In situ construction of Z-scheme FeS2/Fe2O3 photocatalyst via structural transformation of pyrite for photocatalytic degradation of carbamazepine and the synergistic reduction of Cr(VI)

Pyrite is the most abundant sulfide semiconductor mineral with excellent optical properties. However, few reports have investigated its photocatalytic activity because of the low photogenerated carrier separation efficiency. In this work, a Z-scheme FeS₂/Fe₂O₃ composite photocatalyst was fabricated in situ via structural transformation of pyrite through heat treatment. A remarkably enhanced photocatalytic performance was observed over the FeS₂/Fe₂O₃ composite photocatalyst. Compared with the pristine pyrite, the degradation efficiency of carbamazepine (CBZ) reached 65% at the added hexavalent chromium (Cr(Ⅵ)) concentration of 20 mg/L and the Cr(Ⅵ) was nearly completely reduced in the mixed system using FeS₂/Fe₂O₃ within 30 min under simulated solar light irradiation. The enhanced photocatalytic activity can be attributed to the efficient separation and transfer of photogenerated carriers in the FeS₂/Fe₂O₃ composite photocatalyst. This facilitated the generation of ?OH, hole (h⁺) and ?O₂^? species, which participated in the photocatalytic reaction with CBZ. Based on the measurement of the active species and electric properties, a Z-scheme electron transfer pathway was proposed for the FeS₂/Fe₂O₃ composite photocatalyst. This work broadens the application potential of pyrite in environmental remediation.     

磁性活性炭强化SBR脱氮除磷及微生物种群分析

为了提高传统活性污泥法脱氮除磷效率,改善污泥易膨胀等问题,在序批式活性污泥反应器（SBR）中,投加140目1.00g/L的磁性活性炭构建磁性炭基活性污泥系统（1^#）,同时,以不投加任何材料（单独活性污泥系统）为对照组（0^#）,研究磁性活性炭对活性污泥系统除污性能和主要微生物种群结构组成的影响,探讨了磁性活性炭强化活性污泥系统脱氮除磷机理.结果表明：1^#对TN和TP的平均去除率分别为68.59%和78.25%;而0^#对于TN和TP的平均去除率则为53.17%与54.10%,1^#出水NO₃^--N浓度平均降低了7.03mg/L,两系统对NH₄⁺-N和COD的去除效率差别不大,均在95.00%以上.典型周期内1^#中TN、NH₄⁺-N、TP、COD的下降速率快于0^#;0^#同步硝化反硝化效率为60.31%,反硝化速率为4.44mg/（L·h）,1^#同步硝化反硝化效率为80.74%,反硝化速率为6.13mg/（L·h）,实验组1^#脱氮速率明显快于空白对照组0^#.高通量测序结果表明,1^#内污泥的优势菌门为Saccharibacteria（38.74%）、Proteobacteria（22.52%）、Actinobacteria（18.54%）和Chloroflexi（8.40%）.此外,与0^#相比,1^#引发污泥膨胀密切相关的Actinobacteria菌门的微生物相对丰度显著下降;与脱氮除磷功能相关的Micropruina、Shinella、norank_f_Anaerolineaceae和norank_f_Xanthomonadaceae 4种菌属的相对丰度都明显上升.SBR系统中加载一定量的磁性活性炭既能抑制引起污泥膨胀微生物的生长,又能利于脱氮除磷微生物的富集,整个污泥系统表现出良好的稳定性和脱氮除磷性能.     

热活化过硫酸盐联合混凝处理微乳浊液的机理

在冶金冷轧微乳浊液中,醚链较长、αH较多的非离子型表面活性剂的存在导致体系稳定性极高而难于降解,利用热活化过硫酸盐（PS）进行破乳预处理,并联合混凝作用,以实现高效的油水分离.本文研究了PS浓度、体系温度、pH值对上述反应的影响,根据电子顺磁共振等分析技术确定了作用自由基类型及其贡献率,利用气相色谱-质谱联用法分析了反应前后微乳浊液成分,根据激光粒度法测定了反应过程油滴粒径,结果表明：增大PS浓度和温度、降低pH值均有利于提高COD去除率;降解过程包括SO₄^-.、OH^.破乳及聚合硫酸铁促使强疏水性油滴脱稳,且SO₄^-.为破乳主导自由基（贡献率86.33%）;基于联合工艺的COD去除率和运行成本均优于热活化PS单一工艺.     

嘉兴夏季臭氧污染的近地层垂直变化特征

基于2018年浙江省嘉兴市14个环境国控站点的O₃历史资料与气象要素,研究O₃与气象要素的关系,并结合差分吸收臭氧雷达的垂直臭氧探测资料,分析近地层O₃廓线变化特征.结果表明,嘉兴地区发生高浓度O₃污染的关键气象要素为24~36℃的大气温度和36%~77%的相对湿度,24℃以上的大气温度与77%以下的相对湿度可作为启动预警O₃污染的气象指标.差分吸收臭氧雷达监测结果显示,无论O₃超标天与清洁天,在垂直方向上其浓度随高度先升后降,在600~800m范围出现峰值;O₃污染时段,在中午到午后低空形成持续向下的O₃输送带,这种低空O₃与地表O₃的叠加机制加重地表O₃污染程度,导致地表O₃超标与低空高浓度相伴出现;其廓线日变化规律表现出800m以下浓度在夜间和凌晨梯度不显著,日出后近地层O₃随时间快速增加,中午和午后持续高值,傍晚随时间逐渐下降的特征.后向轨迹分析表明,10,500,1000m高度层的气流后向轨迹聚类有相似性,500m处沿闽浙海岸线的轨迹簇对应O₃较10m处来自海上的轨迹簇高,这与500m处前体物输送堆积和紫外线辐射增强有关.污染过程近地层气流来向紧贴地面,但中高层有明显下沉气流使得O₃前体物在500m附近堆积,是造成2个典型污染过程中垂直方向上O₃高值出现在500m左右的原因之一.     

Mechanisms of photochemical release of dissolved organic matter and iron from resuspended sediments

Photochemical reactions can alter the transformation of sedimentary organic matter into dissolved organic matter (DOM) and affect its ultimate fate in water ecosystems. In the present study, the photorelease of DOM and Fe from resuspended lake sediments was investigated under different O₂ and NO₃^? concentration conditions to study the mechanisms of DOM and Fe photorelease. The amount of photoreleased Fe, which ranged from 0.22 to 0.70 μmol/L, was significantly linearly correlated with the amount of photoreleased DOM. O₂ and NO₃^? could promote the photochemical release of DOM and Fe, especially during the initial 4 h irradiation. In general, the order of the photorelease rates of DOM and Fe under different conditions was as follows: NO₃^?/aerobic > aerobic ≈ NO₃^?/anaerobic > anaerobic. The photorelease rates of DOM and Fe were higher for the initial 4 hr irradiation than these for the subsequent 8 hr irradiation. The photorelease of DOM and Fe is thought to proceed via direct photodissolution and indirect processes. The relative contributions of indirect processes (>60%) was much greater than that of direct photodissolution (<40%). The photoproduced H₂O₂ under aerobic and anaerobic conditions indicated that hydroxyl radicals (?OH) are involved in the photorelease of DOM. Using ?OH scavengers, it was found that 38.7%, 53.7%, and 77.6% of photoreleased DOM was attributed to ?OH under anaerobic, aerobic, and NO₃^?/aerobic conditions, respectively. Our findings provide insights for understanding the mechanisms and the important role of ?OH in the DOM and Fe photorelease from resuspended sediments.     

基于重点行业/领域的我国碳排放达峰路径研究

开展碳排放达峰路径研究,明确时间表、路线图、施工图,是支撑我国实现2030年前碳达峰目标的基础性研究工作. 本文采取自上而下和自下而上相结合的方式,以满足社会经济高质量稳定发展需求和国家碳达峰碳中和双重目标为约束开展自上而下的宏观路径研究;以合计贡献了我国碳排放(不含港澳台地区数据) 90%以上的电力、钢铁、水泥、铝冶炼、石化化工、煤化工共6个重点行业以及建筑、交通2个重点领域为对象,开展自下而上的重点行业/领域碳达峰路径研究;通过上下路径反复迭代、行业间耦合优化,打通宏观路径与微观措施的联动和双向反馈,最终形成基于重点行业/领域的我国碳达峰路径. 结果表明:为实现国家碳达峰、碳中和的目标愿景,需抓紧部署、大力推进包括清洁能源降碳、能效提升降碳、资源循环降碳、管理调控降碳等4类关键举措,方可实现我国碳排放量在2030年前达峰的目标,峰值较2020年增加5.0×108~7.0×108 t左右,达峰后将保持3~4年的峰值平台期. 受需求与技术驱动,不同领域碳排放总量将梯次实现达峰,其中工业领域（含钢铁、水泥、铝冶炼、石化化工、煤化工共5个重点行业）预计将在“十四五”期间整体达峰,达峰后碳排放稳定下降;电力行业和交通、建筑领域碳排放均在2030年左右实现达峰. 经测算,2021—2030年间,为推动碳达峰采取的4类关键措施预计需投入2.08×1013元;其中清洁能源降碳是最为有效的措施,同时也是成本最高的措施. 为保障关键举措顺利落地,建议全面加大政策创新,逐步形成系统完善的碳总量控制与交易市场机制、绿色低碳标准体系、行业准入及产业结构政策体系、价格财税及投融资机制等. 本研究分行业及领域的碳达峰路径研究成果及所识别的关键控碳减碳技术手段、措施和政策将为国家碳达峰路径设计提供技术支撑.      

热振森林大型土壤动物群落特征及其影响因素

为了解西藏拉萨市林周县热振国家森林公园不同海拔大型土壤动物群落的空间分布特征及其与环境因子的关系,于2021年7月(夏季)根据其地理特征设置了三个不同海拔共9个样地.采用手捡法对大型土壤动物进行收集,并将其保存在75%酒精的收集管中,同时测定相应的环境因子.共捕获大型土壤动物1427个,经形态学鉴定隶属于2门5纲15目21科,其中优势类群为姬马陆科(Julidae)和蚁科(Formicidae),占总捕获量的66.0%.常见类群共10类,占总捕获量的31.3%;稀有类群占总捕获量的2.7%.热振国家森林公园大型土壤动物的类群、Shannon多样性指数、均匀度指数和优势度指数在三个不同海拔之间无显著性差异(P>0.05).大型土壤动物群落Jaccard相似性系数位于0.15~0.77.Pearson相关性结果显示,大型土壤动物个体数与海拔呈极显著负相关(P<0.01),与土壤温度和pH呈显著正相关(P<0.05);冗余分析显示,排序轴1和轴2共同解释了的类群组成变化的55.0%,全磷(TP)和有效磷(AP)为显著性解释变量,对大型土壤动物群落的解释率分别为29.6%和18.5%,是影响大型土壤动物群落的主要环境因子.     

Migration and transformation of Sb are affected by Mn(III/IV) associated with lepidocrocite originating from Fe(II) oxidation

Antimony (Sb) is a recognized priority pollutant with toxicity that is influenced by its migration and transformation processes. Oxidation of Fe(II) to Fe(III) oxides, which is a common phenomenon in the environment, is often accompanied by the formation of Mn(III/IV) and might affect the fate of Sb. In this study, incorporated Mn(III) and sorbed/precipitated Mn(III/IV) associated with lepidocrocite were prepared by adding Mn(II) during and after Fe(II) oxidation, respectively, and the effects of these Mn species on Sb fate were investigated. Our results indicated that the association of these Mn species with lepidocrocite obviously enhanced Sb(III) oxidation to Sb(V), while concomitantly inhibiting Sb sorption due to the lower sorption capacity of lepidocrocite for Sb(V) than Sb(III). Additionally, Mn oxide equivalents increased in the presence of Sb, indicating that Sb oxidation by Mn(III/IV) associated with lepidocrocite was a continuous recycling process in which Mn(II) released from Mn(III/IV) reduction by Sb(III) could be oxidized to Mn(III/IV) again. This recycling process was favorable for effective Sb(III) oxidation. Moreover, Sb(V) generated from Sb(III) oxidation by Mn(III/IV) enhanced Mn(II) sorption at the beginning of the process, and thus favored Mn(III/IV) formation, which could further promote Sb(III) oxidation to Sb(V). Overall, this study elucidated the effects of Mn(III/IV) associated with lepidocrocite arisen from Fe(II) oxidation on Sb migration and transformation and revealed the underlying reaction mechanisms, contributing to a better understanding of the geochemical dynamics of Sb.     

念青唐古拉山西段小冰期以来冰川变化

小冰期是指15世纪到20世纪早期之间一系列相对寒冷的气候波动阶段,研究小冰期以来的冰川规模变化,对于了解百年尺度上冰川变化及其气候指示意义具有重要意义。利用Google Earth和Arc GIS10.3研究了念青唐古拉山西段的现代冰川和小冰期冰川,统计了冰川的基本信息和小冰期以来的变化情况,分析了面积、高程、坡度和坡向因素对冰川变化的影响,探讨了平衡线高度变化的气候指示意义。结果表明:念青唐古拉山西段共发育现代冰川847条,总面积约689.71 km~2,共识别出小冰期冰川306条,总面积约746.12 km~2。小冰期以来冰川面积减少约31%,平衡线高度平均上升约58 m,冰川的面积、坡度和高程对冰川面积变化的解释率为71%,平衡线高度变化与印度季风关系密切。