Spatially distributed modeling of the long-term carbon balance of a boreal landscape

Spatially and temporally distributed information on the sizes of biomass carbon (C) pools (BCPs) and soil C pools (SCPs) is vital for improving our understanding of biosphere-atmosphere C fluxes. Because the sizes of C pools result from the integrated effects of primary production, age-effects, changes in climate, atmospheric CO₂ concentration, N deposition, and disturbances, a modeling scheme that interactively considers these processes is important. We used the InTEC model, driven by various spatio-temporal datasets to simulate the long-term C-balance in a boreal landscape in eastern Canada. Our results suggested that in this boreal landscape, mature coniferous stands had stabilized their productivity and fluctuated as a weak C-sink or C-source depending on the interannual variations in hydrometeorological factors. Disturbed deciduous stands were larger C-sinks (NEP₂₀₀₄ = 150 gC m⁻² yr⁻¹) than undisturbed coniferous stands (e.g. NEP₂₀₀₄ = 8 gC m⁻² yr⁻¹). Wetlands had lower NPP but showed temporally consistent C accumulation patterns. The simulated spatio-temporal patterns of BCPs and SCPs were unique and reflected the integrated effects of climate, plant growth and atmospheric chemistry besides the inherent properties of the C pool themselves. The simulated BCPs and SCPs generally compared well with the biometric estimates (BCPs: r = 0.86, SCPs: r = 0.84). The largest BCP biases were found in recently disturbed stands and the largest SCP biases were seen in locations where moss necro-masses were abundant. Reconstructing C pools and C fluxes in the ecosystem in such a spatio-temporal manner could help reduce the uncertainties in our understanding of terrestrial C-cycle.     

同源地人工湖水体和底泥中有机物组成及有机结构的分析研究

采用XAD-8大孔吸附树脂对水体和底泥中的有机物进行组分分离,并通过傅里叶变换红外光谱(FTIR)、紫外-可见光谱(UV-Vis)和三维荧光光谱(3DEEMs)对自然水体和底泥中的疏水酸(腐殖酸、富里酸)、疏水碱、疏水中性物质和亲水物质进行表征和对比.结果表明,水体中有机物含量:亲水物质富里酸腐殖酸疏水碱疏水中性物质,底泥中有机物的含量为:腐殖酸富里酸亲水物质疏水碱疏水中性物质.根据红外、紫外、三维荧光光谱可知底泥中有机物的芳香程度、不饱和程度及分子量大小略高于水体有机物.根据荧光指数(FI)和自生源指标(BIX)可知,底泥和水体的腐殖酸和富里酸主要来源于陆生动植物和土壤有机质,而其余物质主要源于细菌和藻类活动.     

2015年干季佛山一次重空气污染过程形成机理研究

2015年12月21-23日,广东珠三角佛山地区出现了一次PM_2.5重污染过程.利用佛山地区顺德、禅城、三水3个站点风廓线雷达、激光雷达和微波辐射计观测资料,结合地面气象观测数据和污染物浓度数据,分析研究了这次重污染过程的形成机理.结果表明：1形成这次污染过程的主要原因是近地层偏南风和偏北风对峙导致水平风速减小,大气水平输送能力变差;持续时间长且强度达到3℃·km^-1的强逆温抑制了污染物的垂直扩散;800 m以下超过90%的高相对湿度造成气溶胶粒子吸湿增长显著.2持续时间长且比较深厚的小风层是造成这次污染过程的直接原因,小风层厚度是预报空气质量变化的较好工具.与地面风速相比,PM_2.5浓度与小风层厚度的相关系数最多能提高0.36,且具有较长的预报时效.佛山地区小风层的风速阈值为3.8 m·s^-1.3这次污染过程存在两种不同的污染形成机制,污染前期（21-23日中午）主要以本地污染物累积为主,污染后期（23日下午）下风向地区（三水）的污染主要是受上风向地区（顺德和禅城）的污染输送影响.     

佛山地区干季边界层垂直风温结构对空气质量的影响

利用佛山地区2013年12月大气边界层观测试验得到的垂直风温资料和相应逐日AQI资料、逐时PM_(2.5)浓度资料,研究了佛山地区大气边界层垂直风温结构对空气质量的影响.结果表明:佛山地区干季持续存在的逆温结构是导致PM_(2.5)污染较重的重要原因.干季污染日近60%的最低逆温层高度低于1000 m,而非污染日低于1000 m的最低逆温层仅占36%,污染日佛山贴地逆温频率高达31.2%.逆温层出现高度较低,将污染物压缩积累在贴地层大气中导致污染较重.在大陆冷高压控制下,佛山地区的边界层结构演化非常典型,最大边界层高度和最大边界层通风量表现出了显著相关,污染日日平均边界层高度始终维持在较低的水平,多数时候不足500 m,最大边界层高度则大部分小于1000 m,日平均边界层通风量主要分布在500~1500 m~2·s~(-1)之间,在极端情况下甚至不足300 m~2·s~(-1),最大边界层通风量大部分处于1500~5000 m~2·s~(-1)之间,导致污染物始终聚集在较低的大气边界层内,使得PM_(2.5)浓度长时间维持在较高的污染水平.佛山地区风场存在显著的3层结构,较小的底层风速意味着大气的输送和扩散能力较弱,高度较低的中层使得污染物进一步被压缩累积在大气底层,垂直风场的不稳定性使得污染日佛山地区局地回流活跃,回流(RF)指数极小值多分布在0.2~0.4之间,污染日RF指数普遍小于非污染日,垂直风场的有效输送能力被显著削弱.     

Quantum chemical investigation on photodegradation mechanisms of sulfamethoxypyridazine with dissolved inorganic matter and hydroxyl radical

Sulfamethoxypyridazine(SMP) is one of the commonly used sulfonamide antibiotics(SAs).SAs are mainly studied to undergo triplet-sensitized photodegradation in water under natural sunlight with other coexisting aquatic environmental organic pollutants.In this work,SMP was selected as a representative of SAs.We studied the mechanisms of triplet-sensitized photodegradation of SMP and the influence of selected dissolved inorganic matter,i.e.,anions(Br~-,Cl~-,and NO~-_3) and cations ions(Ca~(2+),Mg~(2+),and Zn~(2+)) on SMP photodegradation mechanism by quantum chemical methods.In addition,the degradation mechanisms of SMP by hydroxyl radical(OH·) were also investigated.The creation of SO_2 extrusion product was accessed with two different energy pathways(pathway-1 and pathway-2) by following two steps(step-I and step-II) in the tripletsensitized photodegradation of SMP.Due to low activation energy,the pathway-1 was considered as the main pathway to obtain SO_2 extrusion product.Step-II of pathway-1 was measured to be the rate-limiting step(RLS) of SMP photodegradation mechanism and the effect of the selected anions and cations was estimated for this step.All selected anions and cations promoted photodegradation of SMP by dropping the activation energy of pathway-1.The estimated low activation energies of different degradation pathways of SMP with OH·radical indicate that OH·radical is a very powerful oxidizing agent for SMP degradation via attack through benzene derivative and pyridazine derivative ring.     

Simulated reaction of formaldehyde and ambient atmospheric particulate matter using a chamber

The reaction of HCHO with Beijing winter's real ambient particulate matter(PM) inside a 3.3 m~3 Teflon Chamber was conducted in this study. NO_2, O_3 and H_2O gases were removed from the ambient aerosol before entering into the chamber. The decays of HCHO were monitored(acetylacetone spectrophotometry method) during the reactions at different PM number concentrations(N_a) and relative humidities(RHs), and the formed particulate formate was detected by IC and XPS techniques. The results showed that when RH was10%–15%, the decay rate of HCHO in the chamber was higher with the existence of PM from relatively clean days(with number concentration(N_a) 200,000 particle/L, 0.35–22.5 μm)compared to dirty days(N_a 200,000 particle/L, 0.35–22.5 μm). When RH increased to 30%–45%, PM can hardly have significant influences on the decay of HCHO. The formations of formate on the reacted PM were consistent with the HCHO decay rates at different ambient PM N_aand RH conditions. This is a first study related to the "real" ambient PM reacted with HCHO and suggested that in the clean and low RH days, PM could be an effective medium for the conversion of HCHO to formate.     

阜新城区降尘重金属污染及其健康风险评价

为研究阜新市大气降尘重金属分布情况及可能存在的健康风险,于2015年3月—2016年3月对阜新城区(32个采样点)及周边地区(13个对照采样点)进行大气降尘湿法采集,并利用电感耦合等离子体质谱仪(ICP-MS)对降尘中的7种重金属元素(Cr、Ni、Zn、Cd、Pb、As、Cu)含量进行测定.结果表明:① 阜新市大气降尘中重金属含量存在明显差异,表现为w(Zn)＞w(Pb)＞w(Cr)＞w(Cu)＞w(Ni)＞w(As)＞w(Cd). w(Zn)平均值最高,为756.9 mg/kg; w(Cd)平均值最低,为4.8 mg/kg,其他几种重金属含量范围为10~120 mg/kg. ② 城区大气降尘中Cd的背景比值(H)最高,为44.89,其次为Zn(H=11.92),城区大气降尘重金属污染受人为活动影响显著. ③ 地累积指数评价结果显示,Cd为严重-极度污染,Zn为中度-严重污染,Pb、Cu为中度污染,Cr、Ni为轻度污染,As为无污染. ④ 研究区健康风险评价表明,儿童通过3种暴露途径接触Cu、Zn、Pb、Cd、Ni的非致癌健康风险水平均高于成人,Cr、As的非致癌健康风险水平低于成人. ⑤ Cr经呼吸途径对成人的非致癌风险(HQ_inh)达2.53,非致癌风险总值(HI)达3.41,均大于限值(1),表明Cr经呼吸途径对于成人存在非致癌风险,其余6种重金属元素经呼吸途径对于成人的非致癌风险相对较低. ⑥ Cd、Cr、As、Ni经呼吸途径的致癌风险值(10-9~10-7)均低于可接受水平(10-6),表明致癌元素Cd、Cr、As、Ni经呼吸途径对人体可能不具有致癌风险.鉴于研究区大气降尘重金属元素经3种途径对成人、儿童均构成一定非致癌风险,阜新市应当及时加强对海州露天矿、经济开发区及皮革工业园等主要大气颗粒物污染源的排放及监测管控.      

覆盖金属氧化物对湖泊沉积物溶解性有机质特征的影响

为揭示不同金属氧化物对湖泊沉积物DOM（溶解性有机质）影响机制,通过室内模拟试验,在沉积物表层分别覆盖Fe、Al、Mn氧化物及湖沙后培养1 a,并利用三维荧光和紫外光谱方法进行表征.结果表明:① 覆盖Al、Fe、Mn氧化物和湖沙主要降低了0~3 cm沉积物的w（DOC）,降幅分别为8.61%、6.27%、22.38%和0.44%. ② 沉积物中DOM的类络氨酸峰（peak B₁）和类色氨酸峰（peak T₂）均产生较大变化.其中三种氧化物均显著降低了上层沉积物中DOM的peak T₂,使底层DOM的peakT₂显著增加. Mn氧化物使DOM的peak B₁降低,Fe和Al氧化物使DOM的peak B₁增加,湖沙则使两类峰均降低. ③ 覆盖金属氧化物改变了沉积物DOM结构特征,其中覆盖Fe氧化物增强了其芳香性,而覆盖Mn氧化物和Al氧化却降低其芳香性,但三者均使DOM腐质化程度及官能团数量增加,并使FI（Fluorescence Index,荧光指数）增大,表明DOM向生物源转化.研究显示,沉积物表层覆盖金属氧化物影响了沉积物中DOM迁移和转化,并促进了其降解,导致其分子量和腐殖化程度增加.      

Effects of Cu2+ and humic acids on degradation and fate of TBBPA in pure culture of Pseudomonas sp. strain CDT

Soil contamination with tetrabromobisphenol A(TBBPA) has caused great concerns;however, the presence of heavy metals and soil organic matter on the biodegradation of TBBPA is still unclear. We isolated Pseudomonas sp. strain CDT, a TBBPA-degrading bacterium, from activated sludge and incubated it with ~(14)C-labeled TBBPA for 87 days in the absence and presence of Cu~(2+)and humic acids(HA). TBBPA was degraded to organic-solvent extractable(59.4% ± 2.2%) and non-extractable(25.1% ± 1.3%) metabolites,mineralized to CO_2(4.8% ± 0.8%), and assimilated into cells(10.6% ± 0.9%) at the end of incubation. When Cu~(2+)was present, the transformation of extractable metabolites into non-extractable metabolites and mineralization were inhibited, possibly due to the toxicity of Cu~(2+)to cells. HA significantly inhibited both dissipation and mineralization of TBBPA and altered the fate of TBBPA in the culture by formation of HA-bound residues that amounted to 22.1% ± 3.7% of the transformed TBBPA. The inhibition from HA was attributed to adsorption of TBBPA and formation of bound residues with HA via reaction of reactive metabolites with HA molecules, which decreased bioavailability of TBBPA and metabolites in the culture. When Cu~(2+)and HA were both present, Cu~(2+)significantly promoted the HA inhibition on TBBPA dissipation but not on metabolite degradation. The results provide insights into individual and interactive effects of Cu~(2+)and soil organic matter on the biotransformation of TBBPA and indicate that soil organic matter plays an essential role in determining the fate of organic pollutants in soil and mitigating heavy metal toxicity.