Advanced molecular-fingerprinting analysis of dissolved organic sulfur by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry using optimal spray solvent

Molecular level characterization of dissolved organic sulfur (DOS) by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS) is necessary for further understanding of the role of DOS in the environment. Here, ESI spray solvent, a key parameter for ion production during ESI process, was investigated for its effect on the molecular characterization of DOS by ESI-FTICR MS. 100% MeOH as spray solvent was found for the first time to remarkably enhance the ionization efficiency of the majority of CHOS-molecules in NOM, which facilitated a total of 1473 CHOS-molecular formulas with one sulfur atom to be detected. The number of CHOS-molecular formulas obtained using 100%MeOH as spray solvent increased notably over 740 in comparison with those using 50% MeOH aqueous solution (731) or 50% ACN aqueous solution (653). Moreover, due to the enhancement of ionization efficiency of DOS during ESI processes, the tandem mass spectra of the NOM CHOS-molecules could be easily obtained using 100% MeOH as spray solvent, which were hardly obtained using 50% MeOH aqueous solution as spray solvent. The results of the tandem mass spectra suggested the first discovery of organosulfates or sulfonic acids in Suwannee River NOM sample. A simple method based on 100% MeOH as ESI spray solvent for advanced molecular characterization of DOS by ESI-FTICR MS was proposed and applied, and the results revealed more molecular information of DOS in sea DOM samples.     

用EXAFS研究Zn在水锰矿上的吸附-解吸机理

用延展X光吸收精细结构光谱(EXAFS)研究了重金属Zn(Ⅱ)在水锰矿(γ-MnOOH)上吸附产物的微观结构及其吸附机理.结果表明,Zn(Ⅱ)-水锰矿体系中(pH 7.5,0.1mol/LNaNO₃介质,25℃),Zn²⁺主要是通过共用水合Zn²⁺的O原子及水锰矿表面上的O原子形成Zn-O键,从而结合到水锰矿固体表面上的.平均Zn-O原子间距为1.998±0.010 A(n=3).这个Zn-O键键长是六配位的Zn(H₂O)²⁺₆及其水解产物四配位的Zn(OH)₂或Zn(OH)₄^2-各以一定比例混合吸附于水锰矿表面而形成的.同时,对第二配位层(Zn-Mn相互作用)的EXAFS图谱分析证明存在2个典型的Zn-Mn原子间距,即R₁=3.08±0.024A(n=3)和R2=3.54±0.018 A(n=3).这2个Zn-Mn原子距分别对应于水锰矿结构单元MnO6八面体与Zn水合离子ZnO多面体结合的2种方式,即共用2个O原子的边-边结合与共用1个O原子的角-角结合.边-边结合是较强的吸附位,Zn-Mn原子距较短(R₁=3.08A),吸附较不可逆.角-角结合是较弱的吸附位,Zn-Mn原子距较长(R₂=3.54A),吸附较为可逆.这一结果从微观上证明了亚稳平衡态吸附理论(MEA理论)的基本假设,即具有相同吸附密度的同一吸附质由于吸附力强弱以及微观构型的不同可具有不同的化学位,因而证明了修正传统吸附热力学的基本假设(吸附密度为热力学状态函数)的必要性.宏观的吸附-解吸热力学实验表明Zn(Ⅱ)在水锰矿上的吸附是不可逆的,EXAFS结果指出这种不可逆性主要是由Zn水合离子中ZnO多面体与水锰矿结构单元MnO₆八面体之间的边-边结合所导致的.     

生物炭对含As(Ⅲ)水铁矿还原过程中砷形态及矿物转化的影响

生物炭的施用对土壤铁（氢）氧化物还原、砷（As）的形态转化有重要作用,极大地影响了As的环境行为.本文研究了生物炭/AQDS （蒽醌-2,6-二磺酸盐）对含As （Ⅲ）水铁矿化学还原和异化还原的影响,探索了由此产生的非生物和生物过程中Fe和As的形态转化及次生矿物的形成.结果表明,生物炭和AQDS的添加可以促进水铁矿的化学还原和As （Ⅲ）的化学氧化,AQDS促进水铁矿化学还原和As释放的能力强,生物炭促进As形态转化的能力强;生物组在添加Shewanella oneidensis MR-1后发现,生物炭和AQDS的添加可以促进Fe （Ⅱ）的生成,AQDS的添加促进Fe （Ⅱ）的生成、As形态转化和释放的能力要高于生物炭.EEM结果表明,生物炭产生的DOM可以与溶液中的物质发生氧化还原作用从而被消耗.循环伏安曲线在0.25 V处观察到一个小而宽的阳极峰（B）,可能对应了As （Ⅲ）氧化为As （V）.XRD结果显示AQDS处理的非生物组和生物组出现了蓝铁矿,表明AQDS可以促进次生矿物的生成.EDX-SEM结果表明,新矿物的生成有利于As的固定（BCF：0.73%相似文献   

基于SPOT5影像多辐射校正水平的植被绿量遥感估算

选用南京市SPOT5图像的灰度值(DN)、星上辐射率(SR)、表观反射率(TOA)和地物反射率(PAC)数据,提取了两种植被指数(VI),即归一化植被指数(NDVI)和比值植被指数(RVI),并与地面实测的绿量(LVV)进行相关分析,建立了165个关系模型.结果表明,LVV与VI呈极显著的相关关系,其相关系数多以相对均质植被高于植被总体,基于灰度值高于常用的地物反射率为主.LVV-VI关系模型的R~2均值以多元线性回归模型最高(0.821),指数模型最低(0.536),而1～3次多项式模型均接近0.7.每种植被样方优选出一个模型,即阔叶林LVV-7.802 RVI_(PAC)-2.455(R~2=0.827,RMSE=0.498);针阔叶混交林LVV=-15.421 RVI_(TOA)+26.971 RVI_(DN)-8.261(R~2=0.918,RMSE=0.356);灌木LVV=-342.591 NDVI_(DN)~3-20.553 NDVI_(DN)~2+14.013 NDVI_(DN)+1.509(R~2=0.764,RMSE=0.689);草地LVV=2.934 RVI_(PAC)+2.147 RVI_(TOA)-3.193(R2=0.903,RMSE=0.464);总体植被LVV=1.789RVI_(PAC)-6.814NDVIs+4.258NDVI_(PAC)+12.854 NDVI_(DN)-0.342(R~2=0.810,RMSE=0.638).这些优选模犁的自变量包括了4种辐射校正水平下提取的两种植被指数,显示基于不同辐射校正水平的植被指数在植被LVV遥感反演中具有一定的应用潜力.     

The coupling of sand with ZVI/oxidants achieved proportional and highly efficient removal of arsenic

• Simply doping sands with ZVI achieved an even activation of ZVI by oxidants. • Sand doping facilitated proportional As trapping along the ZVI/oxidants column. • ZVI/sand/oxidants are highly efficient for arsenic removal. • ZVI/sand/oxidants reduced significantly the Fe²⁺ leaching and effluent turbidity. • More than 54% of arsenic was reduced to As(III) in ZVI/sand/oxidants system. The coupling of zero-valent iron (ZVI) with common oxidants has recently achieved very rapid and highly efficient removal of Heavy metals from wastewater. However, the uniform activation of ZVI throughout the column and the proportional removal of target contaminants are urgently required for the prevention of premature filter clogging and the extension of the effective column operational time. In this study, we successfully achieved this objective by simply doping granular sand with ZVI at appropriate weight ratios. When pure ZVI packed column was spiked with oxidants, the majority of As trapping occurred between the column inlet and the first sampling point. In a packed column with a 1:20 mixture of ZVI and sand, the average As removal efficiency was 36 (1st), 13.1 (2nd), 18.5 (3rd), 19.2 (4th) and 5.9% (5th outlet). The overall arsenic removal performance of the composite filling system of ZVI/sand was equally as efficient as that of the previous pure ZVI-packed system. Moreover, the leaching of Fe was significantly reduced with an increased sand ratio, resulting in clearer water with less turbidity. The results of X-ray photoelectron spectroscopy (XPS) demonstrated that more than 54% of the arsenic was reduced to As(III). X-ray diffraction (XRD) and scanning electron microscopy (SEM) confirmed the extensive corrosion of the ZVI surface, which resulted in various species of iron oxyhydroxides responsible for the highly efficient sequester of arsenic through reduction, adsorption, and coprecipitation.     

西太平洋上空气溶胶的来源及其化学特征的研究

报道了西太平洋海域上空气溶胶的变化情况.尘土粒子的输入量控制着海洋上空气溶胶中元素Al、Fe、Sc、Mn、Co、La、Ce、Eu、Hf、Ta及Th的浓度.相对于海洋和地壳来源的异常富集元素在西太平洋上空气溶胶中富集程度很高.在开阔海域大气中的海盐元素浓度受海盐气溶胶粒子的量所控制,而其它元素则受来自陆地的地壳风化物影响.由于环境污染物的输入.使开阔海域大气的化学组成发生了变化.     

用荧光光谱研究腐殖酸与金属离子Al^3＋的配合作用

用同步荧光法对两种来源不同的腐殖酸与金属离子Ａｌ＾３＋的配合作用进行了研究,采用非线性回归分析,用荧光强度变化数据,拟合出金属配合物（１：１）的条件稳定常数Ｋ,在配合滴定进行的同时,探讨了溶液在５００ｎｍ处的瑞利散射现象。     

Cr(VI) uptake mechanism of Bacillus cereus

In this study, we investigated the Cr(VI) uptake mechanism in an indigenous Cr(VI)-tolerant bacterial strain -Bacillus cereus through batch and microscopic experiments. We found that both the cells and the supernatant collected from B. cereus cultivation could reduce Cr(VI). The valence state analysis revealed the complete transformation from Cr(VI) into Cr(III) by living B. cereus. Further X-ray absorption fine structure and Fourier transform infrared analyses showed that the reduced Cr(III) was coordinated with carboxyl and amido functional groups from either the cells or supernatant. Scanning electron microscopy and atomic force microscopy observation showed that noticeable Cr(III) precipitates were accumulated on bacterial surfaces. However, Cr(III) could also be detected in bacterial inner portions by using transmission electron microscopy thin section analysis coupled with energy dispersive X-ray spectroscopy. Through quantitative analysis of chromium distribution, we determined the binding ratio of Cr(III) in supernatant, cell debris and cytoplasm as 22%, 54% and 24%, respectively. Finally, we further discussed the role of bacterium-origin soluble organic molecules to the remediation of Cr(VI) pollutants.     

基于西门子S7 200 PLC的某反应釜压力安全监测与报警系统

实现化工反应装置的反应釜压力安全监测与报警,在现实化工生产中具有重要的意义。本文是基于西门子S7200PLC控制器,并且配备了触摸屏MT4300CE,以实现对4台化工反应釜的反应压力参数进行快速探测并进行预警。并就其安全预警系统的硬件组成和控制程序设计等方面都进行了较为详细的介绍。     

Digitalization and environment: how does ICT affect enterprise environmental performance?

Environmental Science and Pollution Research - Despite the increasing use of digital technology in industrial production, how industrial digitalization affects the environmental performance of...