铁基硅盐对土壤环境镉砷赋存形态及转化影响

为探明铁基硅盐对土壤镉砷赋存形态影响及各形态间转化规律,采用室内长期淹水培养吸附实验,研究不同比例铁硅材料对土壤离子态镉砷活性影响;筛选适宜铁基硅盐(FS)配比同时添加腐殖酸(FSC)和金属氧化物(FSCa),明确复配处理土壤中镉砷分级形态转化程度.结果显示,铁:硅比值增加10%,土壤pH值平均降低0.35;F₂-S₈处理土壤离子态镉降幅71%;F₁₀-S₀处理土壤离子态砷降低59.9%,离子态镉砷含量与硅酸盐-铁盐施用量互呈反比;处理F₄-S₆和F₆-S₄之间镉、砷钝化率产生交点,约为25%~30%.土壤中镉主要以可溶态为主,占比58%;砷主要以铁铝氧化态和钙结合态为主,占比40%和23%.铁硅比例为5:5或5.5:4.5左右复配能有效将铝结合态砷和铁铝氧化态砷转变为钙结合态砷和残渣态砷,可溶态镉转化为碳酸盐结合态镉以及铁锰氧化态镉,同步降低土壤中镉砷的活性.     

Effects of artificially induced complete mixing on dissolved organic matter in a stratified source water reservoir

Naturally complete mixing promotes the spontaneous redistribution of dissolved oxygen(DO), representing an ideal state for maintaining good water quality, and conducive to the biomineralization of organic matter. Water lifting aerators(WLAs) can extend the periods of complete mixing and increase the initial mixing temperature. To evaluate the influence of artificial-induced continuously mixing on dissolved organic matter(DOM) removal performance, the variations of DOM concentrations, optical cha...     

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.     

Chemical characterization and source identification of PM2.5 in Luoyang after the clean air actions

Luoyang is a typical heavy industrial city in China, with a coal-dominated energy structure and serious air pollution. Following the implementation of the clean air actions, the physicochemical characteristics and sources of PM_2.5 have changed. A comprehensive study of PM_2.5 was conducted from October 16, 2019 to January 23, 2020 to evaluate the effectiveness of previous control measures and further to provide theory basis for more effective policies in the future. Results showed that the aerosol pollution in Luoyang in autumn and winter is still serious with the average concentration of 91.1 μg/m³, although a large reduction (46.9%) since 2014. With the contribution of nitrate increased from 12.5% to 25.1% and sulfate decreased from 16.7% to 11.2%, aerosol pollution has changed from sulfate-dominate to nitrate-dominate. High NO₃⁻/SO₄²⁻ ratio and the increasing of NO₃⁻/SO₄²⁻ ratio with the aggravation of pollution indicating vehicle exhaust playing an increasingly important role in PM_2.5 pollution in Luoyang, especially in the haze processes. Secondary inorganic ions contributed significantly to the enhancement of PM_2.5 during the pollution period. The high value of Cl⁻/Na⁺ and EC concentration indicate coal combustion in Luoyang is still serious. The top three contributor sources were secondary inorganic aerosols (33.3%), coal combustion (13.6%), and industrial emissions (13.4%). Close-range transport from the western and northeastern directions were more important factors in air pollution in Luoyang during the sampling period. It is necessary to strengthen the control of coal combustion and reduce vehicle emissions in future policies.     

Identification and characterization of Fe3O4/peroxodisulfate advanced oxidation products from sulfameter

Sulfonamides (SAs) are one of the most widely used antibiotics and their residuals in the environment could cause some negative environmental issues. Advanced oxidation such as Fenton-like reaction has been widely applied in the treatment of SAs polluted water. Degradation rates of 95%-99.7% were achieved in this work for the tested 8 SAs, including sulfisomidine, sulfameter (SME), phthalylsulfathiazole, sulfamethoxypyridazine, sulfamonomethoxine, sulfisoxazole, sulfachloropyridazine, and sulfadimethoxine, in the Fe₃O₄/peroxodisulfate (PDS) oxidation system after the optimization of PDS concentration and pH. Meanwhile, it was found that a lot of unknown oxidation products were formed, which brought up the uncertainty of health risks to the environment, and the identification of these unknown products was critical. Therefore, SME was selected as the model compound, from which the oxidation products were never elucidated, to identify these intermediates/products. With liquid chromatography-high resolution tandem mass spectrometry (LC-HRMS/MS), 10 new products were identified, in which 2-amino-5-methoxypyrimidine (AMP) was confirmed by its standard. The investigation of the oxidation process of SME indicated that most of the products were not stable and the degradation pathways were very complicated as multiple reactions, such as oxidation of the amino group, SO₂ extrusion, and potential cross-reaction occurred simultaneously. Though most of the products were not verified due to the lack of standards, our results could be helpful in the evaluation of the treatment performance of SAs containing wastewater.     

Clean and effective removal of Cl(-I) from strongly acidic wastewater by PbO2

Recycling strongly acidic wastewater as diluted H₂SO₄ after contaminants contained being removed was previously proposed, however, Cl(-I), a kind of contaminant contained in strongly acidic wastewater, is difficult to remove, which severely degrades the quality of recycled H₂SO₄. In this study, the removal of Cl(-I) using PbO₂ was investigated and the involved mechanisms were explored. The removal efficiency of Cl(-I) reached 93.38% at 50℃ when PbO₂/Cl(-I) mole ratio reached 2:1. The identification of reaction products shows that Cl(-I) was oxidized to Cl₂, and PbO₂ was reduced to PbSO₄. Cl₂ was absorbed by NaOH to form NaClO, which was used for the regeneration of PbO₂ from the generated PbSO₄. Cl(-I) was removed through two pathways, i.e., surface oxidation and •OH radical oxidation. •OH generated by the reaction of PbO₂ and OH⁻ plays an important role in Cl(-I) removal. The regenerated PbO₂ had excellent performance to remove Cl(-I) after six-time regeneration. This study provided an in-depth understanding on the effective removal of Cl(-I) by the oxidation method.     

贵州梵净山九龙池沉积物14C年代学研究及全新世碳累积速率变化

放射性碳同位素加速器质谱（ASM¹⁴C）测年法是湖泊沉积物定年的主要方法,并且是全新世年代学研究的热点。随着对全新世古气候与环境变化研究的深入,选取不同介质定年可能对年代模型的准确性造成误差,进而影响到气候指标的解译。本文选取贵州东北部梵净山九龙池沉积物中树枝、树叶、树皮、种子等植物残体和全样有机质作为测年介质,利用ASM¹⁴C进行定年。结果表明,相比全样有机质,使用植物残体定年可以在一定程度上避免碳库效应的影响。但相比于原位沉积且生长年限较短的叶片,树枝的定年结果偏老,不是一种理想的定年介质。另外,根据定年结果及总有机碳含量重建了全新世九龙池的碳累积速率,发现碳累积速率可以指示该地区亚洲夏季风强度的变化历史。     

鄱阳湖典型湿地土壤-植物系统重金属沿湖向富集及迁移转换特征分析

特殊的水文节律导致鄱阳湖形成面积较大的周期性环湖消落带,大量的营养物质和污染物极易在消落带中发生沉积,选择鄱阳湖典型河口型消落带,沿湖向按照不同植被类型设置采样断面,采集土壤-沉积物和优势植物样品(不同组织),分析不同时空下土壤/沉积物和优势植物体中重金属(Cr、 Ni、 Cu、 Zn、 As、 Cd、 Sb和Pb)的含量特征及富集水平,并进一步分析土壤-植物系统中重金属的迁移转换特征,揭示鄱阳湖典型消落带土壤-植物系统重金属迁移转换的影响因素.结果表明,消落带土壤/沉积物重金属含量沿湖向表现为明显的分布规律,呈现为先升高后降低的分布特征,即季节性淹水带土壤/沉积物是重金属富集的主要地带,Cu、 Pb和Sb在土壤/沉积物中的富集水平较高,其中Cu和Sb为显著富集(EF>5);潜在生态风险结果表明季节性淹水带总体处于轻度生态危害水平(70≤RI<140),显著高于淹水带和未淹水带.消落带沿湖向带状分布的优势植物体中重金属含量并未表现出显著的空间分布特征,但表现为显著的季节差异,生长季(4月)优势植物体内重金属具有较高的含量水平,重金属不同介质和组织的分配大体遵循基质>根...     

不同性质硅肥影响土壤生物有效态镉砷的主要因素

为研究硅肥影响土壤中生物有效态镉(Cd)和砷(As)的主要因素,选择不同性质的3种碱性硅肥[Na₂SiO₃、 CaSiO₃与ASSF (pH 9～11)]和一种弱酸偏中性可溶硅肥(NSSF,pH 5～6)并通过添加不同用量硅肥(25～800 mg·kg^-1,以Si计)开展室内土盆试验,淹水共育21 d后对土壤基本理化性质进行检测,同时利用薄膜扩散梯度(DGT)提取土壤生物有效态Cd和As.结果表明,不同性质硅肥施用对土壤基本理化性质的影响差异显著,具体来说：3种碱性硅肥均显著提升土壤pH值(P<0.05),其中Na₂SiO₃提升土壤pH能力最强;而NSSF的施用则显著降低土壤pH值但提升了土壤Eh值(P<0.05),每单位质量(mg) Si添加量的NSSF可使土壤pH下降0.001 7个单位;在Si添加量达到400 mg·kg^-1后,3种碱性硅肥和NSSF土壤pH和Eh变化都趋于平缓. 4种不同性质硅肥提升土壤有效硅含量能...     

KOH活化小麦秸秆生物炭对废水中四环素的高效去除

活化是提高生物炭吸附性能的重要手段.以小麦秸秆为研究对象,KOH为活化剂,制备KOH活化生物炭（K-BC）,同时制备原状生物炭（BC）作为对照.对生物炭进行比表面积和孔径、元素分析、XPS、FTIR、Raman、XRD和pH_pzc等表征,考察KOH活化对生物炭理化性质的影响,并探究生物炭对水体中四环素的吸附性能和机制.结果表明,KOH活化之后生物炭的比表面积和孔体积可达996.4 m²·g^-1和0.45 cm³·g^-1.KOH活化会制造更多的碳结构缺陷,影响生物炭的官能团和表面电性.拟二级动力学和Langmuir模型可以较好地拟合生物炭吸附四环素的过程.环境温度升高能提高生物炭对四环素的吸附量.K-BC吸附四环素是自发、吸热和无序度增加的过程.K-BC对四环素的最大吸附量理论可达到491.19 mg·g^-1（实验温度为45℃）.结合吸附后生物炭的Raman、FTIR和XPS表征,发现孔隙填充和π-π作用是K-BC吸附四环素的主要机制,氢键和络合作用也发挥重要作用.此外,K-BC还具有良好的循环使用性能.综上所述,KOH活化小麦秸秆生物炭是有效和可行的,可用于废水中四环素的去除.