ZrO_2空气焙烧与氮气焙烧对Au/ZrO_2水煤气变换催化剂性能的影响  

Preparation of Highly Active Au/ZrO_2 Catalysts for Water-Gas Shift Reaction:Calcination of ZrO_2 in Air vs. N_2

作　　者：张燕杰 陈崇启 詹瑛瑛[2] 林棋 娄本勇 郑国才 郑起[2] ZHANG Yanjie;CHEN Chongqi;ZHAN Yingying;LIN Qi;LOU Benyong;ZHENG Guocai;ZHENG Qi(Chemical Engineering and Materials Department of Ocean College, Minjiang University, Fuzhou, Fujian 350108, China;National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, China;Engineering Research Center of Green Dyeing and Finishing in Fujian Provincial University, Fuzhou, Fujian 350108, China)

机构地区：[1]闽江学院海洋学院化工与材料系,福建福州350108 [2]福州大学化肥催化剂国家工程研究中心,福建福州350002 [3]绿色染整福建省高校工程研究中心,福建福州350108

出　　处：《闽江学院学报》2018年第2期54-61,共8页Journal of Minjiang University

基　　金：国家自然科学基金(21503105);福建省自然科学基金(2017J05025;2017J01584);福建省教育厅JK类项目(JK2015038);福建省中青年教师教育科研项目(JA15419);福建省高校杰出青年科研人才培育计划(2016)

摘　　要：分别以空气和氮气焙烧的ZrO_2圆形纳米片(标记为ZrO_2-Air和ZrO_2-N_2)为载体,采用沉积-沉淀法制得1%Au/ZrO_2催化剂(标记为Au/ZrO_2-Air和Au/ZrO_2-N_2).考察了富氢气氛下上述催化剂的水煤气变换反应(WGSR)催化性能,发现Au/ZrO_2-Air的催化活性明显高于Au/ZrO_2-N_2,且显著优于Au负载量较高的Au/Fe_2O_3和Au/CeO_2催化剂.采用XRD、AAS、N_2物理吸脱附、TEM、UV-Vis DRS及EPR等手段研究了两种气氛焙烧的ZrO_2载体和相应Au/ZrO_2催化剂的结构及表面性质.结果表明,两种ZrO_2载体的晶相结构及织构性能无明显差异,但两种ZrO_2载体上表面缺陷种类和浓度分布差别较大.相较于ZrO_2-N_2,ZrO_2-Air的表面具有较多的配位不饱和Zr3+,这些位点有助于提高负载Au的分散度,使得Au/ZrO_2-Air具有较高的催化活性.The ZrO2 nanodisks were calcined in air and N2 atmosphere to obtain ZrO2-Air and ZrO2-N2,respectively. Then,the gold was deposited on different ZrO2 to produce 1% Au/ZrO2 catalysts（ denoted as Au/ZrO2-Air and Au/ZrO2-N2,respectively） by a deposition-precipitation method. The catalysts were evaluated in the water-gas shift reaction（ WGSR） under H2-rich reformate atmosphere.It is found that the Au/ZrO2-Air shows much higher catalytic activity than Au/ZrO2-N2. Importantly,the catalytic activity of Au/ZrO2-Air is also significantly higher than that of the previously reported Au/Fe2 O3 and Au/CeO2 catalysts. The structural and surface properties of ZrO2 calcined in air and N2 atmosphere were studied by XRD,AAS,N2-physisorption,TEM,UV-Vis DRS and EPR characterizations. The results show that the calcination atmosphere has a great influence on the type and concentration distribution of surface defects on ZrO2. The ZrO2-Air possesses more surface coordinatively unsaturated Zr3＋centers,which have strong interaction with supported Au species,resulting in an increased Au dispersion and a higher catalytic activity of Au/ZrO2-Air.

关 键 词：Au/ZrO2催化剂 水煤气变换反应 空气焙烧 氮气焙烧 配位不饱和Zr3+ Au分散度 

分 类 号：O643[理学—物理化学]