富氧空位/梯次结构CeO2的制备及光催化CO2还原

采用Ce-BTC(均苯三甲酸)为模板,通过尿素溶液浸渍合成了具有富氧空位/梯次结构的CeO₂催化剂,并用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、拉曼光谱(Raman)和紫外可见漫反射(DRS)等手段对其进行了表征.结果表明,与金属有机框架(MOFs)浸渍尿素高温煅烧可以获得金属氧化物/g-C₃N₄复合材料不同,Ce-BTC/尿素体系煅烧后产品中未检测到g-C₃N₄,这可能与CeO₂的存在抑制了尿素分解产物的热缩聚过程,影响了g-C₃N₄的生成有关,但尿素的引入改变了Ce-BTC煅烧产物CeO₂的氧空位浓度,且获得梯次结构.将具有富氧空位/梯次结构的CeO₂-5用于光催化CO₂还原,催化结果表明:反应4h的CO产率可达2.06μmol/g,CH₄产率可达1.42μmol/g,性能是Ce-BTC未...     

Potassium ferrate pretreatment promotes short chain fatty acids yield and antibiotics reduction in acidogenic fermentation of sewage sludge

During the acidogenic fermentation converting waste activated sludge (WAS) into short-chain fatty acids (SCFA), hydrolysis of complex organic polymers is a limiting step and the transformation of harmful substances (such as antibiotics) during acidogenic fermentation is unknown. In this study, potassium ferrate (K₂FeO₄) oxidation was used as a pretreatment strategy for WAS acidogenic fermentation to increase the hydrolysis of sludge and destruct the harmful antibiotics. Pretreatment with K₂FeO₄ can effectively increase the SCFA production during acidogenic fermentation and change the distribution of SCFA components. With the dosage of 0.2 g/g TS, the maximum SCFA yield was 4823 mg COD/L, which is 28.3 times that of the control group; acetic acid accounts for more than 90% of the total SCFA. The higher dosage (0.5 g/g TS) can further increase the proportion of acetic acid, but inhibit the overall performance of SCFA production. Apart from the promotion of hydrolysis and acidogenesis, K₂FeO₄ pretreatment can also simultaneously oxidizes and degrades part of the antibiotics in the sludge. When the dosage is 0.5 g/g TS, the degradation efficacy of antibiotics is the most significant, and the contents of ofloxacin, azithromycin, and tetracycline in the sludge are reduced by 69%, 42%, and 50%, respectively. In addition, K₂FeO₄ pretreatment can also promote the release of antibiotics from sludge flocs, which is conducive to the simultaneous degradation of antibiotics in the subsequent biological treatment process.     

Ozone episodes during and after the 2018 Chinese National Day holidays in Guangzhou: Implications for the control of precursor VOCs

The impact of reducing industrial emissions of volatile organic compounds (VOCs) on ozone (O₃) pollution is of wide concern particularly in highly industrialized megacities. In this study, O₃, nitrogen oxides (NOx) and VOCs were measured at an urban site in the Pearl River Delta region during the 2018 Chinese National Day Holidays and two after-holiday periods (one with ozone pollution and another without). O₃ pollution occurred throughout the 7-day holidays even industrial emissions of VOCs were passively reduced due to temporary factory shutdowns, and the toluene to benzene ratios dropped from ∼10 during non-holidays to ∼5 during the holidays. Box model (AtChem2-MCM) simulations with the input of observation data revealed that O₃ formation was all VOC-limited, and alkenes had the highest relative incremental reactivity (RIR) during the holiday and non-holiday O₃ episodes while aromatics had the highest RIR during the non-pollution period. Box model also demonstrated that even aromatics decreased proportionally to levels with near-zero contributions of industrial aromatic solvents, O₃ concentrations would only decrease by less than 20% during the holiday and non-holiday O₃ episodes and ozone pollution in the periods could not be eliminated. The results imply that controlling emissions of industrial aromatic solvents might be not enough to eliminate O₃ pollution in the region, and more attention should be paid to anthropogenic reactive alkenes. Isoprene and formaldehyde were among the top 3 species by RIRs in all the three pollution and non-pollution periods, suggesting substantial contribution to O₃ formation from biogenic VOCs.     

废弃物焚烧处理温室气体排放情景模拟与预测

为模拟废弃物焚烧处理过程中产生的温室气体排放,积极推动温室气体减排工作,早日实现碳达峰碳中和目标.基于系统动力学和IPCC温室气体排放计算方法,构建了以基准情景（BAU）为基础,从单一和综合技术类型减排情景出发的焚烧处理温室气体排放模型,并模拟预测了2010~2050年温室气体排放量（以CO_2e计,CO_2e为CO₂当量）的趋势变化、减排潜力以及空间分布.结果表明：①2010~2019年我国废弃物焚烧处理温室气体排放量呈增长趋势,于2016年后显著提升,年增速为18.61%.②2020~2050年,单一技术减排情景的中端改进情景（S2）和终端减排情景（S3）温室气体排放量分别于2043年和2036年达到峰值8410万t和6966万t.综合技术减排情景相较于单一技术减排情景较早达到排放峰值,综合技术减排情景中全过程减排情景（S7）采用多种减排技术协同控制温室气体排放,2050年累积排放量为205927万t,相对BAU情景减排了78.27%,排放达峰时间最早且减排潜力最大.③焚烧处理温室气体排放空间差异显著,排放量较多的省份主要分布在人口密集且经济发达的区域,江苏和广东省排放量最多,甘肃、吉林和宁夏等6个省份为排放低值区.     

光助MIL-101(Fe)活化过氧化氢氧化洛克沙胂及同步吸附生成的砷酸根

采用铁基金属有机框架(MIL-101(Fe))在模拟太阳光下活化过氧化氢氧化降解ROX—吸附去除生成的砷酸根.结果表明,光助MIL-101(Fe)(250mg/L)活化氧化剂H2O2(1.0mmol/L)体系可在120min内实现95.27％的ROX去除率,反应过程中形成的无机砷酸盐(As(Ⅴ))会吸附在MIL-101...     

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.     

城市河网区河流沉积物磷形态分布特征及释放贡献

以嘉兴城市河网区为研究区域,在调查区域水质和沉积物磷空间变化特征的基础上,分析沉积物中各形态磷的垂直与空间赋存状态,通过吸附释放参数计算EPC₀值,明确了沉积物-水界面磷迁移影响因素和沉积物中活跃磷素的释放风险和贡献.结果表明,研究区域水质氮磷污染较为严重,沉积物TP含量均值呈北部河网区>西部河网区>南部河网区,基于单因子指数法的生态风险评价为Ⅱ、Ⅲ和Ⅳ级的样本比例分别为10.91%、25.45%和63.64%.沉积物各形态磷整体呈现TP>IP>HCl-P>NaOH-P>OP,沉积物生物有效磷（BAP）整体呈现Olsen-P>AAP>WSP>RDP;在沉积物垂直剖面中,部分位点受到外界因素的强烈影响垂向波动较大,整体上是随深度的递增而减小,这与近年来研究区域接收的外源磷积累过程在加重有关.相关性分析表明,沉积物磷吸附容量（Q_max）与铁铝氧化物呈显著相关性 （p<0.05）;释放参数EPC₀与TP、IP与HCl-P呈显著相关性 （p<0.05）.结合BAP形态,研究区域河流沉积物NaOH-P、HCl-P、AAP、Olsen-P及WSP存在较高的释放潜力.南部河网区沉积物主要呈现磷“源”角色,西部和北部河网区部分区域沉积物充当磷“源”角色.南部河网区在长短时间尺度下的磷主要释放形态为NaOH-P、HCl-P和OP,北部河网区在长时间尺度下主要释放磷形态为NaOH-P、HCl-P,西部河网区在短时间尺度下主要释放形态以HCl-P为主,在长时间尺度下3种磷形态的释放风险仍然较高.     

京津冀臭氧污染特征、气象影响及基于神经网络的预报效果评估

基于生态环境监测和气象观测数据,分析了2016~2020年京津冀13个城市臭氧（O₃）浓度特征,讨论了O₃污染高发月份日最高温度（T_max）、日均地面气压（p）、日均地面相对湿度（RH）和日均地面风速（v）等气象要素对O₃-8h浓度和O₃-8h超标情况的影响规律,并采用AQI级别预报准确率、O₃浓度范围预报准确率和O₃级别预报准确率等方法,评估了基于神经网络的O₃统计预报效果.结果表明,2016~2020年期间京津冀13城市ρ（O₃-8h-90per）分别为157.4、177.2、177.3、190.6和175.6μg·m^-3,区域臭氧浓度5a上升了11.6%,2016~2019年期间总体呈波动上升趋势,2020年环比下降;2020年与2016年相比,除北京、张家口和承德略有下降外,其他10个城市ρ（O₃-8h-90per）上升了6~45.5μg·m^-3.O₃-8h月均值呈现"两头低,中间高"现象,ρ（O₃-8h）在4~9月的月均值超过了100 μg·m^-3,在6月最高,为158.10 μg·m^-3.城市O₃-8h超标率范围为8.6%~19.2%,97.8%的O₃-8h超标情况发生在4~9月.区域尺度上O₃-8h浓度与日最高温度相关性最强,当T_max在25~28℃区间时,所有城市开始出现O₃-8h超标.O₃-8h浓度与日均地面气压呈负相关关系;当RH在60%以下时,大部分城市O₃-8h浓度随相对湿度上升缓慢增长;当RH在61%~70%以上时,大部分城市O₃-8h浓度随日均相对湿度上升而下降.O₃-8h超标时的地面主导风向主要为偏南风,大部城市O₃-8h浓度高值易集中出现在2~3m·s^-1及以下低风速区间.OPAQ统计模式提前1~9 d预报相关系数范围为0.72~0.86,AQI级别预报平均准确率为67%~86%,O₃-8h浓度范围预报平均准确率为63%~84%.在O₃-8h超标情况多发的4~9月,模式对O₃轻度污染和O₃-8h超标情况提前3 d预报准确率分别为69%和66%,可为O₃-8h超标管控提供参考依据.     

Overestimate of remediation efficiency due to residual sodium persulfate in PAHs contaminated soil and a solution

Oxidation remediation is a commonly used technology for PAHs contaminated soil presently,but the overestimate of efficiency due to ongoing remediation by residual oxidants during extraction and testing has not been paid enough attention.In this study,persulfate was activated by Fe（Ⅱ） to inve stigate the effects of residual oxidants on PAHs removal during detection process and the elimination effects of adding Na₂ SO₃ and extending sampling time on residual oxidants.Results ...