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1.
Environ Sci Technol ; 57(8): 3334-3344, 2023 02 28.
Article in English | MEDLINE | ID: mdl-36734031

ABSTRACT

Accelerating the rate-limiting Fe3+/Fe2+ circulation in Fenton reactions through the addition of reducing agents (or co-catalysts) stands out as one of the most promising technologies for rapid water decontamination. However, conventional reducing agents such as hydroxylamine and metal sulfides are greatly restricted by three intractable challenges: (1) self-quenching effects, (2) heavy metal dissolution, and (3) irreversible capacity decline. To this end, we, for the first time, introduced redox-active polymers as electron shuttles to expedite the Fe3+/Fe2+ cycle and promote H2O2 activation. The reduction of Fe3+ mainly took place at active N-H or O-H bonds through a proton-coupled electron transfer process. As electron carriers, H atoms at the solid phase could effectively inhibit radical quenching, avoid metal dissolution, and maintain long-term reducing capacity via facile regeneration. Experimental and density functional theory (DFT) calculation results indicated that the activity of different polymers shows a volcano curve trend as a function of the energy barrier, highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap, and vertical ionization potential. Thanks to the appropriate redox ability, polyaniline outperforms other redox-active polymers (e.g., poypyrrole, hydroquinone resin, poly(2,6-diaminopyridine), and hexaazatrinaphthalene framework) with a highest iron reduction capacity up to 5.5 mmol/g, which corresponds to the state transformation from leucoemeraldine to emeraldine. Moreover, the proposed system exhibited high pollutant removal efficiency in a flow-through reactor for 8000 bed volumes without an obvious decline in performance. Overall, this work established a green and sustainable oxidation system, which offers great potential for practical organic wastewater remediation.


Subject(s)
Hydrogen Peroxide , Iron , Iron/chemistry , Hydrogen Peroxide/chemistry , Reducing Agents , Electrons , Oxidation-Reduction
2.
Hepatology ; 73(5): 1764-1782, 2021 05.
Article in English | MEDLINE | ID: mdl-32869873

ABSTRACT

BACKGROUND AND AIMS: Long noncoding RNAs (lncRNAs) are involved in almost every stage of tumor initiation and progression. Here, we have identified an antisense lncRNA, LINC00624, that arises from the antisense strand of chromo-domain-helicase-DNA-binding protein 1-like (CHD1L), located on chr1q21.1, with significant copy number gain and transcriptional activation of CHD1L and B-cell CLL/lymphoma 9 protein (BCL9), in hepatocellular carcinoma (HCC). APPROACH AND RESULTS: Overexpression of LINC00624 enhances tumor growth and metastasis in vitro and in vivo. Mechanistically, higher levels of LINC00624 strengthen the interaction between histone deacetylase 6 (HDAC6) and tripartite motif containing 28 (TRIM28), which accelerates HDAC6 ubiquitination and degradation. Moreover, LINC00624 binds to the RBCC domain of TRIM28, inhibits trimer formation, and weakens the interaction between TRIM28 and zinc finger protein 354C (ZNF354C). Thus, LINC00624 overexpression disrupts the formation of the HDAC6-TRIM28-ZNF354C transcriptional corepressor complex, resulting in the dissociation of the complex from the promoter of CHD1L and BCL9, thereby removing transcription inhibition. CONCLUSIONS: Our findings suggest that LINC00624 acts as a molecular decoy that sequesters the HDAC6-TRIM28-ZNF354C transcriptional corepressor complex away from the specific genomic loci, and that it can potentially be a therapeutic target in HCC.


Subject(s)
Carcinoma, Hepatocellular/pathology , Histone Deacetylase 6/metabolism , Liver Neoplasms/pathology , RNA, Long Noncoding/metabolism , Repressor Proteins/metabolism , Tripartite Motif-Containing Protein 28/metabolism , Carcinoma, Hepatocellular/metabolism , Disease Progression , Gene Expression Regulation, Neoplastic , Humans , Liver Neoplasms/metabolism , Transcription Factors/metabolism
3.
Water Environ Res ; 92(9): 1363-1375, 2020 Sep.
Article in English | MEDLINE | ID: mdl-32159886

ABSTRACT

Peroxymonosulfate (PMS) heterogeneous activation by Co3 O4 -modified catalyst has shown significant implications to generate free radicals for organic pollutants degradation in water. In this study, PMS heterogeneous activation was applied to degrade atrazine (ATZ) using Co3 O4 -mediated titanium dioxide nanoparticles (Co3 O4 /TiO2 NPs), which were synthesized by sol-gel method. Firstly, characteristics of the fresh and used Co3 O4 /TiO2 NPs were analyzed via SEM, TEM, XRD, EDS, and XPS techniques. Then, the influences of several key parameters (i.e., Co3 O4 /TiO2 NPs dose (0.02-0.3 g/L), PMS dose (0-0.6 mM), initial pH (3.0-11.0), and co-existing anions) on the ATZ degradation were investigated systematically. Besides, control systems were set up to verify the high efficiency of Co3 O4 /TiO2 NPs. In addition, the radical scavenging experiments revealed that sulfate and hydroxyl radicals were generated in the Co3 O4 /TiO2 -PMS system, while sulfate radicals were the dominant reactive species responsible for ATZ degradation. Furthermore, the stability and reusability of the Co3 O4 /TiO2 NPs were investigated after four consecutive experiments. Based on the identified products, possible degradation pathways of ATZ in the Co3 O4 /TiO2 -PMS system were proposed. Finally, the possible reaction mechanism of Co3 O4 /TiO2 -PMS system was proposed according to the comprehensive analysis. Findings of this study provided useful information for the application of Co3 O4 /TiO2 NPs in recalcitrant organic contaminants degradation. PRACTITIONER POINTS: Co3 O4 /TiO2 NPs were synthesized via the simple sol-gel method. Co3 O4 /TiO2 NPs possessed excellent catalytic performance for PMS to eliminate ATZ. Sulfate radicals play a dominant role in the degradation of ATZ. ATZ degradation pathways and reaction mechanism in the system were proposed.


Subject(s)
Atrazine , Water Pollutants, Chemical , Peroxides , Solutions , Titanium , Water , Water Pollutants, Chemical/analysis
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