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Y2O3负载金属Cu在催化甲醛水溶液制氢反应中的Y2O3载体效应
Effect of Y2O3 Supporter on the Catalytic Hydrogen Production from an Aqueous Formaldehyde Solution Catalyzed by Metal Cu Loaded on Y2O3
【摘要】 采用NaBH4还原法将纳米金属Cu负载在Y2O3上.通过X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)和测定氢氧根在Y2O3和Cu上的吸附等手段对样品进行了表征.结果表明,Y2O3表面存在一层薄的Y(OH)3,能优先吸附OH-使其在Y2O3表面"富集";金属Cu以纳米粒子形式负载在Y2O3上.在碱性甲醛溶液中考察了Y2O3负载Cu(Cu/Y2O3)的催化性能.结果表明,在低碱度条件下,相对于未负载纳米Cu的Y2O3,Cu/Y2O3具有较高的产氢活性.当氢氧化钠浓度为0.050 mol/L时,在氮气气氛下Cu/Y2O3产氢量约为未负载纳米Cu的7.8倍;而在空气气氛下约为4.3倍.在2种气氛下,Cu/Y2O3产氢的最佳氢氧化钠浓度均为0.25 mol/L.这可归结为Y2O3表面对OH-的"富集"效应,使其表面产生更多的活性物种CH2(OH)O-(甲二醇负离子).相对于未负载纳米Cu的Y2O3,Y2O3负载Cu提高了催化剂的稳定性,其原因是Y2O3负载阻止了Cu粒子在反应过程的生长.
【Abstract】 Nano metal Cu was loaded on Y2O3 by NaBH4 reduction method. The sample was characterized by X-ray diffraction( XRD),X-ray photoelectron spectroscopy( XPS),transmission electron microscopy( TEM)and adsorption measurement of OH-on Y2O3 and Cu. The results show that there is a thin layer of Y( OH)3on the surface of Y2O3,which can preferentially adsorb OH-,that is,"enrichment"of OH-on Y2O3; metal Cu was loaded on Y2O3 in the form of nano particles. The performance of Cu supported on Y2O3( Cu/Y2O3)catalyst was investigated in alkaline formaldehyde solution. The results show that under low alkalinity,Cu/Y2O3 exhibits higher activity for hydrogen production than unloaded nano metal Cu. When the concentration of Na OH is 0. 050 mol/L,the hydrogen amount produced over Cu/Y2O3 is 7. 8 times as high as that over nano Cu under N2 atmosphere,whereas the former is 4. 3 times as high as the latter under air atmosphere. The optimal Na OH concentration for hydrogen production over Cu/Y2O3 is 0. 25 mol/L under both atmospheres. The results can be attributed to "enrichment"effect of OH-on Y2O3,leading to production of the higher concentration of active CH2( OH) O-( formaldehyde anion) species on Y2O3. The stability of Cu/Y2O3 is improved compared with that of unloaded nano Cu. The reason is that the load of Cu on Y2O3 prevents growth of Cu particles during the reaction.
【Key words】 Formaldehyde; Hydrogen production; Load of Cu; Y2O3; Enrichment of OH-;
- 【文献出处】 高等学校化学学报 ,Chemical Journal of Chinese Universities , 编辑部邮箱 ,2017年10期
- 【分类号】O643.36;TQ116.2
- 【被引频次】8
- 【下载频次】214