considering that unsaturated coordinated Zr species could act as Lewis acid sites and phosphotungstic acid (PTA) could dissociate protons as Brønsted acid sites, UiO-66 (Zr) was thus "acidified" by encapsulating PTA in its channels to tune the ratio of Brønsted to Lewis acid sites as a bifunctional catalyst so as to better understand the catalytic structure-performance relationship in the CTH process. To address the dilemma of encapsulated PTA that is prone to leach, a rapid surface sealing strategy was adopted to establish a polyimide (PI) coating over the surface of UiO-66 introducing a space confinement effect via an anhydride-amine coupling reaction. The as-synthesized PTA/UiO-66@PI catalyst exhibited 100% of LA conversion, a 93.2% of GVL yield and high recyclability for at least five consecutive cycles. Moreover, a reaction pathway followed by esterification, hydrogenation and dealcoholization as well as a catalytic hydrogenation mechanism based on intermolecular hydride ß-H transfer were proposed. Current work not only provides a high-performance and high-stability catalytic system to selectively produce GVL from LA or its esters, but also sheds light on the catalytic mechanism of the CTH process at the molecular level.

7.
Chem Commun (Camb) ; 59(52): 8143-8146, 2023 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-37309840

RESUMO

Activity trends for 22 metals and metal alloys are reported for the conversion of CO2 and CH4 to 2 : 1 H2 : CO syngas and carbon. A correlation is observed between CO2 conversion and the free energy of oxidation by CO2 on pure metal catalysts. Indium and indium alloys activate CO2 at the highest rates. We identify a new bifunctional 20 : 80 mol% Sn-In alloy that activates both CO2 and CH4 while catalyzing both reactions.

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