Through converting the surface complex on TiO2 nanorods to generate superoxide and singlet oxygen to remove CN-

Cyanide(CN^-) is extensively used in the process of plating devices and for surface treatment in the electroplating industry and is extremely hazardous to humans and the environment. Peroxymonosulfate(PMS)- based advanced oxidation processes(AOPs) hold considerable promise for CN^- removal. However, the activity of sulfate radical and hydroxyl radical generated in the PMS activation process is low in the base condition, leading to a drop in its efficiency in CN^- re...     

Efficient nitrogen doped porous carbonaceous CO2 adsorbents based on lotus leaf

In this work, the waste biomass lotus leaf was converted into N-doped porous carbonaceous CO₂ adsorbents. The synthesis process includes carbonization of lotus leaf, melamine post-treatment and KOH activation. For the resultant sorbents, high nitrogen content can be contained due to the melamine modification and advanced porous structure were formed by KOH etching. These samples were carefully characterized by different techniques and their CO₂ adsorption properties were investigated in detail. These sorbents hold good CO₂ adsorption abilities, up to 3.87 and 5.89 mmol/g at 25 and 0°C under 1 bar, respectively. By thorough investigation, the combined interplay of N content and narrow microporous volume was found to be responsible for the CO₂ uptake for this series of sorbents. Together with the high CO₂ adsorption abilities, these carbons also display excellent reversibility, high CO₂/N₂ selectivity, applicable heat of adsorption, fast CO₂ adsorption kinetics and good dynamic CO₂ adsorption capacity. This study reveals a universal method of obtaining N-doped porous carbonaceous sorbents from leaves. The low cost of raw materials accompanied by easy synthesis procedure disclose the enormous potential of leaves-based carbons in CO₂ capture as well as many other applications.     

腐殖酸定向修饰Ce-Co铁基生物焦汞吸附机理

使用腐殖酸对铁基改性生物焦进行定向修饰,并借助固定床吸附装置考察改性后生物焦汞吸附性能,探究了不同腐殖酸负载量下的铁基改性生物焦的汞吸附能力.采用BET、XPS、FTIR表征手段,考察了定向修饰后生物焦的孔隙结构、表面元素价态及表面功能基团的组成,通过SEM扫描电镜探究生物焦微观形貌,并利用EDS能谱分析生物焦表面活性金属成分分布.结果表明,使用腐殖酸对铁基改性生物焦定向修饰后的生物焦汞脱除性能大幅提高,使用5%质量分数包裹后的生物焦汞脱除性能最高,3h单位累积汞吸附量为18025ng/g,相较于未被修饰的铁基改性生物焦汞吸附性能提高65%;负载腐殖酸后的生物焦以介孔为主,表面活性金属种类丰富,有利于单质汞的氧化;样品表面羧基、醇羟基等含氧官能团数量增加,定向修饰后生物焦表面出现大量氨基等利于重金属吸附的含氮官能团;定向修饰后的生物焦表面出现团聚现象,包裹量过高会将生物焦表面活性位点完全包裹,阻碍了氧化还原反应的进行,不利于汞的进一步氧化;汞在生物焦表面的吸附过程同时存在化学吸附与物理吸附.     

Fe (II)活化过硫酸盐处理喹啉工艺参数优化及生物毒性

以喹啉为处理目标物,采用Fe²⁺活化K₂S₂O₈（PS）的高级氧化体系在不同环境因素下降解喹啉.结果表明：与单一PS体系和Fe²⁺体系相比,Fe²⁺/PS体系可以有效降解喹啉.在初始喹啉浓度为250mg/L,喹啉/PS物质的量比为1：10,PS/Fe²⁺物质的量比为3,初始pH3,反应温度为45℃,反应时间为80min的条件下,喹啉降解率可达100%.提高PS和Fe²⁺浓度均能有效提高喹啉降解率,但超过一定限值后对喹啉去除效果不明显.Fe²⁺/PS去除喹啉的过程符合一级反应动力学.溶液初始pH值越高,喹啉去除率越低;反应温度越高,喹啉去除率越高.自由基淬灭实验证实,Fe²⁺活化PS体系中有SO₄^-·和OH·的存在,其中由SO₄^-·产生的OH·对喹啉的降解占主导地位.通过GC/MS检测到2种中间产物8-羟基喹啉和2（1H）-喹啉酮,据此推测基于硫酸根自由基强化喹啉降解的可能路径.大肠杆菌急性毒性实验结果证实,虽然Fe²⁺/PS体系去除喹啉过程中产生了毒性更强的中间产物,但酸性条件和较高的反应温度有利于体系脱毒.     

热活化过硫酸盐联合混凝处理微乳浊液的机理

在冶金冷轧微乳浊液中,醚链较长、αH较多的非离子型表面活性剂的存在导致体系稳定性极高而难于降解,利用热活化过硫酸盐（PS）进行破乳预处理,并联合混凝作用,以实现高效的油水分离.本文研究了PS浓度、体系温度、pH值对上述反应的影响,根据电子顺磁共振等分析技术确定了作用自由基类型及其贡献率,利用气相色谱-质谱联用法分析了反应前后微乳浊液成分,根据激光粒度法测定了反应过程油滴粒径,结果表明：增大PS浓度和温度、降低pH值均有利于提高COD去除率;降解过程包括SO₄^-.、OH^.破乳及聚合硫酸铁促使强疏水性油滴脱稳,且SO₄^-.为破乳主导自由基（贡献率86.33%）;基于联合工艺的COD去除率和运行成本均优于热活化PS单一工艺.     

基于性能参数退化的发动机推进剂加速退化试验建模

目的 针对某火箭弹发动机推进剂加速退化试验数据,建立性能参数退化模型,分别基于最大伸长率和最大抗拉强度等不同参数,计算推进剂的激活能和不同温度下的加速因子。方法 建立基于退化轨迹的性能参数退化模型,对发动机推进剂进行加速退化试验建模,利用最小二乘法计算性能变化参数,利用阿伦尼斯模型计算加速模型的参数,并得到激活能和加速因子。结果 针对推进剂加速试验数据,给出推进剂激活能和不同温度下加速因子的计算方法。采用基于退化轨迹的性能参数退化模型,可有效评估推进剂的寿命。结论 该方法可有效地对推进剂加速试验数据进行建模,给出激活能和加速因子,更能反映推进剂的寿命特征,为寿命评估提供支撑。     

A novel graphene oxide-carbon nanotubes anchored α-FeOOH hybrid activated persulfate system for enhanced degradation of Orange II

Persulfate activation has been applied as one of the efficient advanced oxidation processes(AOPs) to remediate polluted environments. In this study, a novel α-FeOOH anchored by graphene oxide(GO)-carbon nanotubes(CNTs) aerogel(α-FeOOH@GCA) nanocomposite activated persulfate system(α-FeOOH@GCA + K_2S_2O_8) was applied for decolorization of Orange Ⅱ(OⅡ). The decolorization of OⅡ was remarkably enhanced to a level of ～ 99% in this system compared with that of pristine α-FeOOH(～ 44%) or GO-CNTs(～18%). The enhanced catalytic activity of α-FeOOH@GCA was due to the formation of a heterojunction byα-FeOOH and GO-CNTs as confirmed by the presence of Fe–O–C chemical bonds. The degradation intermediates of OⅡ were comprehensively identified. The proposed degradation pathway of OⅡ begins with the destruction of the conjugated structures of OⅡ by the dominant reactive oxygen species, surface-bound SO_4~(·-). The decolorization efficiency of OⅡ by the α-FeOOH@GCA activated persulfate system decreased from the first to third cycle of recycling. Ultraviolet(UV) irradiation or introduction of a small amount of Fe~(2+) could restore the activation of this system. The results show that the α-FeOOH@GCA persulfate activation system promises to be a highly efficient environmental remediation method for organic pollutants.     

温度对海洋厌氧氨氧化菌脱氮效能的影响

采用ASBR反应器,研究了不同温度对海洋厌氧氨氧化菌处理含海水污水脱氮效能的影响,并利用修正的Logistic模型模拟不同温度下海洋厌氧氨氧化菌的动力学特性.结果表明,在25~35℃之间,温度对反应器的脱氮效能影响不大,总氮去除率(TNRE)基本保持在(82±2)%,总氮容积负荷去除速率(TNRR)稳定在(0.62±0.01)kg·(m~3·d)~(-1);在20℃时,TNRE从起始的59%经过13d上升到79%,说明在此温度下,海洋厌氧氨氧化菌仍然具有较强的脱氮能力,反应器在较低温处理含海水污水具有较好的发挥潜能;然而当温度降到15℃和10℃时,反应器的脱氮效能受到明显的抑制,TNRE分别下降至(40±8)%和(11±4)%,TNRR也下降至(0.30±0.04)kg·(m~3·d)~(-1)和(0.08±0.03)kg·(m~3·d)~(-1).根据Arrhenius方程得到,在25~35℃时,海洋厌氧氨氧化反应的活化能为26 k J·mol~(-1),在10~25℃时,海洋厌氧氨氧化反应的活化能为76 k J·mol~(-1).此外,通过Logistic模型对海洋厌氧氨氧化脱氮进行动力学分析,得到不同温度下NRE和出水总氮浓度(ceff)的预测公式,相关系数R2在0.966 8~0.995 7之间.     

应用铁铜双金属有机骨架活化过硫酸盐催化剂去除水中有机污染物的研究

基于MIL-101(Fe)的合成方法,首次采用合成前金属掺杂法制备了双金属有机骨架MIL-101(Fe,Cu)催化剂,并利用X射线衍射仪(XRD)、傅里叶变换红外光谱仪(FTIR)、扫描电镜(SEM)和X射线能谱仪(EDS)对催化剂进行表征.同时,以罗丹明B(Rh B)为目标降解物,研究此催化剂催化过硫酸盐降解Rh B的性能,并初步尝试将催化剂应用于邻苯二甲酸二丁酯(DBP)的催化降解.XRD、FTIR、SEM和EDS等分析结果表明,铜离子的掺杂导致MIL-101(Fe)的结构与形貌发生了改变,提高了对污染物的吸附和催化降解作用.相比MIL-101(Fe),在90 min时MIL-101(Fe,Cu)对Rh B的去除率达到95%,在180 min时对DBP的去除率达到68%.此外,分析了催化剂催化性能提高的原因:配位竞争导致铁离子的不饱和趋向;形貌的变化加强了对污染物的吸附作用.     

紫外光强化Fe(Ⅱ)-EDTA活化过硫酸盐降解直接耐酸大红4BS

为探索硫酸根自由基对偶氮染料的降解能力,以直接耐酸大红4BS（下称大红4BS）为模拟污染物,通过UV/Fe（Ⅱ）-EDTA/PDS（PDS为过硫酸钠）体系,探讨了初始c（PDS）、Fe（Ⅱ）/EDTA（摩尔比）、无机盐阴离子等对大红4BS降解的影响.结果表明,大红4BS的脱色率随着初始c（PDS）的增加而增大,当c（PDS）超过15 mmol/L时无显著变化.Fe（Ⅱ）/EDTA比在5:1时效果最好,5 min时使0.038 0 mmol/L大红4BS的脱色率达到93.6%.反应符合二级动力学模型.HCO₃-、Cl-、NO₃-、SO₄2-等无机盐阴离子表现出明显抑制作用,c（无机盐阴离子）在100 mmol/L条件下,脱色率分别降低66.9%、13.2%、12.1%、9.43%.利用紫外可见光谱,依据其结构与特征吸收的关系,初步推测自由基离子对大红4BS降解的途径:苯环最先遭到破坏,随后偶氮键断裂、萘环开裂.研究显示,UV光可有效强化Fe（Ⅱ）-EDTA活化过硫酸盐形成SO₄-·自由基,对偶氮染料具有很好的脱色能力,最佳反应条件[PDS:Fe（Ⅱ）:EDTA（摩尔比）为15:5:1]下,大红4BS在10 min时脱色率高达98.1%.