The question of whether Fe(IV) or SO4 •– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered. In this study, besides Fe(IV), SO4 •– and HO• were shown to be produced in the Fe(II)/PDS process by using multiple probes [dimethyl sulfoxide, methyl phenyl sulfoxide, p-nitrobenzoic acid (p-NBA), and benzoic acid (BA)]. The removal of p-NBA and BA and the influence of BA on the yield of methyl phenyl sulfone (PMSO2) indicated that the major oxidizing intermediate changed from Fe(IV) to SO4 •–/HO• with an increase in the PDS/Fe(II) molar ratio at pH 3.0. Fe(IV), SO4 •–, and HO• were all involved in this process at pH 3.0–6.5, but their available amounts that contributed to abating organic contaminants decreased with an increase in pH considering the influence of pH on the generation of PMSO2 and p-hydroxybenzoic acid. Furthermore, Fe(IV), SO4 •–, and HO• contributed differently to abating different organic contaminants because of the different reactivities of these oxidizing oxidants toward different organic contaminants. Overall, this study demonstrates that multiple oxidizing species [Fe(IV), SO4 •–, and HO•] are generated in the Fe(II)/PDS process, which was significant for the application of this process and understanding the mechanisms of Fe(II)-activated peroxide processes.
The iron(II)-activated peroxymonosulfate [Fe(II)/ PMS] process is effective in degrading organic contaminants with a rapid oxidation stage followed by a slow one. Nevertheless, prior studies have greatly underestimated the degradation rates of organic contaminants in the rapid oxidation stage and ignored the differences in the kinetics and mechanism of organic contaminants degradation in these two oxidation stages. In this work, we investigated the kinetics and mechanisms of organic contaminants in this process under acidic conditions by combining the stoppedflow spectrophotometric method and batch experiments. The organic contaminants were rapidly oxidized with rate constants of 0.18−2.9 s −1 in the rapid oxidation stage. Meanwhile, both Fe(IV) and SO 4•− were active oxidants and contributed differently to the degradation of different organic contaminants in this stage. Additionally, the presence of Cl − promoted the degradation of both phenol and estradiol but the effects of Br − and humic acid on phenol degradation differed from those on estradiol degradation in the rapid oxidation stage. In contrast, the degradation of phenol and estradiol was slow and the amounts of Fe(IV) and SO 4•− generated were small in the slow oxidation stage. This work updates the fundamental understanding of the degradation of organic contaminants in this process.
The past two decades have witnessed the rapid development and wide application of Fe(VI) in the field of water de-contamination because of its environmentally benign character. Fe(VI) has been mainly applied as a highly efficient oxidant/disinfectant for the selective elimination of contaminants. The in situ generated iron(III) (hydr)oxides with the function of adsorption/coagulation can further increase the removal of contaminants by Fe(VI) in some cases. Because of the limitations of Fe(VI) per se, various modified methods have been developed to improve the performance of Fe(VI) oxidation technology. Based on the published literature, this paper summarized the current views on the intrinsic properties of Fe(VI) with the emphasis on the self-decay mechanism of Fe(VI). The applications of Fe (VI) as a sole oxidant for decomposing organic contaminants rich in electron-donating moieties, as a bi-functional reagent (both oxidant and coagulant) for eliminating some special contaminants, and as a disinfectant for inactivating microorganisms were systematically summarized. Moreover, the difficulties in synthesizing and preserving Fe(VI), which limits the large-scale application of Fe (VI), and the potential formation of toxic byproducts during Fe(VI) application were presented. This paper also systematically reviewed the important nodes in developing methods to improve the performance of Fe(VI) as oxidant or disinfectant in the past two decades, and proposed the future research needs for the development of Fe(VI) technologies.
The sequence of anterior pituitary deficiencies in Chinese primary LYH patients was atypical (LH/FSH>TSH>ACTH>IGF-1 axis deficiency). A pharmacological dose of glucocorticoids was significantly associated with the improved anterior pituitary insufficiency.
Postoperative abdominal infectious complication (AIC) is associated with metastasis in locally advanced gastric cancer (GC) patients after radical gastrectomy. However, the underlying mechanism remains unclear. Herein, we report that neutrophil extracellular traps (NETs), the DNA meshes released by neutrophils in response to infection, could promote GC cells proliferation, invasion, migration and epithelial–mesenchymal transition dependent on TGF-β signaling. Then we model nude mice with cecal puncture without ligation to simulate postoperative AIC and find that NETs in peripheral blood and ascites fluid facilitate GC cells extravasation and implantation into liver and peritoneum for proliferation and metastasis. Notably, TGF-β signaling inhibitor LY 2157299 could effectively impede liver and peritoneal metastasis but not concurrently aggravate sepsis in those AIC-bearing nude mice. These findings implicate that targeting downstream effectors of NETs such as TGF-β signaling might provide potential therapeutic prospect to reduce the risk of GC metastasis.
Although intermediate manganese species can be generated during the reactions of permanganate (Mn(VII)) with organic pollutants in water, the role of the in situ generated MnO2 colloids in the Mn(VII) oxidation process remained controversial and the contribution of Mn(III) was largely neglected. This study showed that the apparent second-order rate constants (k app) of Mn(VII) oxidation of methyl phenyl sulfoxide and carbamazepine remained constant with time. However, the degradation of four selected phenolic contaminants by Mn(VII) exhibited an autoaccelerating trend and a linear trend at pH 3.0–6.0 and pH 7.0–9.0, respectively. Multiple lines of evidence revealed that the occurrence of the autoaccelerating trend in the Mn(VII) oxidation process was ascribed to the oxidation of the phenolic organics by MnO2 colloids. The influence of pyrophosphate on the oxidation of different organic contaminants by MnO2 colloids suggests that Mn(III) was also responsible for the autoaccelerating oxidation of organic contaminants by Mn(VII) under specific reaction conditions. The kinetic models revealed that the overall contributions of MnO2 colloids and Mn(III) ranged within 6.6–67.9% during the autoaccelerating oxidation of phenolic contaminants by Mn(VII). These findings advance the understanding of the roles of MnO2 colloids and Mn(III) in the Mn(VII) oxidation process.
Background Gastric cancer (GC) remains a refractory cancer worldwide. Currently, exploring the differences of the immune status in GC patients with different subgroups might provide promising immunotherapeutic approaches for the treatment of GC. Methods In this study, a total of 598 surgically resected FFPE primary gastric cancer samples were assessed for FOXP3, CD163, CD3, CD8, and PD-L1 markers. The correlations between the immune markers expression and clinicopathological features and prognosis were investigated retrospectively. Results In general, PD-L1, CD3, and CD8 could be regarded as favorable prognostic factors. Our data demonstrated that high infiltration of FOXP3 + Treg indicates better prognosis in stage I–II patients, while the converse outcome was noted in stage III–IV patients. Our data also confirmed different prognostic value in different pathological classifications, chemotherapy strategies, and locations, with or without lymph node metastasis. Also, M2 macrophages indicated poor prognosis in general. However, high M2 macrophage infiltration suggests a favorable prognosis in signet ring cell carcinoma and mucinous adenocarcinoma. Moreover, the prognostic value of the two indices when they are combined is reported. Conclusions These results suggested that different immune statuses are exhibited in different subgroups of GC, which may direct further understanding of the immune status of GC as well as provide a further theoretical basis and potential targets for GC immunotherapy. Electronic supplementary material The online version of this article (10.1186/s12967-019-1929-9) contains supplementary material, which is available to authorized users.
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