Differences in nitrous oxide fluxes from red soil under different land uses in mid-subtropical China

Red soil may play an important role in nitrous oxide (N₂O) emissions due to its recent land use change pattern. To predict the land use change effect on N₂O emissions, we examined the relationship between soil N₂O flux and environmental determinants in four different types of land uses in subtropical red soil. During two years of study (January 2005-January 2007), biweekly N₂O fluxes were measured from 09:00 to 11:00 a.m. using static closed chamber method. Objectives were to estimate the seasonal and annual N₂O flux differences from land use change and, reveal the controlling factors of soil N₂O emission by studying the relationship of dissolved organic carbon (DOC), microbial biomass carbon (MBC), water filled pore space (WFPS) and soil temperature with soil N₂O flux. Nitrous oxide fluxes were significantly higher in hot-humid season than in the cool-dry season. Significant differences in soil N₂O fluxes were observed among four land uses; 2.9, 1.9 and 1.7 times increased N₂O emissions were observed after conventional land use conversion from woodland to paddy, orchard and upland, respectively. The mean annual budgets of N₂O emission were 0.71-2.21 kg N₂O-N ha⁻¹ year⁻¹ from four land use types. The differences were partly attributed to increased fertilizer use in agriculture land uses. In all land uses, N₂O fluxes were positively related to soil temperature and DOC accounting for 22-48% and 30-46% of the seasonal N₂O flux variability, respectively. Nitrous oxide fluxes did significantly correlate with WFPS in orchard and upland only. Nitrous oxide fluxes responded positively to MBC in all land use types except orchard which had the lowest WFPS. We conclude that (1) land use conversion from woodland to agriculture land uses leads to increased soil N₂O fluxes, partly due increased fertilizer use, and (2) irrespective of land use, soil N₂O fluxes are under environmental controls, the main variables being soil temperature and DOC, both of which control the supply of nitrification and denitrification substrates.     

Shellac-coated iron oxide nanoparticles for removal of cadmium(II) ions from aqueous solution

This study describes a new effective adsorbent for cadmium removal from aqueous solution synthesized by coating a shellac layer, a natural biodegradable and renewable resin with abundant hydroxyl and carboxylic groups, on the surface of iron oxide magnetic nanoparticles. Transmission Electron Microscopy (TEM) imaging showed shellac-coated magnetic nanoparticle (SCMN) adsorbents had a core-shell structure with a core of 20 nm and shell of 5 nm. Fourier Transform Infrared Spectroscopic analysis suggested the occurrence of reaction between carboxyl groups on the SCMN adsorbent surface and cadmium ions in aqueous solution. Kinetic data were well described by pseudo second-order model and adsorption isotherms were fitted with both Langmuir and Freundlich models with maximum adsorption capacity of 18.80 mg/g. SCMN adsorbents provided a favorable adsorption capacity under high salinity conditions, and cadmium could easily be desorbed using mild organic acid solutions at low concentration.     

氢氧化钽对水体中磷酸盐的吸附去除作用

采用氢氧化钽为吸附剂,对水中磷酸盐的吸附性能进行了研究,考察了吸附时间、pH值、磷酸盐的初始浓度、反应温度对吸附量的影响。实验结果表明:pH值越小,氢氧化钽对磷酸盐的吸附量越大,当pH值为2时氢氧化钽对磷酸盐的吸附性能优,并且pH值对磷酸盐的吸附量影响较大;磷酸盐的初始浓度越大,吸附量越大,吸附平衡时间越短;氢氧化钽对磷酸盐的吸附量和吸附速率都随着温度的升高而增加。在25℃、pH=2、初始浓度为200 mg/L、吸附30 min时达到平衡时最大吸附量为76.69 mg/g。吸附后的氢氧化钽红外谱图在1066 cm-1处出现特征峰,该峰恰好是吸附磷酸盐的伸缩振动峰,并且在638 cm-1与670 cm-1之间Ta-O键由于磷酸盐的吸附发生了蓝移。采用6 mol/L的NaOH对吸附了磷酸盐的氢氧化钽进行解吸,当pH=12时解吸率为52.45%。研究结果表明,氢氧化钽能够有效的去除水溶液中磷酸盐的吸附剂。     

长江上游典型农业源溪流溶存氧化亚氮(N2O)浓度特征及影响因素

随着农业非点源氮（N）污染的加剧,农田周边溪流成为重要的活性N汇和潜在的氧化亚氮（N₂O）排放源.为查明长江上游农业源溪流中溶存N₂O浓度的全年动态变化特征,于2014年12月~2015年10月开展紫色土丘陵区典型农田源头溪流N₂O浓度的连续采样观测,采用水-气顶空平衡-气相色谱法测定顶空气体中N₂O浓度,根据相关参数计算出本研究水体中的溶存N₂O浓度,并同步测定溪流水体物理化学指标,分析水中溶存N₂O浓度的主要影响因素.结果表明,长江上游紫色土丘陵区的典型农业源溪流的硝态氮（NO₃^--N）是最主要的活性N赋存形态（年均1.45 mg·L^-1）,溪流水体溶存N₂O质量浓度（以N计）全年平均为0.57 μg·L^-1（范围0.26~1.28 μg·L^-1）,冬、春、夏和秋季的均值分别为0.63、0.45、0.53和0.64 μg·L^-1,但季节间无显著差异.溪流水体溶存N₂O浓度全年都处于过度饱和状态（饱和度年平均为203.9%,范围109.7%~546.5%）,可见,农业源溪流全年均为潜在的N₂O释放源.溪流溶存N₂O浓度的变化主要由水体NO₃^--N浓度决定,N₂O的主要产生机制为反硝化作用;溪流季节平均N₂O饱和度在夏、秋季显著高于冬、春季,水中溶存N₂O饱和度的变化主要受水温和NO₃^--N浓度的共同影响.研究还发现农业源溪流中溶存N₂O浓度在4~10月（湿润季节）间波动明显,较强降雨可促使其水中NO₃^--N浓度在雨后短期内升高,进而促进水体反硝化作用,导致雨后溪流中溶存N₂O浓度的增加.     

羟胺强化过渡金属活化过硫酸盐降解磺胺甲恶唑

以典型磺胺类抗生素—磺胺甲恶唑(SMZ)为降解对象,选取赤铁矿(α-Fe_2O_3)、氧化钴(Co_2O_3)和氧化铜(CuO)3种过渡金属氧化物(M_xO_y),研究了羟胺(HA)对3种过渡金属氧化物活化过硫酸盐(PDS)降解SMZ的强化效果及机理.结果表明,HA对M_xO_y/PDS体系降解SMZ具有明显的促进作用,初始HA、PDS、M_xO_y和SMZ浓度均对SMZ的降解具有重要影响.电子顺磁共振(EPR)实验结果证实,α-Fe_2O_3/HA/PDS和Co_2O_3/HA/PDS体系中的主要活性自由基是·OH,而CuO/HA/PDS体系中SMZ的降解并不依赖于自由基的生成,表面活化态PDS是降解SMZ的主要活性物种.此外,采用高效液相色谱-离子阱质谱联用仪(HPLC-ESI-MS)检测了SMZ在Co_2O_3/HA/PDS体系中的降解产物.结果表明,SMZ主要通过3条路径进行降解矿化,分别为氨基官能团的硝基化、不饱和碳碳双键的羟基加成及磺胺键的断裂.     

活性炭的表面性质对CeOx/AC催化臭氧氧化水中苯甲酸的影响机制

实验对活性炭(activated carbon,AC)进行了氧改性、氮改性、硫改性和氮-硫共改性,考查AC的表面性质对CeO_x/AC催化臭氧氧化苯甲酸性能的影响.结果表明,相比氧改性活性炭ACO、硫改性活性炭ACS和氮改性活性炭ACN,氮-硫共改性活性炭ACNS由于含氮官能团和含硫官能团的引入,提高了对苯甲酸的吸附性能和催化臭氧氧化性能.采用氮-硫共改性活性炭为载体制备的CeO_x/ACNS催化剂表面Ce~(3+)含量最高,因而具有最高的催化活性,反应30 min,苯甲酸的去除率由单独臭氧氧化的22%提高到88%,TOC的去除率单独臭氧氧化的7%提高到55%.CeO_x/ACNS催化剂具有良好的稳定性,循环使用6次,苯甲酸的去除率仅从88%降低到82%,整个过程中活性组分Ce的流失只占负载量的0.32%,是一种很有应用潜力的臭氧氧化催化剂.     

两种不同形态MnO2降解卡马西平的效果及途径对比

研究了两种不同形态MnO₂（δ-MnO₂和胶体MnO₂）对难降解有机药物卡马西平（carbamazepine,CBZ）的去除效果,并通过液相色谱质谱联用技术（LC/MS）分析了不同pH值条件下δ-MnO₂和胶体MnO₂氧化转化CBZ的产物,探究其氧化转化途径.结果表明,δ-MnO₂和胶体MnO₂能通过化学氧化作用在2h内去除约1mg/L CBZ,相比之下,胶体MnO₂受pH影响较小且单位质量Mn对CBZ具有更好的去除效果.δ-MnO₂和胶体MnO₂与CBZ反应过程中各检出7种和4种产物.胶体MnO₂具有更强的氧化能力,越过了多种中间产物的产生步骤,使CBZ的降解途径更加简明.     

氧化石墨烯对淡水微藻生长及生物活性物质的影响

为掌握氧化石墨烯（GO）的水环境风险,以斜生栅藻（Scenedesmus obliquus）和湖泊微拟球藻（Nannochloropsis limnetica）为研究对象,探究了GO对淡水微藻生长及其生物活性物质（碳水化合物、总蛋白质、总脂）的影响.结果表明,GO对2种微藻具有中等毒性,72h EC₅₀值分别为25.63和48.44mg/L.透射电镜（TEM）观察发现,GO纳米片层既能附着于藻细胞表面也能进入藻细胞内部,造成藻细胞超微结构明显变化,包括：质壁分离;叶绿体收缩;淀粉粒数量减少甚至消失.较低浓度（10mg/L）GO会促进微藻中光合色素（叶绿素a、叶绿素b、类胡萝卜素）合成;而较高浓度（100mg/L）GO暴露下,2种微藻的类胡萝卜素和斜生栅藻叶绿素a的含量显著降低.2种浓度的GO总体上刺激了藻细胞内生物活性物质的合成,这是污染胁迫下的一种主动防御机制;而较高浓度GO造成碳水化合物含量显著降低,可能原因是细胞中储能物质由淀粉向中性脂转化.     

溶解性微生物产物在GO/PVDF杂化膜面的污染行为

为了解析溶解性微生物产物（SMP）在GO/PVDF杂化膜面的污染特性,对膜片进行了宏观污染实验,并采用耗散石英微晶天平（QCM-D）从微观角度分析了SMP在自制镀膜芯片上的吸附规律和污染层结构变化.结果表明,GO含量为0.5wt%的膜污染恢复率最高（79.95%）,抗污染能力最强.QCM-D实验发现,GO含量为0wt%镀膜芯片表面SMP吸附量最大,污染较为严重.膜片亲水性越强,吸附频率变化越小,抗污染能力越强.此外,GO含量为0.5wt%镀膜芯片表面的污染物结构比较疏松和柔软,其他膜表面的污染物结构较为坚硬和致密.