Greenhouse Gases-Science and Technology
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2022
·Vol. 12
·期 2
·305-320
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IF 2.518
Zichen Liu,Shuman Xu,Jing Hao,Lina Song,Mingben Chong,Dang-Guo Cheng,Fengqiu Chen
The conversion of CO 2 into high-value chemicals has drawn a great deal of consideration, of which the most ideal product is lower olefins. However, the modified Fischer–Tropsch (F-T) synthesis with CO as an intermediate shows poor selectivity for lower olefins. Here, a list of bifunctional catalysts consisting of SAPO-34 zeolites with adjustable silicon contents and In 2 O 3 /ZrO 2 were synthesized. In the reaction process, CO 2 is first hydrogenated to methanol over an In 2 O 3 /ZrO 2 catalyst, and then the generated methanol rapidly diffuses to the adjacent zeolite catalyst to react to lower olefins. The selectivity of lower olefins (88.3%) and conversion rate of CO 2 (23.3%) was achieved over In 2 O 3 /ZrO 2 and SAPO-34-0.05 at 633 K, a gas hourly space velocity (GHSV) of 4500 ml·gcat –1 ·h –1 , and H 2 /CO 2 /Ar = 3:1:1. The catalytic performance remained stable after 50 h of reaction. Characterization analysis showed that Si content affected the content of Brønsted acid sites (BAS) and morphology of SAPO-34, resulting in different distribution of reaction intermediates. Tetramethyl-benzenes, as important intermediate species, had a slower conversion rate on the SAPO-34 with low Si content and nanosheet morphology, which led to high lower olefins selectivity. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Zhang Changsheng,Chu Shaoqi,Jiang Jie,Zhao Jinchong,Wen Song,Sun Bing,Xu Wei
Synthesis of zeolites in more efficient and greener methods is of great significance in both industrial and academic fields. However, the relative long time for zeolite crystallization and much consumption of water solvent make the target challengeable. Herein, a route for ultrafast synthesis of nano Silicalite-1 zeolites in 10 min with much less water consumption has been developed. Comprehensive characterizations, i.e., X-ray powder diffraction, N2 sorption, scanning electron microscope, and NMR, confirm the high quality of such obtained Silicalite-1 zeolites. In the catalytic deoxygenation of O2-containing ethylene (mixture of O2 and ethylene), these reported Silicalite-1 zeolite samples show the comparable performance with the conventional Silicalite-1 zeolites synthesized under hydrothermal conditions. This research therefore provides a new trial toward the ultrafast synthesis of zeolite materials in an environment-friendly route.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Shiqing Li,Xiaomeng Si,Rusi Peng,Huang Pan,Hao Xu,Jingang Jiang,Yanhang Ma,Peng Wu
Hierarchical Beta zeolite (named ECNU-41) was directly synthesized with commercially available ionic liquid 1-butyl-1-methylpyrrolidinium hydroxide as organic structure-directing agent (OSDA) in the absence of any surfactants or polymers. The ECNU-41 crystals were composed of nanorods through a unique stacking manner, exhibiting a morphology resembling the Chinese traditional toy “burr puzzle”. The orderly crisscrossed stacking ECNU-41 possesses high hydrothermal stability, abundant intercrystal mesoporosity, and enriched phase of polymorph B. In comparison to conventional nanosized Beta zeolites, ECNU-41 aluminosilicate and titanosilicate exhibited more remarkable and competitive catalytic performances in a variety of reactions, including benzene alkylation , methanol to propylene , and alkenes epoxidation. With improved diffusion rate and mass transfer due to the hierarchical structure, ECNU-41 is expected to serve as promising catalysts for those reactions involving bulky molecules.
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Drug Design Development and Therapy
·
2022
·
IF 4.319
Xuemeng Xie,Jinfu Tu,Heyi You,Bingren Hu
Given the important role that inhibitory kappa B (IκB) kinase β (IKKβ) plays in pancreatic cancer (PC) development and progression, inhibitors targeting IKKβ are believed to be increasingly popular as novel anti-PC therapies. Two synthetic molecules, named EF24 and EF31, exhibited favorable potential in terms of inhibition of both IKKβ activity and PC cell proliferation. Aiming to enhance their cellular efficacy and to analyze their structure–activity relationship, four series of EF24 and EF31 analogs were designed and synthesized. Through kinase activity and vitality screening of cancer cells, D6 displayed excellent inhibition of both IKKβ activity and PC cell proliferation. Additionally, multiple biological evaluations showed that D6 was directly bound to IKKβ and significantly suppressed the activation of the IKKβ/nuclear factor κB pathway induced by tumor necrosis factor-α, as well as effectively inducing cancer cell apoptosis. Moreover, molecular docking and molecular dynamics simulation analysis indicated that the dominant force between D6 and IKKβ comprised hydrophobic interactions. In conclusion, D6 may be a promising therapeutic agent for PC treatment and it also provides a structural lead for the design of novel IKKβ inhibitors.
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International Journal of Environmental Research and Public Health
·
2022
·Vol. 19
·期 19
·12547
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IF 4.614
Nan Wang,Zhengwu Cui,Yang Wang,Jingjing Zhang
In this study, eleven organochlorine pesticides (OCPs) in fresh vegetables in the Changchun suburb were investigated, and their potential health risks were evaluated. The average concentrations of OCPs in edible parts of vegetables were found in the following descending order: Σhexachlorocyclohexanes (ΣHCHs) (6.60 µg·kg−1) > Σdichlorodiphenyltrichloroethanes (ΣDDTs) (5.82 µg·kg−1) > ΣChlordanes (2.37 µg·kg−1) > heptachlor (0.29 µg·kg−1). Moreover, OCPs in different types of vegetables exceeded the maximum residue limits (MRLs), and the exceeding rates in various vegetables decreased in the following order: leafy vegetables (19.12%) > root vegetables (18.75%) > fruit vegetables (3.85%). The proportions of OCPs exceeding MRL in different vegetables were found in the following descending order: Welsh onion (22.50%) > radish (18.75%) > Chinese cabbage (14.29%) > pepper (6.90%) > cucumber (3.23%) > eggplant (2.94%) > tomato (2.78%). The sources’ identification results showed that DDTs in vegetables came mainly from newly imported technical DDTs and dicofol, while HCHs originated mainly from lindane. For both adults and children, the average target hazard quotients (avg. THQ) were all less than 1, and the average hazard index (avg. HI) values were 0.043 and 0.036, respectively. There were no significant health risks associated with OCP exposure for the inhabitants of the study area.Keywords:suburban vegetables;organochlorine pesticides;maximum residue limit (MRL);sources identification;target hazard quotient (THQ)
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Drug Design Development and Therapy
·
2022
·
IF 4.319
Yali Zhang,Chengguang Zhao,Wenfei He,Zhe Wang,Qilu Fang,Bing Xiao,Zhiguo Liu,Guang Liang,Shulin Yang
Sepsis is a systemic inflammatory response syndrome and is mainly caused by lipopolysaccharides (LPS) – a component of the cell walls of gram-negative bacteria, via toll-like receptor 4–mitogen-activated protein kinases/nuclear factor-kappa B-dependent proinflammatory signaling pathway. Here, we synthesized 26 asymmetric monocarbonyl analogs of curcumin and evaluated their anti-inflammatory activity by inhibiting the LPS-induced secretion of tumor necrosis factor-α and interleukin-6 in mouse RAW264.7 macrophages. Five active compounds (3a, 3c, 3d, 3j, and 3l) exhibited dose-dependent inhibition against the release of tumor necrosis factor-α and interleukin-6, and they also showed much higher chemical stability than curcumin in vitro. The anti-inflammatory activity of analogs 3a and 3c may be associated with their inhibition of the phosphorylation of extracellular signal-regulated kinase and the activation of nuclear factor-kappa B. In addition, 3c exhibited significant protection against LPS-induced septic death in vivo. These results indicate that asymmetrical monocarbonyl curcumin analogs may be utilized as candidates for the treatment of acute inflammatory diseases.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Huijie Xie,Wei Xu,Saiai Ran,Xiaolong Li,Bin Li,Yanyan Li,Lei Wang
Green synthesis of zeolite has been made much progress due to solvent-free grinding methods. Although solid-state synthesis is a simple green process with a high yield, its kinetics of the solid-phase crystallization process is still slow and the precursor materials are not uniformly heated throughout the reactor resulting into the poor uniformity of the particles. Herein, we report a high-efficiency organotemplate-free synthesis of ZSM-5 combining solid state grinding and steam-assisted crystallization. Solid state grinding (SSG) of aluminosilicate precursor avoids usage of solvent and steam-assisted conversion (SAC) in an organic-template-free condition grants a fast crystallization rate of ZSM-5. More importantly, the vapor fulfilled in the reactor ensures uniform heating of solid feedstock for crystallization of ZSM-5, leading the high crystallinity and the uniform particle size distribution . This combination can guarantee 100% relative crystallinity of ZSM-5 in 12 h, compared to that of 80% crystallinity from sole solid state at the same crystallization temperature (180 °C). Furthermore, this combination can achieve 83% relative crystallinity of ZSM-5 at 160 °C, compared to that of 37% crystallinity from the solid state alone. Highly dispersed ZSM-5 zeolite with adjustable SiO 2 /Al 2 O 3 ratio is prepared by steam-assisted crystallization of grinding solid raw materials. The catalytic activity of ZSM-5 catalyst from this combination strategy for the acetalization of cyclohexanone is superior to that of the solid-state method alone. This sustainable and green synthesis method provides a potential way for the preparation of zeolites in an industrial scale.
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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
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2022
·
IF 5.168
Peng Fang,Jia Wu,Botian Li,Bin Cheng,Daofu Song,Ningning Zhong
Asphaltenes are the heaviest compound group in crude oil. The complex and porous macromolecular network of asphaltenes both adsorbs and occludes small hydrocarbon molecules, which are considered source-related petroleum biomarkers as they are shielded from secondary alterations. The current method to isolate the occluded content involves mild oxidative degradation of asphaltenes with CH 3 COOH/H 2 O 2 , but it is generally not suitable for quantitative studies, as side reactions that chemically alter the bound hydrocarbons are difficult to mitigate. In the current study, we compared the performance of dispersive solid-phase extraction (DSPE) and mild oxidative degradation in isolating asphaltene-occluded hydrocarbons, using Lower Cambrian solid bitumen from northwestern Sichuan and Ordovician crude oil from the Tazhong area of Xinjiang, China. We demonstrated that DSPE was effective in extracting occluded hydrocarbons from asphaltene aggregates without undesirable chemical alterations, thereby allowing subsequent quantitative analysis. Further investigations revealed that the chemical composition of the occluded n -alkanes provided useful information with regard to the origin of the petroleum. Importantly, the enrichment of aromatic hydrocarbons inside the asphaltene aggregates, particularly the relative abundance of different methylphenanthrene isomers, provided crucial experimental evidence in support of our earlier hypothesis that the occluded hydrocarbons were protected from secondary alterations, and therefore had remained relatively stable over a long geologic period.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Shanqi Zhou,Mengru Fu,Kailun Luo,Zhihua Qiao,Cheng Peng,Wei Zhang,Juying Lei,Siyuan Ling,Bingsheng Zhou
Due to the characteristics of persistent organic pollutants (POPs), some legacy brominated flame retardants (LBFRs) were prohibited from use, and then gradually replaced by novel brominated flame retardants (NBFRs). However, till now little research focused on the effects of NBFRs on the benthos . In the present study, 0.5, 5, and 50 mg/kg dw of pentabromotoluene (PBT), hexabromobenzene (HBB), 1,2-bis(2,4,6-tribromophenoxy) ethane (BTBPE), decabromodiphenyl ethane (DBDPE) and decabromodiphenyl ether (BDE209) were added into sediments to test freshwater clams ( Corbicula fluminea ). In the 35-day exposure experiment, C. fluminea had different enrichment behaviors in three treatment groups. It was conjectured that in the lower dose group, the clams ingested contaminants and tended to be stable over time. While in higher dose groups, the clams were induced by the chemicals, leading to the changes in physiological activities so that the concentrations showed a downward trend first and then went up. The half-lives of contaminants in freshwater clams were between 0.911 and 11.6 days. DBDPE showed stronger bioaccumulation ability than BDE209 in this study. Parabolic relationships were observed between log BSAF and log K ow values in clam tissues. Debromination, hydroxylation, and methoxylated products were detected. Additionally, the gill samples of C. fluminea exposed to 50 mg/kg dw of single substance were observed by scanning electron microscope (SEM), indicating that the adhesions, tissue hyperplasia, and messy cilia occurred on the surface. Our research potentially contributes to further evaluations of the environmental risks posed in sediments contaminated by PBT, HBB, BTBPE, DBDPE, and BDE209, particularly the benthic organisms.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 33
·15959-15966
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IF 3.925
Kai Zong,Ke Li,Ziyue Zhou,Lei Gong,Dongshun Deng
The uptake of NH3 in the industrial tail gas will improve the environmental quality for human health and ecology. Adsorption separation has the advantages of simple operation and low energy consumption. However, the relatively low adsorption capacity severely hinders its practical utilization. In this work, four glycerol-based deep eutectic solvents (DESs) were incorporated into porous silica gels (SGs) and Al2O3 with a large surface area and pore structure to form novel DES/SG and DES/Al2O3 composites. The obtained materials were systematically characterized by FTIR, SEM, BET, and TGA and further evaluated for NH3 adsorption. The results showed that the acidic GuSCN:Gly DES played an indispensable role for the high adsorption ability of the composite. 40 wt% GuSCN : Gly (1 : 3) DES/SG can capture 115.40 mg NH3 per gram adsorbent, which is better than most of the solid adsorption materials reported in the literature and even 30% higher than the original SG. The high adsorption capacity, outstanding thermal stability, and good reusability confirm the success of the present strategy. This study will provide a useful idea for designing DES-supported composites for NH3 separation applications.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2022
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IF 6.364
Yulong Yang,Wanyi Fu,Xixi Chen,Li Chen,Congyu Hou,Yanyi Wang,Tianhao Tang,Xihui Zhang
Silica sol is widely used in the preparation of mullite-based fiber porous ceramics (MFPCs), but it aggregates at the top surface of MFPCs during the drying process. This leads to the decrease in mechanical strength and porosity. To overcome the problem and fabricate homogeneous MFPCs, the sodium silicate solution and glass fibers were applied in the fabrication process of MFPCs. The effects of concentrations of sodium silicate solution and silica sol, amounts of glass fibers and sintering temperatures on the properties of prepared MFPCs were studied. The sodium silicate solution consolidated the silica sol and mullite fibers, forming a homogeneous structure and ensuring the even distribution of silica sol. Compared with other reported MFPCs, this process required low sintering temperature while maintaining high compressive strength (2.14 MPa) and porosity (75.93%). This study provides an effective method for preparing MFPCs with high strength, uniformity and porosity.
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Nano Research
·
2021
·Vol. 14
·期 11
·4347-4355
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IF 8.897
Lu Xiaowen,Guo Chunmu,Zhang Mingyang,Leng Leipeng,Horton J. Hugh,Wu Wei,Li Zhijun
Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals. Herein, we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31 (SAPO-31) as a highly active, chemoselective, and reusable catalyst for hydrodeoxygenation of vanillin. Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed, without forming strong palladium-palladium metallic bonding, over the SAPO-31 support. This catalyst, with a full metal availability to the reactants, exhibits exceptional catalytic activity (TOF: 3,000 h −1 , Yield: > 99%) in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol (MMP) under mild conditions (1 atm, 80 °C, 30 min), along with excellent stability, scalability (up to 100-fold), and wide substrate scope. The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters, as well as the strong metal-support interactions. This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.
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