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Electrocatalyst engineering from the atomic to macroscopic level of electrocatalysts is one of the most powerful routes to boost the performance of electrochemical devices. However, multi-scale structure engineering mainly focuses on the range of atomic-to-particle scale such as hierarchical porosity engineering, while catalyst engineering at the macroscopic level, such as the arrangement configuration of nanoparticles, is often overlooked. Here, a 2D carbon polyhedron array with a multi-scale engineered structure via facile chemical etching, ice-templating induced self-assembly, and high-temperature pyrolysis processes is reported. Controlled phytic acid etching of the carbon precursor introduces homogeneous atomic phosphorous and nitrogen doping, as well as a well-defined mesoporous structure. Subsequent ice-templated self-assembly triggers the formation of a 2D particle array superstructure. The atomic-level doping gives rise to high intrinsic activity, while the well-engineered porous structure and particle arrangement addresses the mass transport limitations at the microscopic particle level and macroscopic electrode level. As a result, the as-prepared electrocatalyst delivers outstanding performance toward oxygen reduction reaction in both acidic and alkaline media, which is better than recently reported state-of-the-art metal-free electrocatalysts. Molecular dynamics simulation together with extensive characterizations indicate that the performance enhancement originates from multi-scale structural synergy.
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The present study proposes a novel engineering concept for the customization of functionality and construction of superstructure to fabricate 2D monolayered N-doped carbon superstructure electrocatalysts decorated with Co single atoms or Co2P nanoparticles derived from 2D bimetallic ZnCo-ZIF superstructure precursors. The hierarchically porous carbon superstructure maximizes the exposure of accessible active sites, enhances electron/mass transport efficiency, and accelerates reaction kinetics simultaneously. Consequently, the Co single atoms embedded N-doped carbon superstructure (Co-NCS) exhibits remarkable catalytic activity toward oxygen reduction reaction, achieving a half-wave potential of 0.886 V versus RHE. Additionally, the Co2P nanoparticles embedded N-doped carbon superstructure (Co2P-NCS) demonstrates high activity for both oxygen evolution reaction and hydrogen evolution reaction, delivering low overpotentials of 292 mV at 10 mA cm-2 and 193 mV at 10 mA cm-2 respectively. Impressively, when employed in an assembled rechargeable Zn-air battery, the as-prepared 2D carbon superstructure electrocatalysts exhibit exceptional performance with a peak power density of 219 mW cm-2 and a minimal charge/discharge voltage gap of only 1.16 V at 100 mA cm-2. Moreover, the cell voltage required to drive an overall water-splitting electrolyzer at a current density of 10 mA cm-2 is merely 1.69 V using these catalysts as electrodes.
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Stochastic Configuration Network (SCN) has a powerful capability for regression and classification analysis. Traditionally, it is quite challenging to correctly determine an appropriate architecture for a neural network so that the trained model can achieve excellent performance for both learning and generalization. Compared with the known randomized learning algorithms for single hidden layer feed-forward neural networks, such as Randomized Radial Basis Function (RBF) Networks and Random Vector Functional-link (RVFL), the SCN randomly assigns the input weights and biases of the hidden nodes in a supervisory mechanism. Since the parameters in the hidden layers are randomly generated in uniform distribution, hypothetically, there is optimal randomness. Heavy-tailed distribution has shown optimal randomness in an unknown environment for finding some targets. Therefore, in this research, the authors used heavy-tailed distributions to randomly initialize weights and biases to see if the new SCN models can achieve better performance than the original SCN. Heavy-tailed distributions, such as Lévy distribution, Cauchy distribution, and Weibull distribution, have been used. Since some mixed distributions show heavy-tailed properties, the mixed Gaussian and Laplace distributions were also studied in this research work. Experimental results showed improved performance for SCN with heavy-tailed distributions. For the regression model, SCN-Lévy, SCN-Mixture, SCN-Cauchy, and SCN-Weibull used less hidden nodes to achieve similar performance with SCN. For the classification model, SCN-Mixture, SCN-Lévy, and SCN-Cauchy have higher test accuracy of 91.5%, 91.7% and 92.4%, respectively. Both are higher than the test accuracy of the original SCN.
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BACKGROUND: The role of estrogen receptor alpha (ERa), estrogen receptor beta (ERb) and ERa36 signaling in hepatocellular carcinoma (HCC) is not fully addressed. METHODS: In this study, three cohorts were included: (i) primary HCC patients (N = 76, cohort P), (ii) colorectal liver metastasis (mCRC) (N = 32, cohort S), and (iii) HCC from The Cancer Genome Atlas (TCGA) (N = 121). The levels of ERa36 and wtER36 were measured and their correlation with clinicopathologic features was determined. RESULTS: WtERa was downregulated and that ERa36 was upregulated in tumor tissues in both cohort P and TCGA data set. ERa36 was downregulated in tumor tissues in cohort S. In cohort P, wtERa was differentially expressed in gender (P < 0.000), age (P = 0.004), tumor number (P = 0.043), tumor size (P = 0.002), intrahepatic recurrence (P = 0.054). ERa36 was unequally expressed in different non-tumor liver status (P = 0.040). WtERa was negatively associated with overall survival (OS) and disease free survival (DFS) in cohort P. Compared with non-tumor tissues, the expression of ERa36 was increased in primary HCC but decreased in secondary HCC, showing opposite expression patterns of ERa36 between primary HCC and secondary HCC. CONCLUSIONS: Primary HCC is associated with the decreased WtERa but increased ERa36. The expression pattern of ERa36 is different between primary HCC and secondary HCC, as the former with the increased ERa36 but the latter with the decreased ERa36. Therefore, the expression of ERa36 may be used to differentiate the primary HCC and the secondary one.
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Empalme Alternativo , Carcinoma Hepatocelular/genética , Neoplasias Colorrectales/genética , Receptor alfa de Estrógeno/genética , Regulación Neoplásica de la Expresión Génica , Neoplasias Hepáticas/genética , Biomarcadores de Tumor , Carcinoma Hepatocelular/patología , Carcinoma Hepatocelular/terapia , Estudios de Cohortes , Neoplasias Colorrectales/patología , Neoplasias Colorrectales/terapia , Terapia Combinada , Femenino , Estudios de Seguimiento , Humanos , Técnicas para Inmunoenzimas , Neoplasias Hepáticas/secundario , Neoplasias Hepáticas/terapia , Metástasis Linfática , Masculino , Persona de Mediana Edad , Clasificación del Tumor , Invasividad Neoplásica , Recurrencia Local de Neoplasia/genética , Recurrencia Local de Neoplasia/patología , Recurrencia Local de Neoplasia/terapia , Estadificación de Neoplasias , Pronóstico , Tasa de SupervivenciaRESUMEN
A novel dual-outward contraction mechanism is applied to construct 2D hollow carbon superstructures (HCSs) via pyrolysis of hybrid ZIF superstructures. One outward contraction stress is offered by the in situ formed thin carbon shell, while another originates from the interconnected facets of ZIF polyhedra within the ZIF superstructure.
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Maximizing the utilization efficiency of monatomic Fe sites in Fe-N-C catalysts poses a significant challenge for their commercial applications. Herein, a structural and electronic dual-modulation is achieved on a Fe-N-C catalyst to substantially enhance its catalytic performance. We develop a facile multi-component ice-templating co-assembly (MIC) strategy to construct two-dimensional (2D) arrays of monatomic Fe-anchored hollow carbon nanoboxes (Fe-HCBA) via a novel dual-outward interfacial contraction hollowing mechanism. The pore engineering not only enlarges the physical surface area and pore volume but also doubles the electrochemically active specific surface area. Additionally, the unique 2D carbon array structure reduces interfacial resistance and promotes electron/mass transfer. Consequently, the Fe-HCBA catalysts exhibit superior oxygen reduction performance with a six-fold enhancement in both mass activity (1.84 A cm-2) and turnover frequency (0.048 e- site-1 s-1), compared to microporous Fe-N-C catalysts. Moreover, the incorporation of phosphorus further enhances the total electrocatalytic performance by three times by regulating the electron structure of Fe-N4 sites. Benefitting from these outstanding characteristics, the optimal 2D P/Fe-HCBA catalyst exhibits great applicability in rechargeable liquid- and solid-state zinc-air batteries with peak power densities of 186 and 44.5 mW cm-2, respectively.
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To evaluate the early changes in ganglion cell-inner plexiform layer thickness and macular microvasculature in Posner-Schlossman syndrome (PSS) with a binocular control study involving optical coherence tomography angiography (OCTA). Twenty-six patients with unilateral PSS were included in this cross-sectional study. All subjects underwent a thorough ocular examination. Macular ganglion cell-inner plexiform layer (mGCIPL) and superficial macular microvasculature measurements, including vessel density (VD), perfusion density (PD) and the foveal avascular zone (FAZ), were recorded. In PSS-affected eyes, the mGCIPL thickness was significantly lower in all quadrants than in the contralateral eyes (all p < 0.05). Significant macular microvascular damage was found in the PSS-affected eyes, including whole-image VD (wiVD), wiPD, perifoveal VD (periVD) and periPD (all p < 0.05); but there was no obvious difference in parafoveal VD (paraVD), paraPD and FAZ parameters (all p > 0.05). In addition, a decreased wiVD and wiPD were significantly correlated with a smaller mGCIPL thickness and a decreased MD (all p < 0.05). These parameters may contribute to the early detection of glaucomatous damage and timely supervision of disease progression in PSS.
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Increasing the exposure of active sites and improving the intrinsic activity are necessary considerations for designing a highly efficient photocatalyst. Herein, an In2S3/AgI stable Z-scheme heterojunction with highly dispersed AgI nanoparticles (NPs) is synthesized by the mild self-templated and in-situ ion exchange strategy. Impressively, the optimized In2S3/AgI-300 Z-scheme heterojunction exhibits superior photodegradation activity (0.020 min-1) for the decomposition of insecticide imidacloprid (IMD), which is extremely higher than that of pure In2S3 (0.002 min-1) and AgI (0.013 min-1). Importantly, the three-dimensional excitation-emission matrix (3D EEMs) fluorescence spectra, high-resolution mass spectrometry (HRMS), the photoelectrochemical tests, radical trapping experiment, and electron spin resonance (ESR) technique are performed to clarify the possible degradation pathway and mechanism of IMD by the In2S3/AgI-300 composite. The enhanced photocatalytic performance is attributed to the highly dispersed AgI NPs on hierarchical In2S3 hollow nanotube and the construction of In2S3/AgI Z-scheme heterojunction, which can not only increase active site exposure, but also improve its intrinsic activity, facilitating rapid charge transfer rate and excellent electron-hole pairs separation efficiency. Meanwhile, the practical application potential of the In2S3/AgI-300 composite is systematically investigated. This study opens a new insight for designing catalysts with high photocatalytic performance through a convenient approach.
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It is challenging to explore novel-structure lanthanide coordination polymers (Ln-CPs) for sensing environmental pollutants. Herein, we designed and synthesized an organic bridging linker 3-(carboxymethoxy)-1-(carboxymethyl) pyrazole-4-carboxylic acid (H3ccpc), and then successfully prepared and characterized a novel Ln-CP, namely [Tb2(ccpc)2(H2O)6]·1.5H2O (ccpcTb). Structural analysis indicates that ccpcTb exhibits a two-dimensional structure, in which Tb ions are in an eight-coordinated environment. The photoluminescence performance of ccpcTb was discussed in detail. The ccpcTb displays bright green luminescence and behaves as a multi-responsive luminescent sensor toward Fe3+ ions, Cr2O72- ions and 2,4,6-trinitrophenol with high selectivity and low detection limits. Furthermore, the possible luminescence sensing mechanisms have been addressed in detail. The luminescence quenching mechanism of sensing Fe3+ and Cr2O72- is attributed to the energy competitive absorption, while that of sensing TNP is due to the synergistic effect of energy competitive absorption and photo-induced electron transfer.
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Due to the poor bifunctional electrocatalytic performances of electrocatalysts in zinc-air battery, herein, we first synthesized Ni/Ni12P5@CNx Mott-Schottky heterojunction to ameliorate the high-cost and instability of precious metals. We modulated the different contents of Ni and Ni12P5 in the Ni/Ni12P5@CNx Mott-Schottky heterojunction, and found that 0.6 Ni/Ni12P5@CNx has outstanding electrocatalytic performances, with half-wave potential of 0.83 V, and OER potential of 1.49 V at 10 mA cm-2. Also, the ΔE value is only 0.66 V. Moreover, 0.6 Ni/Ni12P5@CNx is assembled into ZAB, which has a high power density of 181 mW cm-2 and a high specific capacity of 710 mAh g-1. This indicates it has a good cycle stability. The density functional theory (DFT) calculations reveal that electrons spontaneously flow from Ni to Ni12P5 through the formed buffer layer in the Ni/Ni12P5@CNx Mott-Schottky heterojunction. The Schottky barrier formed modulates the electrocatalytic pathway to have good bifunctional electrocatalytic activity for ORR and OER.
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Aim: Altered long noncoding RNA (lncRNA) and mRNA is vital in the progression from Helicobacter pylori (H. pylori, HP) infection to gastric cancer (GC) and mucosa-associated lymphoid tissue (MALT) lymphoma. Materials & methods: Five independent Gene Expression Omnibus datasets (GSE5081, GSE84433, GSE15459, GSE66229 and GSE25638) were included in our study. Results: Differentially expressed lncRNAs and mRNAs in both H. pylori-positive gastritis and GC tissues were identified. Using two GC cohorts, the H. pylori-related mRNA DYNC1I1 and MMP7 were independent predictors of overall survival. Moreover, the expressions of lncRNA GHRLOS and 44 mRNAs were significantly changed in gastric MALT lymphoma patients. Conclusion: The lncRNA/mRNA response to H. pylori infection in gastritis and GC influence the outcome of GC and progression of MALT lymphoma.
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Infecciones por Helicobacter/complicaciones , Infecciones por Helicobacter/genética , Helicobacter pylori , Interacciones Huésped-Patógeno/genética , Linfoma de Células B de la Zona Marginal/etiología , Neoplasias Gástricas/etiología , Transcriptoma , Biomarcadores , Bases de Datos Genéticas , Susceptibilidad a Enfermedades , Perfilación de la Expresión Génica , Regulación Neoplásica de la Expresión Génica , Infecciones por Helicobacter/microbiología , Humanos , ARN Largo no CodificanteRESUMEN
The nitrogen and phosphorus removal characteristics during the start-up and the long-term operational stability of an anaerobic/anoxic (A/A) ABR coupled aerobic MBR system treating low C/N domestic wastewater were investigated. The results showed that the denitrifying phosphorus bacteria (DPBs) were successfully enriched within 46 d by controlling the nitrate recycling ratio (increasing from 150% to 300%), with a temperature of 30â±2â, volume loading rate of 0.8 kg·(m3·d)-1 and sludge reflux ratio of 80% in the ABR, sludge retention time (SRT) in the denitrifying phosphorus removal functional area of 25 d, and the dissolved oxygen (DO) of 1-2 mg·L-1 in the MBR. The net phosphorus release and phosphorus uptake of DPBs reached 20.56 mg·L-1and 27.74 mg·L-1, respectively. Batch tests demonstrated that about 84.8% of phosphorus-accumulating organisms (PAOs) could use NO3--N as an electron acceptor for denitrifying phosphorus removal. After 50 d of stable operation after the successful system start-up, the average removal rates of COD, NH4+-N, TN, and PO43--P were 91.8%, 99.0%, 71.5%, and 94.2%, respectively. The results also suggested that 0.83 mg·L-1NO3--N was consumed per 1 mg·L-1 PO43--P removed during the denitrifying phosphorus removal, indicating that the simultaneous nitrogen and phosphorus removal was achieved in the ABR-MBR system.
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Reactores Biológicos , Desnitrificación , Fósforo/aislamiento & purificación , Eliminación de Residuos Líquidos , Bacterias , Nitrógeno , Aguas del Alcantarillado , Aguas ResidualesRESUMEN
pH is one of the most important means of control for the realization and stability of the nitrosation system. To study the change rule of pH values of the nitrosation system and the influence of pollution removal and transformation at different pH under the conditions of different C/N (0, 1, 2, 3,4) and sludge concentrations (sludge amount:water content was 1:6, 1:3, 1:1), batch tests were conducted with tapered bottles using sodium acetate as the carbon source and inoculated with mature nitrosation sludge. The results showed that the higher the C/N, the higher the pH increment and the denitrification efficiency at the same sludge concentration. At the same C/N, a higher sludge concentration corresponded to a smaller pH increment but a higher denitrification efficiency. The removal and transformation of carbon and nitrogen was highly correlated with pH changes in the reaction system, and the denitrification and nitrosation reactions were in sequence. Throughout the operational period of the system, as pH increased, the specific organic matter removal rate was 7-16 times as much as when pH decreased. However, as pH decreased, the specific ammonia oxidation rate (SAOR) was 1-20 times that of when pH increased. When pH was less than 6.1, the system lost its ability to oxidize ammonia-nitrogen. The highest removal efficiency of carbon and nitrogen in the system was achieved when C/N was 4. Ammonia transformation 80% COD removal at the three sludge concentrations took 480, 350, and 300 min, respectively. Under different conditions, the proportion of nitrosation in the system remained above 50% and the concentration of NO3--N remained below 5 mg·L-1, which indicated that the system was dominated by nitrosation.
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Reactores Biológicos , Nitrosación , Aguas del Alcantarillado , Eliminación de Residuos Líquidos , Carbono , Desnitrificación , Concentración de Iones de Hidrógeno , NitrógenoRESUMEN
In this work, the effects of the sludge retention time (SRT, 35, 25, or 15 d) and pH (7.5, 8.0, 8.5) on denitrifying phosphorus removal were investigated using denitrifying phosphorus bacteria (DPBs) enriched in a sequencing batch reactor (SBR). The results indicated that shortening the SRT from 35 d to 25 d resulted in a decrease in the mixed liquor volatile suspended solids (MLVSS) from 2821 to 2301 mg·L-1, while the sludge loading rate (F/M) increased from 0.256 kg·(kg·d)-1to 0.312 kg·(kg·d)-1. Although the quantity of net phosphorus release and net phosphorus uptake decreased at this stage, the rates of anaerobic phosphorus release, anoxic phosphorus absorption, and denitrification reached their highest levels with values of 25.07, 15.92, and 9.45 mg·(g·h)-1, respectively, due to the increased sludge activity. Consequently, the phosphorus content of the sludge increased from 4.78% to 5.33%, and the removal rate of PO43--P was stable at above 95% with an average effluent PO43--P concentration below 0.5 mg·L-1. When the SRT was further shortened to 15 d, the MLVSS decreased to values as low as 1448 mg·L-1, and the proportion of DPBs in the phosphorus accumulating organisms (PAOs) decreased from 82.4% to 65.7%, indicating that the DPBs were gradually washed out from the system due to the excessively short SRT. At this stage, the phosphorus content of sludge decreased to 3.43%, while the rates of phosphorus release, phosphorus absorption, and denitrification also decreased to some extent. When the pH was increased (7.5-8.0), the anaerobic phosphorus release rate and the anoxic phosphorus absorption rate also increased, and reached 25.86 mg·(g·h)-1 and 16.62 mg·(g·h)-1, respectively, at a pH of 8.0. When the pH exceeded 8.0, the phosphorus removal efficiency dropped rapidly, supposedly due to phosphorus chemical precipitation.
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Reactores Biológicos , Desnitrificación , Fósforo/aislamiento & purificación , Aguas del Alcantarillado , Concentración de Iones de Hidrógeno , NitrógenoRESUMEN
The effect of volume loading rate (VLR) on denitrifying phosphorus removal was investigated in a continuous-flow ABR-MBR combined process treating domestic wastewater to arrive at optimum process parameters. In the experiment, the VLR of the ABR was set at 0.76, 1.01, 1.51, and 2.27 kg·(m3·d)-1. The removal of carbon, nitrogen, and phosphorus in the system and the effect of the VLR in the MBR on nitrification performance were observed for each VLR of the ABR. The results showed that under the condition when the VLR of the ABR was 1.51 kg·(m3·d)-1, the amount of COD removal in the A2 chamber was the largest, and shortcut nitrification was achieved in the MBR when the VLR of the MBR was 1.51 kg·(m3·d)-1. Meanwhile, the removal efficiency of NH4+-N and TN reached more than 90% and 72%, respectively, the anaerobic P-release and anoxic P-uptake were 7.41 mg·L-1and 15.42 mg·L-1, respectively, and the concentration of PO43--P in effluent was lower than 0.5 mg·L-1, which indicated that the shortcut nitrification was more conducive to strengthening the performance of denitrifying phosphorus removal in the ABR-MBR system.
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Reactores Biológicos , Nitrificación , Fósforo/aislamiento & purificación , Eliminación de Residuos Líquidos , Carbono/aislamiento & purificación , Nitrógeno/aislamiento & purificación , Aguas del Alcantarillado , Aguas ResidualesRESUMEN
In order to solve the problem of declining total nitrogen (TN) removal caused by anaerobic ammonium oxidation (ANAMMOX) and the suppression of organic matter for ANAMMOX, the anaerobic baffled reactor (ABR), inoculating ANAMMOX sludge and anaerobic sludge from a municipal WWTP, was selected to construct system of ANAMMOX coupled denitrification (SAD) by the control of different substrate concentration. The SAD was constructed to study the effects of different influent substrates (COD, NO2--N, NH4+-N) on the performance of nitrogen and carbon removal in the coupled system and pollutant removal rules. The results showed that the coupling reaction was achieved in the ABR reactor and the inhibitory effect of organic compounds on anaerobic ammonium oxidation bacteria (AAOB) was relieved. When influent concentrations of COD, NO2--N, and NH4+-N were 260, 185, and 100 mg·L-1, respectively, which equates to a ratio of 2.6â¶1.85â¶1, the concentrations of these substances in the effluent decreased to 10, 1.0, and 0.9 mg·L-1, respectively. The TN removal rate reached 99%, hence stable system operation and ultra-low emissions of carbon and nitrogen pollutants were achieved. Under different conditions of substrate concentrations and ratios, the targeted pollutants were generally eliminated in the first compartment, in which the removal rate reached higher than 75%, and ANAMMOX held the dominant position in the SAD coupled system.
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Reactores Biológicos , Carbono/aislamiento & purificación , Nitrógeno/aislamiento & purificación , Anaerobiosis , Desnitrificación , Oxidación-Reducción , Aguas del AlcantarilladoRESUMEN
AIM: We performed a study to identify the role of microRNA in thymoma. PATIENTS & METHODS: One hundred twenty-three thymoma patients with clinical information and miRNA expression data from The Cancer Genome Atlas were included in the study. Comprehensive bioinformatics analysis was integrated in our analysis. RESULTS & CONCLUSION: Seven miRNAs were found to be associated with overall survival (p < 0.001). Another four miRNAs were found to be associated with disease-free survival (p < 0.001). Type C thymoma can be distinguished from nontype C thymoma by miRNAs. Interestingly, seven miRNAs showed both prognostic and subtype-specific potential. Our findings suggest that miRNAs can be used for prognostic prediction and subtype stratification.
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Biomarcadores de Tumor/genética , MicroARNs/genética , Timoma/genética , Neoplasias del Timo/genética , Supervivencia sin Enfermedad , Femenino , Humanos , Masculino , Persona de Mediana Edad , Timoma/patología , Neoplasias del Timo/patologíaRESUMEN
The operational control conditions for realizing shortcut nitrification in the membrane bioreactor (MBR) process was investigated in a lab-scale anaerobic baffled reactor (ABR)-MBR combined system, which laid the foundation for further research on the performance of denitrification phosphorus removal in the system. The experimental results under different conditions showed that shortcut nitrification in the MBR was achieved by controlling the dissolved oxygen (DO) concentration to low levels (0.5-1.0 mg·L-1 to 0.3-0.7 mg·L-1) and changing the effective volume of the MBR to control hydraulic retention time (HRT), with the HRT in the ABR equal to 6 h, sludge reflux ratio of 100%, NOx--N reflux ratio of 300%, and temperature of 30â±2â. Finally, the shortcut nitrification deteriorated as the HRT in the MBR increased from 3 h to 5 h, with nitrite accumulation rate dramatically dropping from 60% to 15%. The analysis of the influencing factors of shortcut nitrification showed that maintaining low DO concentration (0.3-0.7 mg·L-1) and gradually shortening HRT were the key factors. The pH, free ammonia (FA), free nitrous acid (FNA), temperature, and sludge retention time (SRT) had a slightly positive effect on shortcut nitrification. During the period of shortcut nitrification, a stable and high efficiency removal of COD and NH4+-N were achieved, and the average concentration of the effluent of COD and NH4+-N, whose removal rates were above 90%, were below 50 mg·L-1 and 2 mg·L-1, respectively, and the removal efficiency of total nitrogen (TN) reached 72%.