科研成果

{BACKGROUND: Globally, toxic metal exposures are a well-recognized risk factor for many adverse health outcomes. DNA methylation-based measures of biological aging are predictive of disease, but have poorly understood relationships with metal exposures. OBJECTIVE: We performed a pilot study examining the relationships of 24-h urine metal concentrations with three novel DNA methylation-based measures of biological aging: DNAmAge, GrimAge, and PhenoAge. METHODS: We utilized a previously established urine panel of five common metals [arsenic (As), cadmium (Cd), lead (Pb), manganese (Mn), and mercury (Hg)] found in a subset of the elderly US Veterans Affairs Normative Aging Study cohort (N = 48). The measures of DNA methylation-based biological age were calculated using CpG sites on the Illumina HumanMethylation450 BeadChip. Bayesian Kernel Machine Regression (BKMR) was used to determine metals most important to the aging outcomes and the relationship of the cumulative metal mixture with the outcomes. Individual relationships of important metals with the biological aging outcomes were modeled using fully-adjusted linear models controlling for chronological age, renal function, and lifestyle/environmental factors. RESULTS: Mn was selected as important to PhenoAge. A 1 ng/mL increase in urine Mn was associated with a 9.93-year increase in PhenoAge (95%CI: 1.24, 18.61

Biofilm, community of bacteria ubiquitously present in natural environment, may interact with plastic particles and affect the transport of plastic particles in environment. The significance of biofilm (Escherichia coli) on the transport and deposition behaviors of three different sized plastic particles (0.02 μm NPs, 0.2 μm MP and 2 μm MP) were examined under both 10 mM and 50 mM NaCl solutions by comparing the breakthrough curves and retained profiles of plastic particles in bare sand versus those in biofilm-coated sand. Regardless of ionic strengths, the presence of biofilm increases the deposition of all three sized plastic particles in porous media. Via employing X-ray microtomography imaging (XMT) and Scanning electron microscope (SEM), we find that the presence of biofilm could narrow the flow path especially near to the inlet of the column and increase the surface roughness of porous media (by decreasing DLVO repulsive interaction), which contributes to the enhanced the deposition of plastic particles. Extracellular polymeric substances (EPS) present on the biofilm are found to contribute to the enhanced deposition of plastic particles. Packed column experiments, quartz crystal microbalance with dissipation (QCM-D) as well as parallel plate flow chamber experiments all show that three major components of EPS, proteins, polysaccharide, and humic substances all contribute to the enhanced deposition of plastic particles. O–H and N–H groups present on cell surfaces are highly likely to form hydrogen bond with plastic particles and increase the deposition plastic particles. Elution experiments show that decreasing solution ionic strength could release small portion of plastic particles from both bare and biofilm-coated sand columns especially from the segments near to the column inlet (with slighter lower percentage from biofilm-coated columns based on the total mass of retained plastics). In contrast, increasing flow rate does not obviously detach the plastic particles that already deposited onto porous media. The results of this study clearly show that the presence of biofilm in natural environment could enhance the deposition and decrease the transport of plastic particles. © 2020

In this study, natural chalcopyrite (NCP) was employed in the activation of peroxymonosulfate (PMS) for bisphenol S (BPS) degradation. Firstly, the NCP catalyst was characterized via X-ray diffraction (XRD), scanning electron microscopy and energy dispersive spectroscopy (SEM-EDS) techniques. Then, several key parameters such as catalyst dosage, PMS dosage and initial pH were investigated in NCP/PMS system. Furthermore, the transformation of various free radicals (SO4•−, •OH and O2•−) with the changes of initial pH were investigated by quenching experiments and electron spin resonance (ESR) study. Also, sulfur species cycling of copper and iron species were investigated via exogenous Cu2+ and Fe3+ addition experiments and X-ray photoelectron spectroscopy (XPS) analysis, the result indicated that sulfur species promoted Fe3+/Fe2+ and Cu2+/Cu+ cycles on the NCP surface. Furthermore, thirteen major degradation intermediates of BPS were detected by UPLC-QTOF-MS/MS and density functional theory (DFT) method was used to illustrate possible reaction pathways of BPS. Finally, a reasonable reaction mechanism of NCP/PMS system for BPS degradation was proposed on the basis of the comprehensive analysis. In brief, this work helps to provide useful information for the application of natural metallic sulfide minerals in treatment of contaminated waters.

Organic Matter (OM) with different molecular weight and functional groups can impact the adsorptive removal of metal ions, and the influence trend can be facilitated, inhibited or unchanged. However, the association capabilities of different ligands were superficially expounded. Based on the sorption behavior of Cr(III) onto titanate nanotubes (TNTs) with coexisting citric acid (CA), humic acid (HA) and fulvic acid (FA), this study highlighted differential absorbance and DFT simulations to quantitatively detect the mutual effect. As results, adsorption capacities of Cr(III) obviously enhanced from ca. 60 mg/g to 85 mg/g with CA or FA; while HA can slightly promote Cr(III) adsorption. UV spectra scanning proved that FA and HA led to the remarkable red shift of peak A1 (232 nm), A2 (262 nm), A3 (295 nm), A4 (431 nm) of Cr(III), and the area ratio of A2/A3 followed the order Cr-HA > Cr-FA > Cr-CA ≈ Cr. DFT calculations further confirmed that the simultaneous formation of ligand-metal-adsorbents complex and electrostatic effect promoted Cr(III) adsorption, with binding energies of −202.9   −420.8 kJ/mol and − 3958 kJ/mol, respectively. Meanwhile, the bridge connection of OM mainly appeared in the outer sphere of TNTs, as the larger molecular scale prevented their insertion into the inner spacing of TNTs, especially for HA and FA. Therefore, the adsorption mechanism was the combined actions of electrostatic attraction, bridge connection of OM and steric effect. This study can give insights into OM effects on metal adsorption, and quantificationally describe the junction state of ternary complex.

Sulfachloropyridazine (SCP) was commonly used as a broad-spectrum sulfonamide antibiotic and hard to be removed through traditional sewage treatment process. In this study, we developed a simple and controllable strategy to realize in-situ construction of Co(OH)2 nanoparticles decorated urchin-like WO3 (Co(OH)2/WO3), which could efficiently remove SCP through peroxymonosulfate (PMS) activation. Some tiny nanoparticles of Co(OH)2 decorated on the spines/nanorods or surfaces of urchin-like WO3 by transmission electron microscopy (TEM) analysis. The obtained 10 wt% Co(OH)2/WO3 realized completely removal of SCP (degradation efficiency 100%) with a high reaction rate constant (k1) of 0.88 min−1 within 3 min at optimal pH 7. That was because the urchin-like WO3 with numerous adsorption functional groups on its surface (e.g., W = O and –OH bonds) could adsorb the Co2+ easily to form CoOH+, which was perceived the rate-limiting step for PMS activation and generating radicals. Radical quenching experiments indicated that SO4•− played a more significant role than HO• radicals. Density functional theory (DFT) calculation revealed that the atoms of SCP with high Fukui index (f−) were active sites, which preferred to be attacked by the electrophilic SO4•− and HO• radicals. The toxicity of the intermediates by SCP degradation was evaluated by quantitative structure–activity relationship (QSAR) prediction through Toxicity Estimation Software Tool (T.E.S.T.). The possible degradation pathway and catalytic mechanism for SCP removal were proposed. Considering the good catalytic properties of Co(OH)2/WO3-PMS, the material will show great application potential in the removal of emerging contaminants in water.

China submitted the Greenhouse gas emission reduction target in the form of Nationally Determined Contributions (NDC) to the Paris Agreement. To reduce the negative impact of global warming, a tighter target is needed, such as the 2-degree target. This study investigated how China could reach its emissions peak and decarbonize its economy through different key countermeasures in various sectors in line with the NDC and 2 degrees C targets by 2030. A dynamic CGE model is used to develop ten scenarios that contain two dimensions consisting of two stringency levels of carbon emission limitation and the availability of different low-carbon options. We found that in the baseline scenario, China's total CO2 emissions in 2030 would reach 14.7 Gt. To meet China's NDC target, it is essential to develop non-fossil fuel energy, restrict the over-expansion of energy-intensive industries and improve end-use efficiency. Meanwhile, the global 2 degrees C target poses higher requirements for China to develop various non-fossil technologies both in electricity production and demand sectors, and vigorously promote low-carbon consumption pattern. Furthermore, we estimated the economic impacts and found that if low-carbon measures are adopted properly, the mitigation cost in 2030 could decline by 92 and 226 USD/ton-CO2 under the NDC target and 2 degrees C target, respectively. Accordingly, GDP loss could fall from 3.8% to barely 0.004% under the NDC target, and from 11.6% to 1.6% under the 2 degrees C target. The welfare will almost not be affected significantly under all scenarios. Moreover, carbon reduction will also bring co-benefits on the air pollution improvement in China. (c) 2020 Elsevier Ltd. All rights reserved.

© 2019 Elsevier B.V. Carbon utilization and storage (CCUS) project represented by enhanced oil recovery (EOR) technology provides a feasible way for the CCS dynamic cost to decline. With the development of CCS and the cost reduction of power plant capture, the possibility of oil companies receiving CO2 from power plants will increase, which makes CO2 and oil resources more fully utilized. Based on this fact, this work proposes a novel model regarding the CCS–EOR project to systematically evaluate the CCS development path and the EOR utilization process. By considering the CO2 source captured by CCS and the utilization process of EOR process, the cost-benefit model of integrated system is established, and the CO2 capture/injection path of CCS/EOR is optimized. This model helps to analyze CCS investment and carbon capture process from the perspective of the whole project process, and provides a feasible reference for practical large-scale engineering decision-making project.