载银磁性Fe_3O_4纳米粒子的制备与催化及抗菌性能

利用磁性纳米粒子Fe_3O_4表面的聚多巴胺(PDA)对银离子的吸附作用,采用种子诱导法制备了载银磁性纳米粒子(PDA-Fe_3O_4@Ag)。采用UV-Vis(紫外-可见)光谱对PDA-Fe_3O_4@Ag纳米粒子的制备过程进行了分析,采用FTIR(红外光谱)、XRD(X射线衍射仪)、TEM(透射电镜)和VSM(振动样品磁强计)等手段对所得的PDA-Fe_3O_4@Ag粒子进行表征;研究了PDA-Fe_3O_4@Ag对4-硝基苯酚还原反应的催化作用,还测试了其抗菌性能。结果表明,纳米金种子的存在是制备PDA-Fe_3O_4@Ag纳米粒子的关键;在外加磁场作用下该磁性催化剂可以容易地从反应体系中分离,经多次循环使用后仍具有良好的催化性能;此外PDA-Fe_3O_4@Ag纳米粒子具有杀菌性能,且经磁分离回收循环利用5次后仍呈现对金黄色葡萄球菌较好的杀菌效果。     

碳纳米钯的生物合成及其催化性能研究

将奥奈达希瓦氏菌(S. oneidensis MR-1)原位还原形成的零价纳米钯颗粒负载在碳纳米管(CNTs)表面,制备了Pd/CNTs纳米复合材料。用TEM、XPS等多种手段对材料进行了表征,并用对硝基苯酚(4-NP)的还原降解反应评价了Pd/CNTs的催化性能。表征结果表明,钯纳米颗粒(直径2~3 nm)较均匀地分散在CNTs表面;钯负载在CNTs上会造成其拉曼峰强的增大和特征峰的偏移,且结晶度和颗粒数目随着负载量的增加而增加。性能评价表明,Pd/CNTs对4-NP还原降解具有较高催化性能,较其催化效率较单一的CNTs降解效率提高了6.3倍;在pH = 10的条件下,5% Pd/CNTs催化18 min可将4-NP降解99.5%,经6个反应循环后对4-NP的去除率仍保持在95.2%。     

AuCu双金属纳米颗粒的制备、表征及性能探究

采用水热法制备AuCu双金属纳米颗粒,并用X射线衍射(XRD)、透射电镜(TEM)和紫外可见光谱(UV-Vis)进行表征,初步研究了其对4-硝基苯酚(4-NP)还原的催化性能和光热效应。结果表明,制备时不同的AuCl_4~-/Cu~(2+)摩尔比(r_(Au))可以调控AuCu双金属纳米颗粒的组分和形貌,XRD和吸收光谱特征随r_(Au)的增加表现出更明显的金的特征,r_(Au)0.5时得到的颗粒具有典型的核-壳结构;核-壳结构的AuCu双金属纳米颗粒对4-NP还原表现出更好的催化活性,受光热效应影响,532 nm激光照射能够加强催化活性;在激光辐射作用下,不同AuCu双金属纳米颗粒具有相似的光热效应。     

溶剂热法合成花状Co_3O_4微球及其对高氯酸铵热分解的催化作用

以醋酸钴为原料,在甲醇体系中采用溶剂热法合成了由纳米片自组装而成的花状(CH_3O)_2Co前驱体微球。将前驱体焙烧后,得到了形貌保持良好的花状多孔Co_3O_4微球。利用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、热重(TG)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和N_2吸附-脱附等手段对样品的物相、化学组成、形貌及孔结构进行了表征。采用差示扫描量热(DSC)技术评价了Co_3O_4花状微球对高氯酸铵(AP)的热分解催化作用。结果表明,花状Co_3O_4微球对AP热分解过程具有良好的催化活性,添加2%(质量分数)的Co_3O_4可使AP的高温分解峰值温度降低122℃,表观分解热提高422 J/g。优异性能的发挥归因于其良好的分散性和丰富的级次孔结构。     

Co_3O_4/AuPt复合材料的制备及光降解亚甲基蓝的研究

采用一步水热合成法制备了具有二维尺寸的Co_3O_4材料,再通过绿色合成法引入NaBH_4还原H_2PtCl_6、HAuCl_4,得到Co_3O_4/AuPt复合纳米材料,用扫描电镜(SEM)、透射电镜(TEM)对其结构和性能进行了表征。采用紫外-可见分光光度法对复合材料的光催化性能进行了研究。结果表明,Co_3O_4/AuPt表现出最强的光催化性能,对于3.7μg亚甲基蓝(MB),当加入的催化剂达到200μg,降解时间为6min时,其降解率可达到100%;对于1000μg 2,4,6-三硝基甲苯(TNT),当加入的催化剂达到90.9μg,降解时间为10min时,其降解率可达到100%;对于55.6μg对硝基苯酚(4-NP),当加入的催化剂达到500μg,降解时间为7min时,其降解率可达到100%;由此表明,Co_3O_4/AuPt催化剂对亚甲基蓝等环境污染物质有较强的光催化降解能力。     

载银磁性Fe3O4纳米粒子的制备与催化及抗菌性能的研究

利用磁性纳米粒子Fe3O4表面的聚多巴胺 (PDA) 对银离子的吸附作用,采用种子诱导法制备了载银磁性纳米粒子 (PDA-Fe3O4@Ag)。采用UV-Vis (紫外-可见) 光谱对PDA-Fe3O4@Ag纳米粒子的制备过程进行了分析,采用FTIR (红外光谱)、XRD (X射线衍射仪)、TEM (透射电镜) 和VSM (振动样品磁强计) 等手段对所得的PDA-Fe3O4@Ag粒子进行表征;研究了PDA-Fe3O4@Ag对4-硝基苯酚还原反应的催化作用,还测试了其抗菌性能。结果表明,纳米金种子的存在是制备PDA-Fe3O4@Ag纳米粒子的关键;在外加磁场作用下该磁性催化剂可以容易地从反应体系中分离,经多次循环使用后仍具有良好的催化性能;此外PDA-Fe3O4@Ag纳米粒子具有杀菌性能,且经磁分离回收循环利用5次后仍呈现对金黄色葡萄球菌较好的杀菌效果。     

无模板法合成大孔Co_3O_4及其储锂性能（英文）

介绍了一种通过快速分解/燃烧反应结合后续空气气氛中热处理制备大孔Co_3O_4的简便方法。采用X-射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、拉曼光谱、元素分析、压汞法、N2吸附脱附测试等技术详细研究了大孔Co_3O_4产物。结果表明,所制备的大孔Co_3O_4粉体具有“蠕虫状”的网络结构,主要暴露晶面为(111)面;粉末比表面积约为2 m2/g,大孔尺寸分布范围为50~350 nm,峰值孔径为120 nm。由于其大孔结构和(111)主暴露晶面,大孔Co_3O_4作为锂离子电池负极时表现出优异的电化学性能。     

Fe3O4@SiO2@mTiO2-Au复合材料的制备及其催化性能研究

以磁性Fe3O4为核,在其表面负载SiO2,并用介孔TiO2 (mTiO2)进行包覆,用3-氨丙基三甲氧基硅烷对其改性,将纳米金颗粒均匀负载在介孔TiO2表面,制备出核壳型纳米Fe3O4@SiO2 @mTiO2 -Au复合材料。用透射电镜(TEM)、振动样品磁强计(VSM)、X射线光电子能谱分析(XPS)和X射线衍射分析(XRD)等对样品进行表征,确认了核壳结构的存在,尺寸约3 nm的纳米金负载在表面。催化活性测试结果表明,该材料对对硝基苯酚在25 min内降解率达83%,对铁氰酸钾在30 min内降解率达84%。     

非晶态NiB纳米催化剂的制备及其对对硝基苯酚加氢的催化活性

对共还原法合成的NiZnB粉体进行NaOH刻蚀后脱锌而制得非晶态NiB纳米催化剂(NiB-etch),考察其对对硝基苯酚(4-NP)加氢的催化活性。通过透射电子显微镜、X射线衍射、氮气吸/脱附等温曲线、电感耦合等离子发射光谱进行材料表征,利用紫外-可见分光光度计定量分析4-NP催化加氢速率。结果表明:与常规NiB催化剂相比,NiB-etch的比表面积增加2.3倍,催化反应速率常数提高2.5倍。另外,对NiZnB进行150℃下热处理,可使NiB-etch催化活性进一步提高1.7倍,反应速率常数增至0.93 min~(-1)。     

锂离子电池复合正极材料LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2/C的制备及性能研究（英文）

通过共沉淀法合成了层状LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2正极材料,并用柠檬酸包覆在LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2/C表面制备出一系列的LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2/C复合材料。利用扫描电镜(SEM),透射电镜(TEM),X射线衍射(XRD)对未包覆样品和复合材料进行表征,采用恒流充放电和交流阻抗技术对其电化学性能进行测试。XRD分析结果表明,碳包覆没有改变LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2/C的晶形结构;C包覆量为5%(质量分数)的LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2样品展现出优良的电化学性能,在2.8~4.6V电压范围内,0.1C倍率充放电条件下,其首次放电比容量为174.2mAh·g-1,远高于未包覆样品的156.7mAh·g-1。     

Catalytic performance and kinetics of Au/γ-Al_2O_3 catalysts for low-temperature combustion of light alcohols

Au/γ-Al2O3 catalysts were prepared by deposition-precipitation method for the catalytic combustion of low concentration alcohol streams(methanol,ethanol,iso-propanol and n-propanol).The catalysts were characterized by X-ray photoelectron spectroscopy(XPS),X-ray diffractometry(XRD) and energy dispersive X-ray micro analysis(EDS) techniques.The XPS results showed that there was only Au0 on the surface of catalysts.The XRD patterns showed that Au was presumably highly dispersed over γ-Al2O3.The temperatures for complete conversion of methanol,ethanol,iso-propanol and n-propanol with concentration of 2.0 g/m3 were 60,155,170 and 137 ℃,respectively,but they were completely mineralized into CO2 and H2O at 60,220,260 and 217 ℃ respectively over the optimized catalyst.The activity of the catalyst was stable in 130 h.The kinetics for the catalytic methanol elimination followed quasi-first order reaction expressed as r=0.652 8c0+0.084 2.The value of apparent activation energy is 54.7 kJ/mol in the range of reaction temperature.     

RuPt双金属在催化加氢反应中的性能研究

采用溶剂热法制备了5%Pt/C、5%Ru/C和5%Ru95Pt5/C三种催化剂。对催化剂的形貌和活性组分分布进行了表征分析,分别研究了不同催化剂在苯乙炔或4-硝基酚加氢反应中的催化性能。结果表明,由于协同效应,双金属负载的催化剂5%Ru95Pt5/C比单金属催化剂具有更好的催化加氢性能。在苯乙炔加氢反应中,5%Ru95Pt5/C具有更高的选择性和优异的活性;在4-硝基酚的加氢中,5%Ru95Pt5/C的催化活性显著增加,且在循环5次后,仍保留了>99%的活性。     

Gold complexes with

The reactions of methane with the gold complexes [Au(OH)]⁻, [Au(OCH₃)₄]⁻, [Au(O(CO)₂O₂]⁻ and [Au(O₂CH)₂]⁺, [Au^I(acac)], [Au^III(acac)₂]⁺ (acac-acetylacetonato) were studied using the DFT/PBE method with the SBK basis set. High activation barriers were obtained for the electrophilic substitution in [Au(OH)]⁻, [Au(OCH₃)⁴]⁻, [Au(O(CO)₂O)₂]-and [Au^III(acac)₂]⁺ complexes, which excludes the possibility that these reactions might proceed under mild conditions. The reactions of the [Au(HCO₂)₂]⁺ and [AuI(acac)] complexes with methane have rather low energy barriers and proceed through the formation of an intermediate complex. The alternative mechanism of methane oxidation with a gold complex in the presence of oxygen is simulated.     

Support effects in the selective gas phase hydrogenation ofp-chloronitrobenzene over gold

The catalytic continuous gas phase hydrogenation of p-chloronitrobenzene (P=1 atm;T=423 K) has been investigated over a series of oxide (Al₂O₃, TiO₂, Fe₂O₃ and CeO₂) supported Au (1 mol %) catalysts. The application of two catalyst synthesis routes,i.e. impregnation (IMP) and deposition-precipitation (DP), has been considered where the DP route generated smaller mean Au particle sizes (1.5-2.8 nm) compared with the IMP preparation (3.5-9.0 nm). The catalysts have been characterised in terms H2 chemisorption and BET area measurements where the formation of metallic Au post-activation has been verified by diffuse reflectance UV-Vis, XRD and HRTEM analyses.p-Chloroaniline was generated as the sole reaction product over all the Au catalysts with no evidence of C-Cl and/or C-NO₂ bond scission and/or aromatic ring reduction. The specific hydrogenation rate increased with decreasing Au particle size (from 9 to 3 nm), regardless of the nature of the support. This response extends to a reference Au/TiO₂ catalyst provided by the World Gold Council. A decrease in specific rate is in evidence for smaller particles (< 2 nm) and can be attributed to a quantum size effect. The results presented establish the basis for the design and development of a versatile catalytic system for the clean continuous production of high value amino compounds under mild reaction conditions.     

Solid-phase extraction of trace Au(III) with SDG and determination by the catalytic spectrophotometric method

The new catalytic kinetic spectrophotometric method for Au(III) determination was developed and validated. It was based on the catalytic effect of gold on the oxidation of sudan red III by ammonium peroxodisulfate ((NH₄)₂S₂O₈) with nitrilo triacetic acid as an activator in microemulsion and H₂SO₄ medium. Under optimum conditions, there was the linearity of the calibration curve in the concentration range from 0 to 20 μg/L Au(III) at 520 nm. The relative standard deviation was 3.0% with a correlation coefficient of 0.9986. The detection limit achieved was 9.75 × 10⁻⁵ μg/mL. A new method using a column packed with sulfhydryl dextrose gel (SDG) as a solid-phase extractant has been developed for the preconcentration and separation of Au(III) ions. The method has been applied to the determination of trace gold with satisfactory results.     

Pdx-Co/C催化甲酸的电氧化性能研究

以活性碳(Vulcan XC-72)为载体,用化学还原法制备了不同Pd/Co摩尔比的Pdx-Co/C催化剂。用透射电镜(TEM)、X射线衍射(XRD)及X射线光电子能谱(XPS)对催化剂进行了表征,采用循环伏安法考察了催化剂对甲酸电氧化反应的催化性能。结果表明,Pdx-Co复合催化剂粒子均匀分散在碳载体表面;催化剂中掺入的少量Co元素部分进入Pd晶格,形成了Pd-Co合金;随着Pd/Co摩尔比的增加,Pd颗粒粒径先增大后减小,催化活性也表现出相同的变化趋势;当Pd:Co=8:1时,所得Pd8-Co/C对甲酸氧化的催化活性最高,峰电流密度可达到15.907 mA/cm²。     

Synthesis and antimicrobial activities of gold(I) sulfanylcarboxylates

Reaction of NaAuCl₄·H₂O and thiodiglycol (1:3 molar ratio) with 3-(aryl)-2-sulfanylpropenoic acids, H₂ xspa = [x:p = 3-phenyl-, f = 3-(2-furyl)-, t = 3-(2-thienyl)-, o-py = 3-(2-pyridyl)-, Clp = 3-(2-chlorophenyl)-, -o-mp = 3-(2-methoxyphenyl)-, -p-mp = 3-(4-methoxyphenyl)-, -o-hp = 3-(2-hydroxyphenyl)-, -p-hp = 3-(4-hydroxyphenyl)-, diBr-o-hp = 3-(3,5-dibromo-2-hydroxyphenyl)] and 2-cyclopentylidene-2-sulfanylacetic acid (H₂cpa) in a 1:1 metal/ligand molar ratio gave compounds of the type [Au(Hxspa)] or [Au(Hcpa)]. These compounds were reacted with diisopropylamine to afford [HQ][Au(xspa)] or [HQ][Au(cpa)] (HQ = diisopropylammonium) and with NaOH to afford Na[Au(xspa)]·H₂O and Na[Au(cpa)]·H₂O. All of the new compounds were isolated and characterised by IR and ¹H and ¹³C NMR spectroscopy. The antimicrobial activities of the complexes against Escherichia coli, Staphylococcus aureus, Bacillus subtilis, Candida albicans, Pseudomonas aeruginosa and carbapenem-resistant P. aeruginosa were evaluated and compared to those of the equivalent silver(I) complexes. The comparison shows that the gold compounds generally show better activity than the silver analogues against S. aureus and B. subtilis, but low sensitivity against E. coli, P. aeruginosa and C. albicans, suggesting a different mode of antimicrobial action for equivalent silver and gold compounds.     

Deposition of Pd on Co(OH)2 nanoplates in stabilizer-free aqueous phase for catalytic reduction of 4-nitrophenol

Palladium-supported cobalt hydroxide (Co(OH)₂-Pd) nanoplates were fabricated in an aqueous solution and employed as a catalyst for the reduction of 4-nitrophenol. For the preparation of Co(OH)₂-Pd, Pd nanoparticles were anchored on the Co(OH)₂ nanoplates after the reduction of Na₂PdCl₄ by ascorbic acid in the absence of a stabilizer at room temperature. The observations under transmission and scanning electron microscopy reveal that Pd nanoparticles with a size of 2–5 nm are uniformly dispersed on the surface of the Co(OH)₂ nanoplates. In catalytic test, the conversion of 4-nitrophenol to 4-aminophenol is completed within 6 min in the presence of Co(OH)₂-Pd(1000) nanoplates with 2.18 at.% Pd, and the corresponding kinetic constant is 0.0089 s^-1 in the first test. The catalyst retains relatively high activity after several cycles. The results demonstrate that the Co(OH)₂-Pd(1000) nanoplates exhibit high catalytic activity toward the reduction of 4-nitrophenol in the presence of NaBH₄.     

Preparation of new sunscreen materials Ce1-xZnxO2-x via solid-state reaction at room temperature and study on their properties

Superfine cerium-zinc oxides Ce1-xZnxO2-x with x = 0, 0.1, 0.3, 0.5, and 1.0 were obtained by grinding Ce(SO4)2·4H2O, ZnSO4·7H2O and NH4HCO3 under the condition of surfactant PEG-400 being present at room temperature, washing the mixture with water to remove soluble inorganic salts, drying at 80°C, and calcining.The precursor and its calcined samples were characterized using thermogravimetry and differential thermal analyses(TG/DTA), UV-vis absorption spectroscopy, X-ray powder diffraction(XRD), and scanning electron microscopy(SEM).The results showed that superfine Ce1-xZnxO2-x behaved as an excellent UV-shielding material.The ZnO-doped CeO2 can facilitate the formation of crystalline state CeO2.The catalytic ability of products used in air oxidation of castor oil was investigated.The results showed that the catalytic abilities of products decreased with increasing zinc amount.