Remediation of soil and groundwater contaminated with organic chemicals using stabilized nanoparticles: Lessons from the past two decades

▪ Overviewed evolution and environmental applications of stabilized nanoparticles. ▪ Reviewed theories on particle stabilization for enhanced reactivity/deliverability. ▪ Examined various in situ remediation technologies based on stabilized nanoparticles. ▪ Summarized knowledge on transport of stabilized nanoparticles in porous media. ▪ Identified key knowledge gaps and future research needs on stabilized nanoparticles. Due to improved soil deliverability and high reactivity, stabilized nanoparticles have been studied for nearly two decades for in situ remediation of soil and groundwater contaminated with organic pollutants. While large amounts of bench- and field-scale experimental data have demonstrated the potential of the innovative technology, extensive research results have also unveiled various merits and constraints associated different soil characteristics, types of nanoparticles and particle stabilization techniques. Overall, this work aims to critically overview the fundamental principles on particle stabilization, and the evolution and some recent developments of stabilized nanoparticles for degradation of organic contaminants in soil and groundwater. The specific objectives are to: 1) overview fundamental mechanisms in nanoparticle stabilization; 2) summarize key applications of stabilized nanoparticles for in situ remediation of soil and groundwater contaminated by legacy and emerging organic chemicals; 3) update the latest knowledge on the transport and fate of stabilized nanoparticles; 4) examine the merits and constraints of stabilized nanoparticles in environmental remediation applications; and 5) identify the knowledge gaps and future research needs pertaining to stabilized nanoparticles for remediation of contaminated soil and groundwater. Per instructions of this invited special issue, this review is focused on contributions from our group (one of the pioneers in the subject field), which, however, is supplemented by important relevant works by others. The knowledge gained is expected to further advance the science and technology in the environmental applications of stabilized nanoparticles.     

Acceleration of the particulate organic matter hydrolysis by start-up stage recovery and its original microbial mechanism

• Carbon availability was partially solved by POM recovery and fermentation. • 12% carbon sources were regenerated by fermentation of the entrapped 35% TCOD. • The unique microbial communities facilitated the efficient hydrolysis of the POM. • Considerable economic benefits in aeration power and ECS dosage were anticipated. To address the availability of carbon sources for denitrification, the accelerated hydrolysis of the most abundant but low-availability fraction of particulate organic matter (POM) was investigated. Mesh sieves with different pore sizes were used as primary pretreatment at the start-up-stage of the biological process to separate some POM from the liquid system. The changes in soluble carbohydrates and proteins were monitored to investigate the hydrolysis performance of the sieved POM, with waste activated sludge (WAS) as the control test. The results showed that an average of 35% POM could be entrapped before filtrate mat development. In addition, benefiting from the high polysaccharides concentration, as well as the high availability due to the relatively loose physical structure, a 23% hydrolysis efficiency of POM was obtained, in contrast to that of WAS (3.4%), with a hydrolysis constant of 0.39 h⁻¹. The prominent performance was also attributed to the unique microbial communities having been domesticated at a lower temperature, especially the cellulose-degrading bacteria Paraclostridium and psychrophile Psychrobacter, making up 6.94% and 2.56%, respectively. Furthermore, the potential benefits and application of improved POM hydrolysis by start-up stage recovery via mesh sieves combined with anaerobic fermentation were evaluated, including selective POM entrapment, alleviation of blockage and wear, and a reduction in aeration energy. By the proposed strategy, carbon availability for biological nutrient removal (BNR) processes is anticipated to be improved more economically than that can be achieved by primary clarifier elimination.     

不同富营养状态下沼蛤的存活与行为特性研究

通过设计不同富营养状态下沼蛤的行为特性的控制实验,探讨了不同富营养状态下沼蛤的生存、运动和粘附特性。研究结果为:(1)富营养状态最优(贫营养)水质不适宜沼蛤的粘附,但是适宜其生存,因此移动距离最短,运动能力最差。轻度富营养水质适宜沼蛤的生存。富营养状态最差(重度富营养)不适宜沼蛤的生存,因此移动距离最远,能生存下来的沼蛤运动能力最强。(2)在不同营养盐浓度下的重度富营养状态水质中,沼蛤适宜在营养盐浓度较低的水体中生存,营养盐浓度越高越不适宜沼蛤生存;营养盐浓度越高越不适宜沼蛤粘附,营养盐浓度相对而言较低的水体适宜沼蛤粘附。(3)在不同藻浓度下的重度富营养水质中,沼蛤适宜在藻浓度较低的水体中生存,藻浓度越高越不适宜沼蛤生存;藻浓度越高越不适宜沼蛤粘附,藻浓度相对而言较低的水体适宜沼蛤粘附;低藻浓度水体相对而言更适宜沼蛤生存,因此移动距离最短,运动能力最差,高藻浓度水体不适宜沼蛤生存,因此移动距离最远,能生存下来的沼蛤运动能力最强。富营养状态是影响沼蛤生长、粘附和运动的关键要素,轻度富营养化状态最适宜沼蛤生长和粘附。水体中营养盐浓度和浮游植物浓度也是影响沼蛤生长、粘附和运动的关键要素,重度富营养化状态中营养盐浓度和浮游植物浓度越低,越适宜适宜沼蛤生长和粘附。     

Hydrochemical characteristics and identification of pollution ions of the springs in the south of Yanbian City,China

Environmental Geochemistry and Health - Mathematical statistics, correlation analysis, Piper and Gibbs diagrams, and geographic information system- based multi-criteria decision analysis were used...     

Reclaiming the spent alkaline zinc manganese dioxide batteries collected from the manufacturers to prepare valuable electrolytic zinc and LiNi0.5Mn1.5O4 materials

A process for reclaiming the materials in spent alkaline zinc manganese dioxide (Zn–Mn) batteries collected from the manufacturers to prepare valuable electrolytic zinc and LiNi_0.5Mn_1.5O₄ materials is presented. After dismantling battery cans, the iron cans, covers, electric rods, organic separator, label, sealing materials, and electrolyte are separated through the washing, magnetic separation, filtrating, and sieving operations. Then, the powder residues react with H₂SO₄ (2 mol L^?1) solution to dissolve zinc under a liquid/solid ratio of 3:1 at room temperature, and subsequently, the electrolytic Zn with purity of ?99.8% is recovered in an electrolytic cell with a cathode efficiency of ?85% under the conditions of 37–40 °C and 300 A m^?2. The most of MnO₂ and a small quantity of electrolytic MnO₂ are recovered from the filtration residue and the electrodeposit on the anode of electrolytic cell, respectively. The recovered manganese oxides are used to synthesize LiNi_0.5Mn_1.5O₄ material of lithium-ion battery. The as-synthesized LiNi_0.5Mn_1.5O₄ discharges 118.3 mAh g^?1 capacity and 4.7 V voltage plateau, which is comparable to the sample synthesized using commercial electrolytic MnO₂. This process can recover the substances in the spent Zn–Mn batteries and innocuously treat the wastewaters, indicating that it is environmentally acceptable and applicable.     

气候变化和人类活动对我国典型草原区植被恢复的影响

草原区作为影响我国陆地生态系统碳水循环和生态安全的重点区域,对气候变化和人类活动极为敏感.然而,有关气候变化和人类活动对该区域植被恢复相对贡献的认识尚存分歧.以生态系统净初级生产力(NPP)为评价指标,通过对比MODIS观测的实际NPP和基于Thornthwaite Memorial模型估算的潜在NPP的趋势差异,量化了2000～2020年气候变化和人类活动对我国典型草原区(北方温性草原区和青藏高原高寒草原区)植被恢复的相对作用.结果表明,研究区内93%的草地植被呈恢复趋势,NPP平均增加速率达(以C计)2.12 g·(m²·a)^-1(P<0.01),其中,近一半植被恢复区受气候变化和人为活动共同控制,约36%和10%植被恢复区分别受气候变化和人类活动的独立控制;此外,不同草地类型气候变化主导植被恢复的面积占比差异大,主要表现为高寒草地明显高于温性草地,气候条件越干旱,气候主导面积占比越大.人类活动不是北方温性草原区和青藏高原高寒草原区植被恢复的主要原因,但在气候条件恶化地区,人类活动可降低甚至抵消气候变化对植被的负面影响.未来需加强长...     

三峡水库消落区自然植被群落分布特征

为了调查清楚三峡水库消落区自然植被群落的分布特征,在三峡水库消落区设置了 251个样地进行调查研究.结果表明,在土质边坡、岩质边坡和混合质边坡中,狗牙根群落占绝对优势;在145～155 m、155～165 m、165～175 m高程区间,狗牙根群落均有分布且数量较多,其次为苍耳群落和狗尾草群落,且随着高程的增加植物种类...     

松花江表层沉积物PAEs分布特征及生态风险评价

为揭示松花江干支流表层沉积物中邻苯二甲酸酯类(phthalate esters,PAEs)的空间分布特征及其生态风险状况本文利用气相色谱三重四级杆质谱联用仪(GC-MS)对松花江干支流表层沉积物中6种PAEs的含量分布和组成特征进行了分析,并采用商值法和环境风险水平(ERL)法对其生态风险状况进行评价.结果表明:①松花江干支流沉积物6种邻苯二甲酸酯(∑_6PAEs)含量范围(以干重计)为6 832.5～36 298.9ng·g~(-1)(平均值为18388.6ng·g~(-1)),邻苯二甲酸(2-乙基己基)酯(DEHP)和邻苯二甲酸二丁酯(DBP)为主要组分,干流点位∑_6PAEs含量(6 832.5～36 298.9 ng·g~(-1),平均值为18 616.9ng·g~(-1))与支流点位∑_6PAEs(10 367.6～26 593.3ng·g~(-1),平均值为18 264.1ng·g~(-1))差异不显著(P0.05),支流点位各PAEs单体含量与干流点位差异不大.从上游到下游干支流∑_6PAEs含量呈现先降后升的趋势.农业自然区域∑_6PAEs平均含量(18 677.5 ng·g~(-1))与城市工业区域(18 063.7 ng·g~(-1))相近(P0.05),DBP和DEHP是两区域内的主要PAEs两者平均值贡献率高达98%以上.②松花江干支流表层沉积物中∑_6PAEs主要来源于人类日用品、农业生产以及含有增塑剂的工业生产.③松花江表层沉积物中DMP和BBP对水生生物无生态风险,DEP具有低水平生态风险,而DEHP和DBP对水生生物具有高生态风险.     

基于iLME+Geoi-RF模型的四川省PM2.5浓度估算

高分辨率PM2.5空间分布数据对动态监测和控制PM2.5污染具有重要意义.选取Himawari-8气溶胶光学厚度(AOD)、ERA5气象再分析资料、DEM、土地利用数据、夜光遥感数据、增强型植被指数和人口数据等作为估算变量,使用改进的重采样法进行数据匹配,并提出改进的线性混合模型(iLME)结合地理智能随机森林(Geoi-RF)构建组合模型估算PM2.5浓度.结果表明:①在选取的估算变量中,气溶胶光学厚度、气压、温度、相对湿度和边界层高度是影响2016年四川省PM2.5浓度的重要因素,其相关系数分别为0.65、0.58、0.55、0.54和0.35.②iLME+Geoi-RF模型精度相较其他模型有较大提升,模型拟合Rl2、RMSR 和 MAE 分别为0.98、3.25 μg·m-3和 1.98 μg·m-3,交叉验证 R2、RMSR 和 MAE 分别为0.89、7.95 μg·m-3和4.81μg·m-3.该模型可获取更高精度的四川省PM2.5时空分布特征,为区域空气质量评估、人体暴露风险评价和环境污染治理提供更加合理地科学参考.③2016年四川省PM2.5浓度存在显著的季节性差异,各季节PM2.5浓度大小关系为:冬季＞秋季＞春季＞夏季.2016年四川省月均PM2.5浓度总体上呈先降后升的"V"型趋势,最小值在6月,最大值在12月,8月和11月有微小起伏.在空间分布上四川省PM2.5浓度总体上呈东高西低和局部污染程度较高的特点,高值区主要分布在城市快速发展和人口密集的东部地区,低值区主要分布在经济发展落后和人口稀疏的西部地区.④虽然不同模型估算出的PM2.5浓度整体分布基本一致,但iLME+Geoi-RF模型能更准确有效地估算本研究区污染的空间分布.     

深圳茅洲河下游柱状沉积物中碳氮同位素特征

对茅洲河下游12根沉积物柱状样中总氮(TN)、有机质(OM)、C/N值、δ~(15)N、δ~(13)C含量进行了测定,分析探讨了茅洲河下游及其主要支流沙井河沉积物中氮和有机质的分布特征及来源.结果表明,沉积物中TN平均含量为1 815.37 mg·kg~(-1),OM平均含量为22 401.68 mg·kg~(-1),与太湖和巢湖流域相比,研究区内TN和OM含量均处于较高水平,且随深度增加变化均较大.茅洲河下游沉积物中δ~(15)N、δ~(13)C含量范围为2.20‰~32.78‰、-27.53‰~-21.95‰,平均值分别为6.78‰、-25.41‰;C/N值范围为0.49~18.23;δ~(13)C随深度变化较为平缓,而δ~(15)N、C/N值随深度增加波动较大.研究区来源分析表明:C3植物与合成化肥为茅洲河下游表层沉积物(0~40 cm)的主要来源;藻类是深层沉积物与支流沙井河沉积物中有机质的主要来源.茅洲河下游表层沉积物(0~40 cm)中的氮素主要来源于无机化肥与土壤有机氮,深层沉积物与支流沙井河沉积物中的氮素主要来源于土壤流失和土壤有机氮.