沈阳市郊区环境空气中醛酮类化合物的污染特征与来源分析

为探究沈阳市郊区环境空气中醛酮类化合物的污染特征,于2017年8月24日—9月2日采用2,4-二硝基苯肼固相吸附/高效液相色谱方法对沈阳市郊区醛酮类化合物进行观测分析,利用美国环境保护局推荐的人体健康风险评价方法对部分有毒有害醛酮类化合物的人体健康风险进行了评价,并利用比值法对醛酮类化合物的来源进行了初步分析.结果表明:醛酮类化合物质量浓度日均值范围为23.16~38.38 μg/m3;质量浓度最高的4种醛酮类化合物依次是丙酮、甲醛、正丁醛和乙醛,其质量浓度日均值的平均值分别为8.71、5.90、5.48和2.95 μg/m3.对·OH消耗速率(L_OH)贡献较大的醛酮类化合物物种是正丁醛、甲醛和乙醛,臭氧生成潜势贡献(OFP)较大的醛酮类化合物物种是甲醛、正丁醛和乙醛,在研究区影响醛酮类化合物光化学反应活性的物种主要是甲醛、乙醛和正丁醛.研究区观测期间,环境空气中甲醛和乙醛的致癌性风险值分别为1.18×10-5和5.91×10-6,对暴露人群存在潜在的致癌风险;乙醛的非致癌风险值为0.05,对暴露人群不存在非致癌风险.在研究区的一次臭氧轻度污染过程期间,环境空气中的甲醛和乙醛受天然源排放的挥发性有机物二次转化的影响减弱,甲醛、乙醛和丙酮受到炼焦工业和机动车等人为源排放的影响增强,而正丁醛主要受当地精细化工产业排放的影响.研究显示,沈阳市应加大对炼焦工业、精细化工和机动车来源排放醛酮类化合物的管制,以降低环境空气中活性醛酮类化合物及有毒有害醛酮类化合物的浓度.      

Green innovation efficiency across China’s 30 provinces: estimate,comparison, and convergence

Mitigation and Adaptation Strategies for Global Change - Considering government and market failure of environmental regulation to combat increasing GHG (greenhouse gas) emissions, green innovation...     

土地承载力研究范式的变迁、分化及其综论

基于Kuhn范式理论,将现有土地承载力研究成果显化、梳理为4种主要研究范式,即基于限制因子的研究范式、基于多因素综合的研究范式、基于参照区的研究范式、基于生态足迹的研究范式。以范式应用的时代背景、空间尺度为着眼点,对各类范式进行综合比较,结果显示：基于限制因子的土地承载力研究范式起源最早、发展最为成熟,基于多因素综合、基于参照区、基于生态足迹的3种研究范式,均是以前者为基础,按照不同的方向分化而成;范式分化的原因在于时空条件的变化所引致的亟需解释、解决的现实问题的变化。范式本身并无优劣之分,但有其独特的适应性：基于限制因子、基于生态足迹的两种研究范式适用于全球及国家等大尺度土地承载力问题,且发展较为成熟,其成果具有较强的理论和实践指导意义;基于多因素综合及基于参照区的两种研究范式适用于市县等中小尺度,但其研究较为薄弱,所得的承载力分值、承载力相对值对区域土地管理实践的指导价值有限。当前,市县等中小尺度土地承载力研究亟需加强,其指导实践的有效性与可操作性亟待大幅度提高。     

生物基聚合物PHBV和PLA复合材料在不同介质中的生物降解及其影响因素

传统工艺的塑料生产不仅依赖石油资源的持续开发利用,同时给环境造成了前所未有的压力,近年来生物基聚合物（聚（3-羟基-3-戊酸酯）-PHBV,聚乳酸-PLA）日渐成为传统石油基塑料的替代产品.本文采用呼吸测试手段,旨在揭示均质复合材料在不同环境介质（土壤、熟化堆肥、水体）条件下及有机添加剂（木质素）,无机添加剂（蒙脱石）和天然有机物链增长剂（Joncryl）作用下的生物降解特征.结果表明：当链增长剂Joncryl添加量为5%时,对所有介质PHBV和PLA复合材料产生显著抑制作用.Joncryl添加量为0.2%时,未对所测样品的生物降解行为产生干扰作用.在熟化堆肥介质中,PLA复合材料比PHBV基质混合物的生物降解速率明显降低.有机木质纤维添加剂（榛子壳粉末）单独在聚合物中添加或者和链增长剂Joncryl以及非有机添加剂（Dellite72T）共同作用下都可促进PLA聚合物中各组分的相容连接性.实验结果表明,新型添加剂在不同介质中以二元或三元添加的方式对生物降解过程产生重要影响,该研究将为新型材料使用后的生物降解效应提供理论依据.     

Effects of Na+ on Cu/SAPO-34 for ammonia selective catalytic reduction

Copper-exchanged chabazite (Cu/CHA) catalysts have been found to be affected by alkali metal and alkaline earth ions. However, the effects of Na⁺ ions on Cu/SAPO-34 for ammonia selective catalytic reduction (NH₃-SCR) are still unclear. In order to investigate the mechanism, five samples with various Na contents were synthesized and characterized. It was observed that the introduced Na⁺ ion-exchanges with H⁺ and Cu^2 + of Cu/SAPO-34. The exchange of H⁺ is easier than that of isolated Cu^2 +. The exchanged Cu^2 + ions aggregate and form “CuAl₂O₄-like” species. The NH₃-SCR activity of Cu/SAPO-34 decreases with increasing Na content, and the loss of isolated Cu^2 + and acid sites is responsible for the activity loss.     

Seasonal variation and size distribution of biogenic secondary organic aerosols at urban and continental background sites of China

Size-resolved biogenic secondary organic aerosols(BSOA) derived from isoprene and monoterpene photooxidation in Qinghai Lake, Tibetan Plateau(a continental background site) and five cities of China were measured using gas chromatography/mass spectrometry(GC/MS). Concentrations of the determined BSOA are higher in the cities than in the background and are also higher in summer than in winter. Moreover, strong positive correlations(R2= 0.44–0.90) between BSOA and sulfate were found at the six sites,suggesting that anthropogenic pollution(i.e., sulfate) could enhance SOA formation,because sulfate provides a surface favorable for acid-catalyzed formation of BSOA. Size distribution measurements showed that most of the determined SOA tracers are enriched in the fine mode( 3.3 μm) except for cis-pinic and cis-pinonic acids, both presented a comparable mass in the fine and coarse( 3.3 μm) modes, respectively. Mass ratio of oxidation products derived from isoprene to those from monoterpene in the five urban regions during summer are much less than those in Qinghai Lake region. In addition, in the five urban regions relative abundances of monoterpene oxidation products to SOA are much higher than those of isoprene. Such phenomena suggest that BSOA derived from monoterpenes are more abundant than those from isoprene in Chinese urban areas.     

Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China

Owing to the vast territory of China and strong regional characteristic of ozone pollution,it's desirable for policy makers to have a targeted and prioritized regulation and ozone pollution control strategy in China based on scientific evidences. It's important to assess its current pollution status as well as spatial and temporal variation patterns across China.Recent advances of national monitoring networks provide an opportunity to insight the actions of ozone pollution. Here, we present rotated empirical orthogonal function(REOF)analysis that was used on studying the spatiotemporal characteristics of daily ozone concentrations. Based on results of REOF analysis in pollution seasons for 3 years' observations, twelve regions with clear patterns were identified in China. The patterns of temporal variation of ozone in each region were separated well and different from each other, reflecting local meteorological, photochemical or pollution features. A rising trend in annual averaged Eight-hour Average Ozone Concentrations(O_3-8 hr) from 2014 to 2016 was observed for all regions, except for the Tibetan Plateau. The mean values of annual and 90 percentile concentrations for all 338 cities were 82.6 ± 14.6 and 133.9 ± 25.8 μg/m~3,respectively, in 2015. The regionalization results of ozone were found to be influenced greatly by terrain features, indicating significant terrain and landform effects on ozone spatial correlations. Among 12 regions, North China Plain, Huanghuai Plain, Central Yangtze River Plain, Pearl River Delta and Sichuan Basin were realized as priority regions for mitigation strategies, due to their higher ozone concentrations and dense population.