Pd/GO/Ni电极的制备及对2,4-二氯酚的降解研究

为去除持久性氯代有机污染物2,4-二氯酚(2,4-DCP),利用电化学沉积法制备了一种新型钯/氧化石墨烯/泡沫镍(Pd/GO/Ni)电极,并通过电化学法降解2,4-二氯酚,取得良好的效果。通过扫描电镜等表征手段观察其表面形貌。结果表明:氧化石墨烯浓度为10 mol/L是制备Pd/GO/Ni电极的最佳浓度,p H为3时,Pd/GO/Ni电极对2,4-二氯酚的去除率达到90.7%。     

Reuse of nickel recovered from spent Ni–Cd batteries for the preparation of C/Ni and C/Ni/Pd layered electrodes for energy sources

Nickel recovered in the recycling process of Ni–Cd batteries was used as a main component of bath for electrodeposition of nickel onto carbon fabric in order to obtain C/Ni composite. A part of the obtained composite was additionally coated with a thin layer of palladium (C/Ni/Pd composite). All the materials were investigated to assess the possibility of their use in the processes of electrochemical storage (sorption/desorption) of hydrogen and electrochemical oxidation of methanol. The obtained results showed the composites to be active electrode materials in these processes. The electrodes exhibited high activity and cyclability, especially in the process of methanol oxidation due to electrocatalytic activity of both nickel deposited onto carbon fabric and the outer layer of porous palladium coating nickel substrate.     

Pd/MCM-41催化水溶液中碘苯Ullmann反应的研究

以水溶剂中Ullmann反应为目标反应,设计具有纳米介孔结构的Pd/MCM-41作为其高效催化剂.与传统SiO2载体负载的Pd催化剂比较,该催化剂在以水为介质的碘苯偶合（Ullmann反应）中显示出优良的催化活性和对联苯的选择性.     

Fe3O4稳定化纳米Pd/Fe对水中2,4-D的催化还原脱氯研究

采用四氧化三铁(Fe3O4)稳定化纳米Pd/Fe催化脱氯水溶液中的2,4-二氯苯氧乙酸(2,4-D),获得了良好的处理效果.实验考察了Fe3O4投加量、pH、钯化率、温度、搅拌速率等因素对2,4-D去除的影响.2,4-D去除率随Fe3O4投加量增加而提高,投加量为4.0 g·L-1时,反应210 min后,2,4-D去除率为93.5%,而未稳定的纳米Pd/Fe,去除率为47.3%.低pH可促进2,4-D还原脱氯,pH为2.6~4.1时,2,4-D在110 min内几乎完全去除.2,4-D去除率随钯化率增加而提高.随着钯化率由0.25%、0.50%增加到0.75%,210 min后,2,4-D的去除率也由51.4%、93.5%提高到99.9%.温度在16.5~30.0℃范围内,反应210 min后,2,4-D去除率均可超过90.0%.温度升高到35.0、40.0℃时,去除率显著下降.2,4-D去除率随着搅拌速率加快而提高.Fe3O4的加入可以使纳米Pd/Fe分散和稳定.此外,Fe0可通过Fe3O4将电子传递给H+和2,4-D,促进2,4-D的还原脱氯.     

纳米级Pd/Fe-MWCNTs-Fe3O4体系对2,3-DCB的降解研究

为有效抑制纳米级Pd/Fe颗粒的团聚和钝化及改善磁分离效果,以多壁碳纳米管(MWCNTs)和磁性纳米级Fe_3O_4颗粒为载体,在超声波辐照下利用液相还原法制备纳米级Pd/Fe-MWCNTs-Fe_3O_4颗粒,并采用XRD、TEM、SEM、EDX及BET表征其物性,最后以2,3-二氯联苯(2,3-DCB)为目标污染物,探究其对2,3-DCB还原脱氯的影响因素、降解机理和动力学.结果表明:制备的纳米级颗粒粒径均匀、分散性好、比表面积大;体系中纳米级Pd/Fe投加量、钯化率、纳米级Fe_3O_4投加量、MWCNTs投加量、反应温度、溶液初始pH及共存阴离子均会对2,3-DCB的降解效果产生明显影响;本研究推测出纳米级Pd/Fe-MWCNTs-Fe_3O_4体系对2,3-DCB的降解机理,发现其降解符合拟一级动力学关系.     

Electrochemical dechlorination of chloroform in neutral aqueous solution on palladium/foam-nickel and palladium/polymeric pyrrole film/foam-nickel electrodes

Electrochemical dechlorination of chloroform in neutral aqueous solution was investigated using palladium-loaded electrodes at ambient temperature. Palladium/foam-nickel （Pd/foam-Ni） and palladium/polymeric pyrrole film/foam-nickel （Pd/PPy/foam-Ni） composite electrodes which provided catalytic surface for reductive dechlorination of chloroform in aqueous solution were prepared using an electrodepositing method. Scanning electron microscope （SEM） micrographs showed that polymeric pyrrole film modified the electrode-surface characteristics and resulted in the uniform dispersion of needle-shaped palladium particles on foam-Ni supporting electrode. The experimental results of dechlorination indicated that the removal efficiency of chloroform and current efficiency in neutral aqueous solution on Pd/PPy/foam-Ni electrode could be up to 36.8% and 33.0% at dechlorination current of 0.1 mA and dechlorination time of 180 min, which is much higher than that of Pd/foam-Ni electrode.     

Dechlorination of disinfection by-product monochloroacetic acid in drinking water by nanoscale palladized iron bimetallic particle

Nanoscale palladized iron(Pd/Fe)bimetallic particles were prepared by reductive deposition method.The particles were characterized by X-ray diffraction(XRD),X-ray fluorescence(XRF),scanning electron microscope(SEM),transmission electron microscope(TEM),and Brunauer-Emmett-Teller-nitrogen(BET-N_2)method.Data obtained from those methods indicated that nanoscale Pd/Fe bimetallic particles containedα-Fe~0.Detected Pd to Fe ratio by weight(Pd/Fe ratio)was close to theoretical value. Spherical granules with di...     

Distribution of Platinum group elements in road dust in the Beijing metropolitan area, China

Dust samples collected from the Beijing metropolitan area （China） were evaluated to determine the distribution and the concentration of platinum group elements （PGEs）. The dust particles that were smaller than 100 mesh size fraction （150 μm） were analyzed after aqua regia digestion. Concentrations ofPt, Rh, and Pd were found to be between 3.96 and 356.3 ng/g, 2.76 and 97.11 ng/g, and 0.1 and 124.9 ng/g, respectively, in the urban areas of Beijing, whereas for the background samples collected from the suburbs of Beijing, the concentrations of Pt, Pd, and Rh were very low and ranged from 0.1 to 0.9 ng/g, 0.5 to 1.4 ng/g, and 0.8 to 2.2 rig/g, respectively. The distributions of PGEs in road dust were an accurate reflection of the levels of pollution and were found to match with the local traffic conditions. A strong positive correlation was established among all the dements found in road dust. This suggests that emissions of abraded fragments from vehicle exhausts may be the source of the high concentration of Pt, Rh, and Pd in road dust along the main roads of Beijing.     

干旱区气候条件对道路灰尘及土壤 Pd、Rh累积的影响

以乌鲁木齐市为研究区,选取河滩路、友好南路、温泉西路、乌奎高速公路及七道湾路等5条典型道路,对道路灰尘与土壤中Pd、Rh季节变化特征进行研究.结果表明,春、夏、秋、冬的灰尘中Pd含量分别为74.61(31.59~126.3),134.26(54.59~332.51),100.49(20.935~244.9), 83.43(47.97~125.40)ng/g;灰尘中Rh含量分别为8.41(4.56~14.63),18.48(11.62~31.56),10.27(3.83~19.1),9.20(5.34~16.68)ng/g;土壤中Pd含量分别为44.42(13.59~109.40),30.47(13.24~70.87),30.01(21.55~49.19),26.28(14.85~44.83)ng/g;土壤Rh含量分别为8.47(5.93~13.40), 8.11(4.65~ 13.45),3.81(1.67~8.02),3.22(2.56~4.26)ng/g. Pd、Rh含量均表现出明显的季节变化,其中,灰尘中Pd、Rh含量在夏秋季高,冬春季低;土壤中Pd、Rh含量在春夏季高,冬季最低,秋季为中间水平,地域气候条件是PGEs季节变化的主要影响因素.冬、春季节的降雪、扫雪及积雪堆积习惯使乌鲁木齐道路环境中灰尘与土壤的季节变化并没有完全相同. 湿润区与干旱区城市PGEs的季节变化明显不同,两类地区的气候特征不同是造成这种差异存在的根本原因.     

Pd/CeO2催化水中溴酸盐的加氢还原研究

采用溶胶-凝胶法制备了CeO2载体,以浸渍法和沉积沉淀法制备了负载型催化剂Pd/CeO2.使用透射电镜(TEM)和Zeta电位仪对催化剂进行了表征.结果表明两种材料的等电点都在5.0左右; Pd颗粒在载体表面具有良好的分散性,且Pd负载量越高,Pd颗粒的粒径越大.采用Pd/CeO2催化剂催化溴酸盐加氢还原,发现在溴酸盐初始浓度为0.39mmol/L时,采用沉积沉淀法和浸渍法合成的Pd/CeO2催化剂反应50min后对溴酸盐的去除率分别为100%和71%,表明使用沉积沉淀法合成的催化剂具有较高的催化活性.改变催化剂用量,溴酸盐的催化还原速率不受传质阻力的影响,反应过程符合Langmuir–Hinshelwood模型,即催化还原反应由溴酸盐在催化剂表面的吸附控制.增加Pd的负载量,溴酸盐的还原速率增大.溶液pH值较低时,有利于对溴酸盐的催化还原.