Competition between phenanthrene, chrysene, and 2,5-dichlorobiphenyl for high-energy adsorption sites in a sediment

We determined the maximum amounts of added phenanthrene, chrysene, and 2,5-dichlorobiphenyl sorbed onto high-energy adsorption sites in a sediment on bi-solute experiments. The bi-solute pairs were phenanthrene/chrysene and phenanthrene/2,5-dichlorobiphenyl. On the bi-solute sorption experiments, one solute was introduced and equilibrated with sediment prior to addition of the second solute. The values for the maximum amounts adsorbed onto high-energy sites revealed that, after equilibration of the first solute, still some high-energy sites could be occupied by the second solute. Phenanthrene, chrysene, and 2,5-dichlorobiphenyl seem to share about 30% of the accessible high-energy adsorption sites in the sediment employed.     

Sorption of native polyaromatic hydrocarbons (PAH) to black carbon and amended activated carbon in soil

Organic pollutants (e.g. polyaromatic hydrocarbons (PAH)) strongly sorb to carbonaceous sorbents such as black carbon and activated carbon (BC and AC, respectively). For a creosote-contaminated soil (Sigma15PAH 5500 mg kg(dry weight(dw))(-1)) and an urban soil with moderate PAH content (Sigma15PAH 38 mg kg(dw)(-1)), total organic carbon-water distribution coefficients (K(TOC)) were up to a factor of 100 above values for amorphous (humic) organic carbon obtained by a frequently used Linear-Free-Energy Relationship. This increase could be explained by inclusion of BC (urban soil) or oil (creosote-contaminated soil) into the sorption model. AC is a manufactured sorbent for organic pollutants with similar strong sorption properties as the combustion by-product BC. AC has the potential to be used for in situ remediation of contaminated soils and sediments. The addition of small amounts of powdered AC (2%) to the moderately contaminated urban soil reduced the freely dissolved aqueous concentration of native PAH in soil/water suspensions up to 99%. For granulated AC amended to the urban soil, the reduction in freely dissolved concentrations was not as strong (median 64%), especially for the heavier PAH. This is probably due to blockage of the pore system of granulated AC resulting in AC deactivation by soil components. For powdered and granulated AC amended to the heavily contaminated creosote soil, median reductions were 63% and 4%, respectively, probably due to saturation of AC sorption sites by the high PAH concentrations and/or blockage of sorption sites and pores by oil.     

Dairy washwater treatment using a horizontal flow biofilm system

In Ireland, dairy farmyard washwater commonly comprises farmyard run-off and dairy parlour washings. Land-spreading is the most widely used method for treating this wastewater. However, this method can be labour intensive and can cause, in some cases, the degradation of surface and ground waters, mainly due to nitrogen contamination. In this study, a horizontal flow biofilm reactor (HFBR) with step-feed was constructed and tested in the laboratory, to remove organic carbon and nitrogen from a agricultural strength synthetic washwater (SWW). The HFBR had an average top plan surface area (TPSA) of 0.1002 m(2) and consisted of a stack of 45 polystyrene horizontal sheets--15 sheets embedded with 25 mm deep frustums above 30 sheets with 10 mm deep frustums. The frustums acted as miniature reservoirs. The sheets were alternately offset to allow the wastewater to flow horizontally along each sheet and vertically from sheet to sheet down through the reactor. Biofilms developed on the sheets and treated the wastewater. During the 212-d study, the total hydraulic loading rate based on the TPSA of the sheets was 35 l m(-2) d(-1). SWW was pumped for 10 min each hour, in a step feed arrangement at a rate of 23.33 l m(-2) d(-1) on to the top sheet during Phases 1 and 2, and 11.67 l m(-2) d(-1) onto Sheet 16 during Phase 1 (days 1-92) and onto Sheet 30 during Phase 2 (days 93-212). The substrate loading rate during Phases 1 and 2 was 94.8 g total chemical oxygen demand (COD) m(-2) d(-1) and 10.5 g total nitrogen (TN) m(-2) d(-1), based on the TPSA. At steady state in Phase 2, the unit achieved excellent carbon removal of 99.7% 5-day biochemical oxygen demand (BOD(5)) and 96.7% total COD, equivalent to TPSA removal rates of 67.5 g BOD(5)m(-2)d(-1) and 91.7 g COD m(-2) d(-1). The nitrogen removal percentages were 98.3% total ammonium-nitrogen (NH(4)-N(t)) and 72.8% TN, which equated to TPSA removal rates of 4.8 g NH(4)-N(t) m(-2) d(-1) and 7.6g TN m(-2) d(-1). No sloughing of solids or clogging of media occurred during the study. The unit was simple to construct and operate, with little maintenance.     

Effect of unburned carbon on lead, zinc, and copper recovery from molten fly ash by chloride-induced volatilization

The present work focuses on investigation of the effective recovery of heavy metals from molten fly ash by applying chloride-induced volatilization. In particular, the effect of unburned carbon on the chloride-induced volatilization of lead, zinc, and copper from model and real molten fly ashes was investigated in the temperature range 873–1173 K under a N₂ atmosphere. As a result, almost 100% of lead and a significant proportion of zinc were volatilized from the real molten fly ash samples at 1173 K. In contrast, for the model fly ash, volatilization ratios of lead and zinc at 1173 K were only 85% and 25%, respectively. Further, the results of X-ray diffraction analysis suggested that PbO in molten fly ash was converted either to Pb₂OCl₂ or Pb by respective chlorination and reduction reactions. Meanwhile ZnO and CuO in the molten fly ash were reduced to Zn and Cu by reaction with unburned carbon. Subsequently, Pb, Zn, and Pb₂OCl₂ were volatilized, but Cu remained in the solid residue. Finally, the volatilization ratio of zinc increased with the addition of carbon, and more than 98% of zinc was volatilized at 1173 K from a fly ash with a carbon content of 20%.     

Elemental Mercury Control by Novel Oxidant and Sorbent in an Entrained-Flow System

An entrained-flow system has been designed and constructed to simulate in-flight mercury capture by sorbents in ducts of coal-fired utility plants. The test conditions of 1.5 s residence time, 140°C temperature, 4.5 ppbv inlet Hg⁰ concentration, and 0–20 lb/MMacf sorbent injection rates were chosen to simulate conditions in the ducts. Novel oxidants developed in previous fixed-bed tests and novel sorbents derived from the novel oxidants were tested for their Hg⁰ capture in the entrained-flow system to examine the possibility of using those sorbents in a full-scale system. Darco-FGD and Darco Hg-LH served as benchmark sorbents with which mercury control capability of the novel oxidants and novel sorbents could be compared. The test results showed that the novel oxidants have remarkable Hg⁰ oxidation capability, and the novel sorbents showed a better performance in Hg⁰ removal than Darco Hg-LH.     

剑麻纤维基多孔炭材料的制备及其吸附氯苯的研究

以剑麻纤维为原料,通过简易的一步炭化活化法制备了一系列多孔炭材料,分别探究了3种温和的金属盐活化剂、活化剂与剑麻纤维的质量比和活化温度对炭材料的氯苯吸附量的影响,并通过BET、SEM、XRD、Raman、FT-IR、元素分析等手段表征其物理化学性质.结果表明,当采用CuCl₂为活化剂、CuCl₂与剑麻纤维的质量比为10∶1及活化温度为800℃时,制备得到的剑麻纤维基多孔炭(PCC)吸附性能最佳,其在氯苯浓度为1560 mg·m^-3时,吸附量达到856 mg·g^-1,而未经CuCl₂活化的炭材料(PC)的氯苯吸附量仅为15 mg·g^-1.氯苯吸附性能的提升主要归因于比表面积、孔容、无序性和表面含氧官能团的增加.此外,采用巨正则系综蒙特卡洛(GCMC)方法模拟氯苯分子在制备的多孔炭材料中的吸附行为,结果表明,该材料中孔径为0.5 nm的孔对氯苯分子的吸附能力最强,且对氯苯吸附起主导作用的为苯环中心和Cl原子与炭材料上连接含氧官能团的H原子之间的静电作用力.     

兰州地区大气污染的化学组成及来源解析

为探究大气污染的特征,于2020年5月—2021年4月在中国西北部的兰州市区采集了总悬浮颗粒物样品227个,利用离子色谱仪、热/光碳分析仪对主要水溶性离子、元素碳(EC)和有机碳(OC)的质量浓度进行了测定.结果显示,兰州地区大气总悬浮颗粒物质量浓度均值为(376.7±974.8)μg·m^-3,高于国家环境空气质量二级标准(NAAQS),呈昼低夜高的变化特征主要是由于兰州地区夜间大气多处于静稳状态导致的污染物累积效应.水溶性阴、阳离子按质量浓度排序为NO₃^->SO₄^2->Cl^-、Ca²⁺>NH₄⁺>Na⁺>K⁺>Mg²⁺,其中二次离子(NO₃^-、SO₄^2-、NH₄⁺     

碳包覆Pd/Al2O3催化剂催化4-溴苯酚加氢脱溴的活性和稳定性调控研究

在污染物液相催化加氢脱卤过程中,提高催化剂的稳定性至关重要.以水热合成法制备了不同碳包覆量的Pd/Al₂O₃@C催化剂,对催化剂进行了系列表征,并将催化剂应用于4-溴苯酚(4-BP)污染物的催化加氢脱溴反应.表征结果显示碳层提高了Pd/Al₂O₃的表面疏水性,有利于4-BP在催化剂上的吸附.并且在Pd/Al₂O₃@C催化剂的碳化过程中,碳还原部分Pd颗粒,并保留部分正价态Pd活性位,增强了4-BP中C-Br键的活化.与Pd/Al₂O₃相比,碳涂层提高了催化剂的催化活性.但当碳包覆量超过最佳包覆量后,暴露的Pd粒子随碳包覆量的增加而减少,导致活性下降.此外,碳层修饰后,催化剂的稳定性显著提高,从而大大抑制了Pd粒子的团聚和损耗.Pd/Al₂O₃@C表面的碳涂层对卤素具有较高的耐受性,从而减轻了液相催化加氢脱卤反应中活性中心的中毒.     

北方泥炭地泥炭土矿化速率、温度敏感性及其影响因素研究

北方泥炭地是全球重要的碳汇,也是全球变暖最为敏感的区域之一.然而,由于泥炭地表层和亚表层泥炭土碳排放过程对全球变暖的响应过程及机制仍存在一定争议,目前对全球变暖背景下泥炭地碳排放的认识仍存在一定不足.本研究于2019年8月在大兴安岭满归泥炭地采集表层(0～10 cm)和亚表层(15～30 cm)泥炭土进行室内增温模拟有氧培养,测定其矿化速率、有机质性质和水解酶活性.结果表明,表层泥炭土矿化速率在5、15、25℃下培养时((142.8±66.9)～(545.3±30.6)、(575.0±62.1)～(1843.0±547.4)、(888.4±123.9)～(3646.7±167.9)μg·g^-1·d^-1)均高于亚表层((113.0±41.5)～(367.1±64.1)、(357.4±52.3)～(1122.1±218.8)、(697.1±38.1)～(2336.4±150.6)μg·g^-1·d^-1),但表层和亚表层矿化作用的温度敏感性不具有显著差异;培养过程中,表层与亚表层泥炭土β-1,4-N-乙酰葡...     

碳中和目标下中国省域碳平衡能力与城镇化的关系

厘清碳平衡能力与城镇化的关系对实现碳中和目标和推动新型城镇化发展具有重要的理论价值及实践意义。采用温室气体清单法、碳吸收清查法、碳平衡指标法和多元城镇化测量法分别测算1999—2018年中国省域碳平衡能力与各类城镇化指标,利用空间自然断点分级法和Granger因果检验法分别分析中国省域碳平衡能力与城镇化的时空演变特征及互动关系。主要结论如下：（1）中国碳排放不断增多,碳吸收不断减少,碳平衡能力呈上升、下降、先减后增和先增后减四种趋势,碳排放呈“东多西少”分布,碳吸收与碳平衡能力分别呈“西多东少”和“西强东弱”分布。（2）中国人口、经济、空间、生态城镇化和城镇化综合指标不断提升,其中空间城镇化大致呈“西高东低”分布,其余则呈“东高西低”分布。（3）除空间城镇化外,中国整体碳平衡能力与各类城镇化的关系均为反馈型,而各省域增长保护型数量最多,中立型数量最少。