天然沸石定向合成A型分子筛及其脱氮性能

针对污水厂尾水深度脱氨问题,以河南巩义的天然沸石为起始原料,采用常压水热合成方法,选用4种不同的工艺方案合成A型分子筛,并对合成产物的吸附氨氮性能及其纯度、晶体结构、形貌特征、孔隙率等材料结构特征进行分析与表征,探讨天然沸石制备高效脱氨分子筛的合成方法.结果表明：与直接碱溶法制备硅源相比,碱熔融活化法对沸石原料硅的利用率较高,硅源纯化合成方案产物的氨氮吸附性能显著得到改善,平衡吸附量达20mg/g以上;其晶体形貌规整有序、杂质含量低、孔道通畅,有利于吸附扩散与传质过程.综合考虑硅源制备能耗、物耗及合成产物吸附性能,天然沸石合成A型分子筛适宜的工艺方案为碱溶纯化合成法.     

海绵城市建设的水质水量控制效果实证研究:以鹤壁试点区为例

首批国家海绵城市试点建设已经完成,有关海绵城市规划与模型模拟的研究也层出不穷,但是对于海绵建设区开展持续监测并进行深入分析的研究较为缺乏,而对于海绵城市实际建设区的水质水量研究是规划建设理论与实践效果差别的唯一检测器,是优化未来海绵城市规划和建设的关键。以河南省鹤壁市国家海绵城市建设试点区为研究对象,开展试点区地表水体与雨水管网的水质水量多年持续监测研究,分析海绵城市建设对地表水主要水质指标和雨水年径流总量控制率的实践作用效果。采用人工监测与设备在线监测相结合的方式,于2015-08—2018-09在海绵城市试点区地表水体10个采样点进行了16次人工采样,共计获得109个地表水样并测定了常规水质。利用试点区内20个雨水管道出口处的流量在线监测设备获得2018-01—12的分钟级流量数据。结果表明:研究区域内波动较大的水质指标为NH₃-N、TN和DO,波动较小的为pH。与海绵城市建设前相比,研究区域的地表水系水质得到改善,试点区该年度的雨水径流总量控制率达到85.7%,满足规划建设要求指标70%。但当实际场次降雨量低于设计雨量23 mm时,仍有雨水外排。不同地块的径流控制率差异明显。以上结果丰富了海绵城市建设的实践研究,可为优化海绵城市的规划与设计建设提供参考。     

厨余和餐厨垃圾混合干式厌氧发酵及活性炭缓解酸抑制研究

分别在中温和高温条件下对厨余垃圾与餐厨垃圾混合干式厌氧发酵产甲烷特性进行研究,结果表明:55℃高温发酵累积产气量均高于35℃中温组;高温组厨余垃圾与餐厨垃圾配比为1:5时发酵累积产气量最大,最大累积产气量达到2492.5 mL,是中温组协同产甲烷的1.4倍。同时,为提高产气率,考察了不同种类活性炭对厌氧发酵的影响,采用甘蔗皮、秸秆、花生藤蔓以及发酵沼渣为原料自制了4种生物质活性炭。实验结果表明,4种活性炭均呈蜂窝煤状的炭孔,其中甘蔗皮活性炭表面炭孔相对规则、完整,微生物可附着面积大,更有利于加快产气进程。添加甘蔗皮活性炭时累积产气3410 mL,相比空白对照组增长20.1%。     

Effect of Al2O3 doping on the structure and performance of an Al2O3/Fe2O3 catalyst for mercury oxidation

In this study,the thermal stability of a Fe_2 O_3 catalyst for mercury oxidation was significantly improved by doping with Al_2 O_3.After 1 hr,the catalyst doped with 10 wt.% Al_2 O_3 still exhibited a mercury conversion efficiency of 70.9%,while the undoped sample even lost its catalytic activity.Doping with Al_2 O_3 retarded the collapse of the catalyst mesoporous structure during high-temperature calcination,and the doped samples maintained a higher specific surface area,smaller pore size,and narrower pore size distribution.Transmission electron microscope images revealed that after calcination at 350℃,the average size of the catalyst grains in Fe_2 O_3 was 23.4 nm;however,the corresponding values for 1%Al_2 O_3/Fe_2 O_3,3%Al_2 O_3/Fe_2 O_3,and 10%Al_2 O_3/Fe_2 O_3 were only 13.3,7.1,and 4.7 nm,respectively.Results obtained from X-ray diffraction and thermogravimetry coupled with differential scanning calorimetry confirmed that doping with Al_2 O_3 also retards the crystallization of the catalysts at high temperature,constraining catalyst grains to a smaller size.     

Cause of PM2.5 pollution during the 2016-2017 heating season in Beijing, Tianjin, and Langfang, China

To investigate the cause of fine particulate matter (particles with an aerodynamic diameter less than 2.5 µm, PM_2.5) pollution in the heating season in the North China Plain (specifically Beijing, Tianjin, and Langfang), water-soluble ions and carbonaceous components in PM_2.5 were simultaneously measured by online instruments with 1-hr resolution, from November 15, 2016 to March 15, 2017. The results showed extreme severity of PM_2.5 pollution on a regional scale. Secondary inorganic ions (SNA, i.e., NO₃^?+SO₄²+ NH₄⁺) dominated the water-soluble ions, accounting for 30%-40% of PM_2.5, while the total carbon (TC, i.e., OC + EC) contributed to 26.5%-30.1% of PM_2.5 in the three cities. SNA were mainly responsible for the increasing PM_2.5 pollution compared with organic matter (OM). NO₃^? was the most abundant species among water-soluble ions, but SO₄^2- played a much more important role in driving the elevated PM_2.5 concentrations. The relative humidity (RH) and its precursor SO₂ were the key factors affecting the formation of sulfate. Homogeneous reactions dominated the formation of nitrate which was mainly limited by HNO₃ in ammonia-rich conditions. Secondary formation and regional transport from the heavily polluted region promoted the growth of PM_2.5 concentrations in the formation stage of PM_2.5 pollution in Beijing and Langfang. Regional transport or local emissions, along with secondary formation, made great contributions to the PM_2.5 pollution in the evolution stage of PM_2.5 pollution in Beijing and Langfang. The favourable meteorological conditions and regional transport from a relatively clean region both favored the diffusion of pollutants in all three cities.     

锰基改性生物炭对弱碱性Cd污染土壤团聚体结构以及Cd含量特征的影响

通过田间试验,探究锰基改性稻壳生物炭对弱碱性Cd污染土壤有机碳含量、团聚体结构以及团聚体各粒级的Cd质量负载和有效态含量的影响.结果表明,施加改性生物炭,土壤有机碳含量表现为随着改性生物炭施加量的增加而呈现出逐渐升高的趋势,较对照增加了3.2%～32.0%.改性生物炭对土壤团聚体的分布结构和稳定性具有改良作用,增加了大团聚体(5～8 mm和2～5 mm粒级)所占的质量分数,微团聚体(≤0.25 mm)则受到抑制,土壤团聚体平均质量直径(GWD)、几何平均直径(MWD)和土壤团粒结构体(R_(0.25))较对照分别增加了15.1%～20.3%、 8.1%～22.4%和0.43%～7.6%.Cd含量主要富集在团聚体小颗粒中,其在土壤团聚体各粒级的质量负载随粒径的减小而逐渐增大.Cd分布因子在0.5～1 mm和0.25～0.5 mm粒级中表现出明显富集状况,而在5～8 mm和2～5 mm粒径中表现出明显亏损状态.与对照相比,添加改性生物炭降低了全土和土壤团聚体各粒级中DTPA-Cd含量,其中在5～8、 2～5、 0.5～1.0和0.25～0.5 mm粒径中分别降低了7.6%～15.1%、 15.6%～24.3%、 3.6%～13.8%和11.6%～13.7%(P0.05).总体而言,改性生物炭不仅对污染土壤团聚体的结构具有良好的优化作用,而且能够降低不同粒径土壤中Cd有效态含量,达到阻控修复Cd污染的目的.     

不同排放源对华东地区PM2.5影响的数值模拟

使用中尺度气象-化学耦合模式WRF-Chem针对MEIC源清单中五大部门来源（工业源、电力源、民用源、交通源和农业源）对华东地区PM_2.5的影响进行了模拟研究,主要得到以下结论：春夏秋季PM_2.5约40%~60%来源于工业源,冬季由于采暖供热燃用大量散烧煤,导致民用源对PM_2.5的贡献最大,在山东、安徽和江苏省等高值区贡献率超过50%;农业源、电力源和交通源对PM_2.5影响的季节差异不大,农业源贡献约20%~30%,交通源和火电源贡献约10%.因此冬季需主要控制民用源排放,春夏秋季主要控制工业源排放,其次是农业源排放.一次PM_2.5在工业、电力和民用源贡献的PM_2.5中所占比例可达50%~60%;NO₃^-和NH+4在交通源贡献的PM_2.5中总比例可达53%,在农业源中总比例高达93%;由于模式对SO₄^2-模拟偏低,SO₄^2-在工业源和电力源贡献的PM_2.5中占比约5%~15%;OC对来自民用源的PM_2.5有30%的贡献,BC对来自交通源的PM_2.5有15%的贡献;Na⁺和Cl^-对PM_2.5的贡献在各大来源中均低于3%.     

中国CDM项目开发现状及存在问题分析研究

清洁发展机制(CDM)是国际社会实现温室气体减排的履约机制之一。目前中国已成为CDM市场的主要输出国,但在CDM项目开发过程中还存在很多问题,例如区域分布不平衡、碳排放权交易标准不统一、缺乏激励机制等。在经济发展和节能减排的双重压力下,中国政府声明将严格遵守《巴黎协定》,正在积极落实已提出的到2020年控制温室气体排放行动目标,并向联合国提交了到2030年的"国家自主贡献"行动目标。中国的积极行动推动了全球气候问题的解决。     

Using X-ray computed tomography and micro-Raman spectrometry to measure individual particle surface area, volume, and morphology towards investigating atmospheric heterogeneous reactions

Heterogeneous reactions on the aerosol particle surface in the atmosphere play important roles in air pollution, climate change, and global biogeochemical cycles. However, the reported uptake coefficients of heterogeneous reactions usually have large variations and may not be relevant to real atmospheric conditions. One of the major reasons for this is the use of bulk samples in laboratory experiments, while particles in the atmosphere are suspended individually. A number of technologies have been developed recently to study heterogeneous reactions on the surfaces of individual particles. Precise measurements on the reactive surface area, volume, and morphology of individual particles are necessary for calculating the uptake coefficient, quantifying reactants and products, and understanding the reaction mechanism better. In this study, for the first time we used synchrotron radiation X-ray computed tomography(XCT) and micro-Raman spectrometry to measure individual CaCO_3 particle morphology, with sizes ranging from 3.5–6.5 μm. Particle surface area and volume were calculated using a reconstruction method based on software threedimensional(3-D) rendering. The XCT was first validated with high-resolution fieldemission scanning electron microscopy(FE-SEM) to acquire accurate CaCO_3 particle surface area and volume estimates. Our results showed an average difference of only 6.1% in surface area and 3.2% in volume measured either by micro-Raman spectrometry or X-ray tomography. X-ray tomography and FE-SEM can provide more morphological details of individual Ca CO3 particles than micro-Raman spectrometry. This study demonstrated that X-ray computed tomography and micro-Raman spectrometry can precisely measure the surface area, volume, and morphology of an individual particle.     

成都市PM10中碳质气溶胶长期来源特点

大气颗粒物中包含多种组分的气溶胶,其中碳质气溶胶由于对人体健康、能见度有较大影响,已受到越来越多的关注.为研究碳质气溶胶的长期变化规律,采集了成都市2009—2013年的PM₁₀样品,对其中所含的无机元素、水溶性离子及碳组分分别进行测定,并使用“PMF（正定矩阵因子分解法）-比值”模型分别对PM₁₀和所含的碳质气溶胶的来源进行分析.结果表明,1月、2月、5月和12月的碳质气溶胶浓度较高,其中1月、2月和12月的OC/EC（有机碳与元素碳质量浓度之比）较高,并且PMF-比值模型计算结果也显示冬季SOC增多,表明冬季可能有更多的二次有机碳（SOC）生成;5月的char-EC/soot-EC（二者质量浓度之比,其中char-EC=EC1-OP,soot-EC=EC2+EC3,它们可更好地区分源类）较高,K含量也较高,表明可能有更多的生物质燃烧排放.PM₁₀解析共发现6类源,依次为地壳扬尘（26.5%）、二次硫酸盐（25.1%）、燃煤&生物质燃烧混合源（17.3%）、二次硝酸盐&二次有机碳混合源（12.3%）、机动车源（11.8%）和水泥尘源（7.0%）;碳质气溶胶解析发现,OC主要来源依次为机动车源（38.2%）、燃煤&生物质燃烧混合源（33.1%）和二次有机碳（25.3%）,char-EC的主要来源是燃煤&生物质燃烧混合源和机动车源,分别占50.5%和45.4%,soot-EC则主要受机动车影响（达73.2%）.研究显示,成都市PM₁₀主要来自于地壳扬尘、二次生成和燃煤&生物质燃烧,而碳质气溶胶主要来自于机动车、燃煤&生物质燃烧.