基于贝叶斯的苯并(α)芘PBPK模型优化与健康风险评估应用

应用基于生理的药代动力学(PBPK)模型预测苯并(α)芘(BaP)暴露的人体内部剂量,基于贝叶斯的马尔科夫链蒙特卡洛模拟(MCMC)方法对模型参数进行校准和优化,最后运用已优化的模型对BaP内暴露基准值进行推导.研究发现,基于贝叶斯的MCMC方法对模型后验参数校准后,模型精度明显提高,两个数据集验证结果显示残差平方和分别降低了72%和94%.PBPK模型以BaP和子代谢物3-羟基苯并(α)芘(3-OHBaP)的体内动力学过程为结构基础,模拟BaP体内浓度分布大小为脂肪>肾脏>皮肤>缓慢灌注组织>快速灌注组织>静脉血>肝脏;3-OHBaP体内浓度分布大小为肾脏>快速灌注组织>脂肪>肺>静脉血>缓慢灌注组织>肝脏>皮肤.敏感性分析显示,快速灌注组织-血分配系数对模型输出影响最大,灵敏度系数超过了200%;排泄系数影响最小,只有肾小球过滤率K_BR的灵敏度系数超过了1%.以美国国家环境保护局推荐的参考浓度2.0×10^-6mg/m³为外暴露安全基准值,基于PBPK模型推导了职业暴露的BaP生物监测当量(BE),结果显示BE值为0.405pmol/mol肌酐(尿液3-OHBaP平均浓度),为基于人体内暴露剂量水平进行定量健康风险评估奠定了基础.     

介质阻挡放电等离子体老化微塑料及对Zn (II)吸附的影响

为了在实验中缩短微塑料的老化时间,更真实地模拟自然老化条件,采用介质阻挡放电（DBD）等离子体老化聚乙烯微塑料（PE-MP）和聚丙烯微塑料（PP-MP）,同时研究了老化前后PE-MP和PP-MP对Zn （II）的吸附过程和机理.随着放电时间延长和输入电压升高,微塑料表面出现微小裂纹或孔洞,形成含氧官能团.老化后PE-MP和PP-MP对Zn （II）的吸附容量分别提高了22.7%和14.8%.老化前后微塑料对Zn （II）的吸附均符合准二级动力学模型.颗粒内扩散模型表明,Zn （II）在微塑料上的吸附过程可分为快速吸附,慢速吸附和吸附平衡3个阶段.同时,老化前后微塑料对Zn （II）的吸附均符合Langmuir吸附等温线模型.热力学结果表明,微塑料对Zn （II）的吸附是自发的吸热过程.Ca²⁺、腐殖酸和低pH值不利于微塑料对Zn （II）的吸附.     

正渗透去除地表水中DOM的效能研究

采用经砂滤处理后的滆湖水作为原料液,氯化钠溶液作为汲取液,在不同影响因素条件下进行正渗透试验,并对试验后的膜片进行清洗,探究膜污染的可逆性.结果表明:提高汲取液浓度、运行温度及膜面流速均可有效增加膜通量;正渗透对滆湖水体中的溶解性微生物代谢产物、类色氨酸、类富里酸和腐殖酸四种主要DOM成分均有较好的去除效果,DOC、UV₂₅₄截留率均在96%以上;短期运行通过水力清洗几乎可以完全恢复膜通量,而长期运行通过超声清洗可以基本恢复全部膜通量,通过分析膜清洗液可知造成膜污染的主要物质为类色氨酸类和类富里酸类物质.     

因子回归和交互联合探索区域植被覆盖度的影响因素——以三江源地区为例

利用SPOT VEGETATION数据获取的归一化植被指数（NDVI）,分析三江源地区植被覆盖度（FVC）的空间异质性,围绕自然和人类活动因素,基于因子回归与交互作用联合探索自然因素和人为因素对三江源地区植被覆盖的影响.结果表明：（1）三江源地区植被覆盖度整体呈现明显的空间异质性;（2）总体上FVC空间分布的影响因素表现为自然环境因素>人类活动因素;（3）降水是影响三江源地区FVC的主要驱动因子,解释力达0.777;（4）因子交互发现：驱动解释系统呈现双因子增强,说明从系统的角度来看不存在独立起作用的因子,年降水量与其他因子的交互作用最强;（5）降水梯度影响了三江源地区FVC空间异质性的解释程度.随着降水增加,因子解释力趋稳,在降水量较多的三江源东部地区,FVC趋向于更易受高程和气温的影响;（6）数据结果亦验证了因子独立的全局最优筛选仅仅是模拟因变量特征的最优函数,其解释效果与因变量的驱动解释不能完全等同.     

外源硫诱导下的Desulfovibrio desulfuricans sub sp.EPS特性及对Zn(Ⅱ)的吸附

研究了3种外源硫(Na₂SO₄、Na₂SO₃和Na₂S₂O₃·5H₂O)对Desulfovibrio desulfuricans sub sp.(D.desulfuricans sp.)的胞外聚合物(EPS)的胁迫/诱导作用。结果表明,在还原性硫源0.50g/L Na₂SO₃的条件下,EPS产量最高,为2104.39mg/g VSS,蛋白质含量为1888.52mg/g VSS,较胁迫/诱导前均提高了300%以上;其对Zn(Ⅱ)的吸附性能最好,为954.4mg/g EPS,提高了98.17%。三维荧光(3D-EEM)结果表明,胁迫/诱导后EPS中类酪氨酸均大量增加;傅里叶红外光谱(FTIR)结果表明,胁迫后-OH、C=O、C-O-C等官能团均大量增加,在Zn(Ⅱ)的吸附中发挥了重要作用;X光电子能谱(XPS)结果表明,在还原性硫源(Na₂SO₃和Na₂S₂O₃·5H₂O)胁迫/诱导后,EPS中C-O/C-N、C=N和某种含氧基团(X)大量增加,可能是吸附Zn(Ⅱ)的主要基团。     

2016~2020年上海市PM2.5化学组成特征和来源解析

2016~2020年在上海市区和郊区的6个点位开展了颗粒物系统性观测研究,分析了PM_2.5的质量浓度以及水溶性离子、有机碳/元素碳、无机元素等化学组分,并利用正矩阵因子分解模型对PM_2.5的来源进行了解析。结果表明,上海PM_2.5浓度水平呈现下降趋势,年均质量浓度依次为46,43,37,40,39μg/m³,表现为冬高夏低,西高东低的时空分布特征。有机物在PM_2.5中占比最高(30%~32%),不同年份和季节间的差异较小。二次无机离子(硫酸盐、硝酸盐和铵盐)的区域性特征明显,其中硝酸盐的占比在5a间升高最多,且在冬季污染过程中起到了关键作用。解析得到PM_2.5的来源有9类,分别为二次硝酸盐(30.6%)、二次硫酸盐(20.7%)、机动车(12.6%)、工业(8.0%)、生物质燃烧(7.7%)、扬尘(6.5%)、燃煤(5.8%)、海盐(4.8%)和船舶(3.2%)。机动车和船舶等移动源、秸秆焚烧和烟花爆竹燃放等生物质燃烧源的贡献浓度在研究期间呈现下降趋势,体现了相关治理措施的管控效果。     

Ambient volatile organic compounds at a receptor site in the Pearl River Delta region: Variations, source apportionment and effects on ozone formation

We present the continuously measurements of volatile organic compounds（VOCs） at a receptor site（Wan Qing Sha, WQS） in the Pearl River Delta（PRD） region from September to November of 2017. The average mixing ratios of total VOCs（TVOCs） was 36.3 ± 27.9 ppbv with the dominant contribution from alkanes（55.5%）, followed by aromatics（33.3%）. The diurnal variation of TVOCs showed a strong photochemical consumption during daytime,resulting in the formation of ozone（O₃）. Five VOC sources were ...     

Hydrothermal-treated Pt/Al2O3 as an excellent catalyst for toluene total oxidation

The preparation of highly active supported noble metal catalysts with a low noble metal loading has always been the ultimate goal of researchers working on catalysis. Hydrothermally treated Pt/Al₂O₃ (Pt/Al₂O₃-H) exhibits better catalytic activity than that (Pt/Al₂O₃-C) treated via the conventional calcination approach. At the high space velocity of 100,000 mL/(g∙hr), the temperature that correspond to 50% toluene conversion (T₅₀) of Pt/Al₂O₃-H is 115°C lower than that of Pt/Al₂O₃-C, and the turnover frequency (TOF) value can reach 0.0756 sec⁻¹. The mechanism by which the hydrothermal approach enhances Pt/Al₂O₃ activity has been investigated. The structure associated with the high catalytic activity of Pt nanoparticles (NPs) can be retained via hydrothermal treatment. Furthermore, the support is transformed to AlO(OH) with numerous surface hydroxyl groups, which in turn can facilitate the adsorption of toluene. And the synergistic effects of Pt NPs and AlO(OH) increases the contents of Pt in oxidation state and active oxygen, which are beneficial for toluene oxidation.     

Short-term inhalation exposure evaluations of airborne antibiotic resistance genes in environments

Antibiotic resistance is a sword of Damocles that hangs over humans. In regards to airborne antibiotic resistance genes (AARGs), critical knowledge gaps still exist in the identification of hotspots and quantification of exposure levels in different environments. Here, we have studied the profiles of AARGs, mobile genetic elements (MGEs) and bacterial communities in various atmospheric environments by high throughput qPCR and 16S rRNA gene sequencing. We propose a new AARGs exposure dose calculation that uses short-term inhalation (STI). Swine farms and hospitals were high-risk areas where AARGs standardised abundance was more abundant than suburbs and urban areas. Additionally, resistance gene abundance in swine farm worker sputum was higher than that in healthy individuals in other environments. The correlation between AARGs with MGEs and bacteria was strong in suburbs but weak in livestock farms and hospitals. STI exposure analysis revealed that occupational intake of AARGs (via PM₁₀) in swine farms and hospitals were 110 and 29 times higher than in suburbs, were 1.5 × 10⁴, 5.6 × 10⁴ and 5.1 × 10² copies, i.e., 61.9%, 75.1% and 10.7% of the overall daily inhalation intake, respectively. Our study comprehensively compares environmental differences in AARGs to identify high-risk areas, and forwardly proposes the STI exposure dose of AARGs to guide risk assessment.     

Dosing low-level ferrous iron in coagulation enhances the removal of micropollutants, chlorite and chlorate during advanced water treatment

Drinking water utilities are interested in upgrading their treatment facilities to enhance micropollutant removal and byproduct control. Pre-oxidation by chlorine dioxide (ClO₂) followed by coagulation-flocculation-sedimentation and advanced oxidation processes (AOPs) is one of the promising solutions. However, the chlorite (ClO₂^–) formed from the ClO₂ pre-oxidation stage cannot be removed by the conventional coagulation process using aluminum sulfate. ClO₂^– negatively affects the post-UV/chlorine process due to its strong radical scavenging effect, and it also enhances the formation of chlorate (ClO₃^–). In this study, dosing micromolar-level ferrous iron (Fe(II)) into aluminum-based coagulants was proposed to eliminate the ClO₂^– generated from ClO₂ pre-oxidation and benefit the post-UV/chlorine process in radical production and ClO₃^– reduction. Results showed that the addition of 52.1-µmol/L FeSO₄ effectively eliminated the ClO₂^– generated from the pre-oxidation using 1.0 mg/L (14.8 µmol/L) of ClO₂. Reduction of ClO₂^– increased the degradation rate constant of a model micropollutant (carbamazepine) by 55.0% in the post-UV/chlorine process. The enhanced degradation was verified to be attributed to the increased steady-state concentrations of HO^· and ClO^· by Fe(II) addition. Moreover, Fe(II) addition also decreased the ClO₃^– formation by 53.8% in the UV/chlorine process and its impact on the formation of chloro-organic byproducts was rather minor. The findings demonstrated a promising strategy to improve the drinking water quality and safety by adding low-level Fe(II) in coagulation in an advanced drinking water treatment train.