杀菌功能载银活性炭的NaBH_4还原法制备及其表征

通过NaBH4还原法制备了银缓释杀菌功能载银活性炭(Ag/AC),研究了其对大肠杆菌(E.coil)的杀灭性能和抗银流失性能.以低温液氮吸附测定活性炭的比表面积,以扫描电子显微镜(SEM)-X射线能谱仪(EDS)分析Ag/AC表面形态以及Ag的含量和分布,以X射线衍射(XRD)观察Ag/AC晶体结构.结果表明,银以单质形式负载在活性炭上.活性炭的载银量、比表面积、银颗粒的粒径及分布取决于AgNO3溶液浓度.在不同AgNO3溶液浓度条件下,银的晶核形成和生长机制发生改变.随着AgNO3溶液浓度的增加,所制备Ag/AC表现出由无活性、抑菌到杀菌活性的变化规律.载银量为2.70%(质量分数)时,Ag/AC能在90 min内杀灭2×106 CFU/mL浓度的大肠杆菌,且在水中振荡600 h的银流失量为21.1%.在保持较高杀菌活性前提下,可以实现银的缓释.     

活性炭性质对其吸附水中硝基苯性能的影响

通过对活性炭进行HNO3氧化及热处理改性,研究了活性炭性质对其吸附硝基苯性能的影响.以低温液氮(N2/77 K)吸附测定活性炭的比表面积和孔容、孔径分布;以Boehm滴定、零电荷点pHPZC的测定及元素分析定量表征活性发表面含氧官能团变化.结果表明:经改性后,活性炭比表面积及总孔容略有减小,表面性质发生较大变化.改性活性炭对硝基苯的吸附容量明显改变,吸附容量大小依次为:AC1′＞AC0′＞AC0＞AC1.经硝酸氧化后,比表面积下降、存在过多表面含氧官能团是导致AC1吸附硝基苯能力降低的主要原因;而AC1'表面适量酚羟基所提供的氢键吸附是其对硝基苯吸附量增加的主要原因.     

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.     

载银活性炭活化过硫酸钠降解酸性橙

采用硝酸氧化的颗粒活性炭浸渍制备Ag/GAC活化剂,利用N2吸附、SEM、FT-IR及XRD对Ag/GAC进行表征,得出Ag成功负载于颗粒活性炭上,并以Ag/GAC在常温常压下活化过硫酸钠(PS)产生硫酸根自由基(SO-4·)降解偶氮染料酸性橙7(AO7).考察了Ag负载量、PS浓度、Ag/GAC投加量、初始p H对AO7降解效果的影响.结果表明,当Ag负载量为12.7mg·g-1、n(PS)∶n(AO7)为120∶1、Ag/GAC投加量为1.0 g·L-1,降解180 min后AO7降解率达95.0%以上.初始p H对Ag/GAC活化PS降解AO7有较大影响,p H为5.0时降解效果最优.通过紫外可见光谱、气相色谱-质谱(GC/MS)对AO7降解过程进行了探讨,在降解过程中AO7的偶氮键和萘环结构均被破坏,并检测出主要降解产物有邻苯二甲酸和乙酰苯.     

载钴活性炭强化电芬顿处理亚甲基蓝废水研究

文章以啤酒酵母为原料制备了载钴活性炭（Co/AC）和活性炭（AC,对照材料）,用于强化电芬顿处理亚甲基蓝（MB）废水,对体系中存在的吸附和催化降解耦合作用进行了研究。独立吸附反应中,Co/AC对MB的吸附动力学过程和等温吸附过程分别符合准二级动力学模型和Langmuir方程,其理论饱和吸附容量为232.48 mg/g,低于AC(399.79 mg/g)。电芬顿反应中,Co/AC催化对MB和TOC去除率分别为99.05%、88.57%,高于AC催化的95.95%、68.87%,以及硫酸亚铁催化的35.53%、32.37%。Co/AC优异的催化降解MB性能主要源于其具有更强的促进·OH生成的能力。Co/AC对MB的吸附和催化降解耦合作用过程符合构建的Langmuir-first-order动力学方程。     

易挥发有毒化合物催化燃烧试验

在富氧条件下以2.0% Ru/Al₂O₃和2.0% Ru/AC(AC为活性炭)为催化剂,在固定床反应装置上研究了甲醇、氨、甲苯的催化氧化活性及反应动力学. 结果表明,Ru/Al₂O₃对3种反应物的催化活性比Ru/AC高,3种反应物的反应活性顺序为甲醇>氨>甲苯,其去除率随反应物浓度的增加呈先增大后减小的趋势. 反应的活化能(Ea)测定结果为甲醇<氨<甲苯. 比表面积检测(BET)和透射电镜(TEM)结果显示,Ru/Al₂O₃与Ru/AC的孔体积(0.54 mL/g)近似相等,而其孔径分别为9.3和2.3 nm;在大孔径的氧化铝上Ru以极细的粒径(<3 nm)形成高度分散体系,在活性炭上Ru则以较大颗粒(4～10 nm)位于活性炭表面,Ru的粒径细化及形成高分散体系可能是Ru/Al₂O₃的催化活性高于Ru/AC的主要原因.      

Pt在燃料电池中的催化性能研究

以硝酸铁为催化剂,棉花为碳源,H2 Ar气氛下高温催化裂解制得的活性炭(active carbon,AC),经过BET测得其比表面积为650 m2/g,在SEM下观察具有多孔、多通道.以这种自行制备的活性炭为载体在恒电位下沉积Pt粒子得到的Pt/AC/GC电极对甲醇电催化氧化具有很好的性能.在相同条件下活性炭为载体的Pt/AC/GC电极是VulcanXC-72(比表面积为520 m2/g)负载的Pt/XC/GC电极电流密度的1.5倍.用恒电位法测试得到Pt/AC/GC电极具有较好的稳定性.     

MOx颗粒活性炭镀层粒子电极对苯酚的电催化降解特性

为研究半导体金属氧化物颗粒活性炭镀层粒子电极苯酚电催化性能,采用溶胶-凝胶、氧化还原与热分解方法,将TiO₂、MnO₂与SnO₂-Sb和SnO₂-Sb-Mn纳米金属氧化物镀层于AC(颗粒活性炭)表面,制备了催化型粒子电极,使用X-射线衍射(XRD)、扫描电镜(SEM)及循环伏安曲线(CV)对其物相组成、微观形貌及电催化活性进行表征与分析. 结果表明,这4类金属氧化物可以不同赋存状态存在于AC表面,粒子电极表面活性组分晶格尺寸分别为10.64、11.34、14.68及13.50 nm;催化型粒子电极电催化活性明显高于未负载AC,各粒子电极电催化活性顺序为SnO₂-Sb-Mn/AC>TiO₂/AC>SnO₂-Sb/AC>MnO₂/AC. 半导体金属氧化物镀层可提高填充床电极反应器苯酚废水的催化降解性能,废水苯酚及COD_Cr去除率显著提升,TiO₂/AC、MnO₂/AC、SnO₂-Sb/AC及SnO₂-Sb-Mn/AC粒子电极在电流密度为8.0 mA/cm2的条件下连续电解2.72 h,出水苯酚及COD_Cr去除率分别为87.1%、92.8%、90.4%、100.0%和92.5%、89.3%、88.7%、97.2%,高于AC粒子电极的84.2%和79.1%,并且可消除苯酚电催化反应中醌类物质积累.      

锰银复合催化剂对NTP降解吸附态甲苯的影响

采用等体积浸渍法制备以13X分子筛为载体的Mn-Ag复合型催化剂,并用SEM、BET和FT-IR手段对催化剂进行表征。在介质阻挡放电反应器(DBD)中,考察了锰、银不同摩尔比和不同负载总量的催化剂对吸附态甲苯降解的影响。结果表明:当n(Mn)∶n(Ag)为1∶3时,Mn-Ag/13X催化剂对甲苯催化氧化活性最高,CO_2选择性为98.84%;不同摩尔比的催化剂对O_3分解性能顺序与对甲苯的催化氧化性能顺序一致,其顺序为n(Mn)∶n(Ag)1∶3>1∶5>1∶1>3∶1>5∶1>0∶0;Mn-Ag/13X(Mn∶Ag=1∶3)催化剂锰和银负载量对催化剂的吸附性能和催化活性有显著影响,随负载量的变化,吸附穿透时间大小关系为:2.5%Mn-Ag/13X≈7.5%Mn-Ag/13X>5%Mn-Ag/13X>10%Mn-Ag/13X;负载量为5%时,吸附穿透时间为125 min,CO_x浓度为4 669.82 mg/m~3,显示出最好的催化活性。     

纳米硒化银的生物合成及其对染料的吸附去除

利用菌株Pantoea sp.IMH实现了硒化银纳米颗粒的生物合成,同时,结合高分辨透射电镜(HRTEM)、能谱成像(EDX-mapping)、X射线粉末衍射(XRD)等多种表征手段对硒化银纳米颗粒进行了表征分析.结果表明,所合成的硒化银纳米颗粒的粒径为10~20 nm,其纳米颗粒的晶面间距为0.225 nm,对应于Ag2Se的(031)晶面.所合成的纳米颗粒的衍射环对应的标准Ag2Se晶面为(013)、(031)和(113)面.XRD结果表明,纳米颗粒的晶面为(111)、(112)和(004)晶面,说明菌株IMH能够合成纳米硒化银晶体.通过以不同电性的染料分子亚甲基蓝(阳性)、日落黄(阴性)、靛蓝(中性)作为目标分子进行吸附去除应用探索,发现硒化银纳米颗粒对阳性和中性染料分子有良好的吸附去除效果.这是由于硒化银纳米颗粒表面带有负电荷(Zeta电位分别为-11.8 m V(p H=5)、-13.0 m V(p H=7)、-13.0 m V(p H=9)).本研究为硒化银纳米颗粒的生物合成提供了新思路,拓展了硒化银纳米颗粒的合成方法.     

Impact of density of coating agent on antibacterial activity of silver nanoparticle impregnated plasma treated activated carbon

To use stabilized nanoparticles(NPs) in water as disinfectants over a very long period, the amount of coating agent(for NP stabilization) needs to be optimized. To this end, silver nanoparticles(Ag-NPs) with two different coating densities of tri-sodium citrate(12.05 and46.17 molecules/nm~2, respectively), yet of very similar particle size(29 and 27 nm, respectively)were synthesized. Both sets of citrate capped NPs were then separately impregnated on plasma treated activated carbon(AC), with similar Ag loading of 0.8 and 0.82 wt.%, respectively. On passing contaminated water(containing 10~4 CFU Escherichia coli/m L of water) through a continuous flow-column packed with Ag/AC, zero cell concentration was achieved in 22 and 39 min, with Ag-NPs(impregnated on AC, named as Ag/AC) having lower and higher coating density, respectively. Therefore, even on ensuring similar Ag-NP size and loading, there is a significant difference in antibacterial performance based on citrate coating density in Ag/AC.This is observed in lower coating density case, due to both:(i) higher Ag~+ ion release from Ag-NP and(ii) stronger binding of individual Ag-NPs on AC. The latter ensures that, Ag-NP does not detach from the AC surface for a long duration. TGA-DSC shows that Ag-NPs with a low coating density bind to AC with 4.55 times higher adsorption energy, compared to Ag/AC with a high coating density, implying stronger binding. Therefore, coating density is an important parameter for achieving higher antibacterial efficacy, translating into a faster decontamination rate in experiments, over a long period of flow-column operation.     

Comparative toxicity of silver nanoparticles and silver ions to Escherichia coli

With the increase in silver(Ag)-based products in our lives, it is essential to test the potential toxicity of silver nanoparticles(Ag NPs) and silver ions(Ag ions) on living organisms under various conditions. Here, we investigated the toxicity of Ag NPs with Ag ions to Escherichia coli K-12 strain under various conditions. We observed that both Ag NPs and Ag ions display antibacterial activities, and that Ag ions had higher toxicity to E. coli K-12 strain than Ag NPs under the same concentrations. To understand the toxicity of Ag NPs at a cellular level, reactive oxygen species(ROS) enzymes were detected for use as antioxidant enzymatic biomarkers. We have also studied the toxicity of Ag NPs and Ag ions under various coexistence conditions including: fixed total concentration, with a varied the ratio of Ag NPs to Ag ions; fixed the Ag NPs concentration and then increased the Ag ions concentration; fixed Ag ions concentration and then increasing the Ag NPs concentration.Exposure to Ag NPs and Ag ions clearly had synergistic toxicity; however, decreased toxicity(for a fixed Ag NPs concentration of 5 mg/L, after increasing the Ag ions concentration) to E. coli K-12 strain. Ag NPs and Ag ions in the presence of L-cysteine accelerated the bacterial cell growth rate, thereby reducing the bioavailability of Ag ions released from Ag NPs under the single and coexistence conditions. Further works are needed to consider this potential for Ag NPs and Ag ions toxicity across a range of environmental conditions.Environmental Significance Statement: As silver nanoparticles(Ag NPs)-based products are being broadly used in commercial industries, an ecotoxicological understanding of the Ag NPs being released into the environment should be further considered. Here, we investigate the comparative toxicity of Ag NPs and silver ions(Ag ions) to Escherichia coli K-12 strain, a representative ecotoxicological bioreporter. This study showed that toxicities of Ag NPs and Ag ions to E. coli K-12 strain display different relationships when existing individually or when coexisting, and in the presence of L-cysteine materials. These findings suggest that the toxicology research of nanomaterials should consider conditions when NPs coexist with and without their bioavailable ions.     

载银活性碳纤维对大肠杆菌吸附作用的研究

以大肠杆菌（Ｅｓｃｈｅｒｉｃｈｉａｃｏｌｉ）为对象，通过细菌吸附实验研究了载银活性碳纤维（ＡＣＦ（Ａｇ））对大肠杆菌的吸附特性．借助扫描电子显微镜（ＳＥＭ）进行细菌分布形态的观察和细菌数量的计算．结果表明，大肠杆菌易分布于ＡＣＦ（Ａｇ）表面的沟槽处；ＡＣＦ（Ａｇ）吸附的细菌数量随银含量、比表面积的增加而增大．此外，细菌吸附量还与ＡＣＦ（Ａｇ）表面银颗粒的大小有关．对吸附细菌的动力学亦进行了研究．     

野外便携净水器净水消毒工艺试验研究

野外便携净水器应具杀菌消毒效率高、净水时间短、使用寿命长、操作方便等功能使用要求。通过试验考察了三碘树脂和载银活性炭两种不同净水消毒工艺流程对原水处理效果。结果表明：三碘树脂材料比载银活性炭材料具有灭菌效果好、反应接触时间短、使用时间长等优势，是一类具有良好军事应用价值的野外便携净水器的净水消毒材料。     

安徽铜陵鸡冠石银(金)矿床地质地球化学特征

鸡冠石银 (金 )矿床是铜陵地区一个具中型规模的银 (金 )矿床 ,在整个长江中、下游地区都有其代表性。矿床分四个主要成矿阶段 :夕卡岩阶段、氧化物 -硫化物阶段、石英 -硫化物阶段和石英多金属硫化物-碳酸盐阶段。对矿床的微量元素分析结果表明 ,独立的银、金矿物和含Au、Ag低的硫化物、含Ag硫盐矿物 ,主要形成于热液成矿期中晚阶段 ;矿床的轻、重稀土元素总浓度比值与辉石二长闪长岩相近 ,反映出二者的同源特征 ;稳定同位素和流体包裹体成分分析结果 ,反映出该矿床以岩浆热液为主的成因标志 ;成矿热液以岩浆水为主 ,但在成矿晚期有大气降水和地层成分加入 ;成矿流体为NaCl-KCl -H2 O体系 ;矿床成因属夕卡岩 -中低温热液充填 -交代型矿床     

Rapid degradation of hexachlorobenzene by micron Ag/Fe bimetal particles

The feasibility of the rapid degradation of hexachlorobenzene (HCB) by micron-size silver (Ag)/iron (Fe) particles was investigated.Ag/Fe particles with different ratios (0,0.05%,0.09%,0.20%,and 0.45%) were prepared by electroless silver plating on 300 mesh Fe powder,and were used to degrade HCB at different pH values and temperatures.The dechlorination ability of Fe greatly increased with small Ag addition,whereas too much added Ag would cover the Fe surface and reduce the effective reaction surface,thereby decreasing the extent of dechlorination.The optimal Ag/Fe ratio was 0.09%.Tafel polarization curves showed that HCB was rapidly degraded at neutral or acidic pH,whereas low pH levels severely intensified H2 production,which consumed the reducing electrons needed for the HCB degradation.HCB degradation was more sensitive to temperature than pH.The rate constant of HCB dechlorination was 0.452 min-1 at 85℃,50 times higher than that at 31℃.HCB was degraded in a successive dechlorination pathway,yielding the main products 1,2,4,5-tetrachlorobenzene and 1,2,4-trichlorobenzene within 2 hr.     

Comparative study of leaching of silver nanoparticles from fabric and effective effluent treatment

Nano silver (Ag_n) is employed as an active antimicrobial agent, but the environmental impact of Ag_n released from commercial products is unknown. The quantity of nanomaterial released from consumer products during use should be determined to assess the environmental risks of advancement of nanotechnology. This work investigated the amount of silver released from three different types of fabric into water during washing. Three different types of fabric were loaded with chemically synthesized Ag nanoparticles and washed repeatedly under simulated washing conditions. Variable leaching rates among fabric types suggest that the manufacturing process may control the release of silver reaching the waste water treatment plants. In an attempt to recover the Ag_n for reutilization and to save it from polluting water, the effluents from the wash were efficiently treated with bacterial strains. This treatment was based on biosorption and was very efficient for the elimination of silver nanoparticles in the wash water. The process ensured the recovery of the Ag_n leached into the effluent for reutilization, thus preventing environmental repercussions.     

载银活性炭活化过硫酸钠降解酸性橙7

采用硝酸氧化的颗粒活性炭浸渍制备Ag/GAC活化剂,利用N₂吸附、 SEM、 FT-IR及XRD对Ag/GAC进行表征,得出Ag成功负载于颗粒活性炭上,并以Ag/GAC在常温常压下活化过硫酸钠(PS)产生硫酸根自由基(SO^－4 ·)降解偶氮染料酸性橙7(AO7). 考察了Ag负载量、 PS浓度、 Ag/GAC投加量、 初始pH对AO7降解效果的影响. 结果表明,当Ag负载量为12.7 mg ·g^-1、 n(PS) :n(AO7)为120 :1、 Ag/GAC投加量为1.0 g ·L^-1,降解180 min后AO7降解率达95.0%以上. 初始pH对Ag/GAC活化PS降解AO7有较大影响,pH为5.0时降解效果最优. 通过紫外可见光谱、 气相色谱-质谱(GC/MS)对AO7降解过程进行了探讨,在降解过程中AO7的偶氮键和萘环结构均被破坏,并检测出主要降解产物有邻苯二甲酸和乙酰苯.     

以保护地下水为目标的Ag土壤环境基准推导案例

土壤环境基准是制订土壤环境质量标准的重要依据. 借鉴国外制订保护地下水的土壤环境基准方法学,以湖南红壤、北京潮土和东北黑土为供试土壤,通过吸附试验获取重金属Ag在3种土壤中的分配系数(K_d),并通过文献调研获取3种土壤及其含水层的相关参数;采用US EPA(美国国家环境保护局)的土壤环境基准技术导则中的SSL(soil screening level)模型,并基于我国饮用水水质标准,对Ag土壤环境基准进行反推. 结果显示:Ag在红壤、黑土和潮土中的分配系数分别为7.10、56.7、132 L/kg,推导出的基于保护地下水的Ag的土壤环境基准值分别为0.440、3.04和7.80 mg/kg. 3种土壤中Ag的基准值均在发达国家或地区保护地下水的土壤环境基准值范围内,与各国基准值的差异主要是由于土壤性质、含水层类型以及Ag在土壤中的分配系数的差异所致.