Au@ZrO_2空心纳米微球的制备及其催化性质
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摘要
以Stober法合成了不同粒径的SiO_2微球。以这些SiO_2微球为硬模板,通过ZrOCl_2前驱体吸附和水解制备得到了ZrO_2@SiO_2复合物,然后用HF溶解去除二氧化硅模板剂,制备得到ZrO_2空心球。以ZrO_2空心球为载体,采用沉积-沉淀法(DP)合成了Au@ZrO_2纳米空心微球。考察了Au@ZrO_2纳米空心微球在对硝基苯胺还原反应中的催化性能。研究结果表明,所合成的SiO_2微球粒径大小均一、形状规则、分散性好;ZrO_2空心微球大小及比表面积可以通过硬模板SiO_2微球粒径进行有效控制;与Au@ZrO_2实心微球相比,Au@ZrO_2空心微球在对硝基苯胺还原反应中表现出良好的催化性能,当反应温度为45℃、反应7 min时,对硝基苯胺能够完全转化为对苯二胺。
SiO_2 microspheres with different diameters were prepared by Stober method, and the SiO_2 microspheres were uniformly coated with ZrO_2 by adsorption and hydrolysis of Zr OCl2. The ZrO_2 hollow microspheres were then obtained after SiO_2 was removed by hydrofluoric acid, and Au@ZrO_2 hollow microspheres were finally prepared by deposition-precipitation(DP) method. Catalytic properties of Au@ZrO_2 hollow microspheres in reduction of paranitroaniline were studied carefully. The research results indicate that the SiO_2 microspheres have regular shape and good dispersity. The sizes and the surface areas of the ZrO_2 hollow microspheres could be controlled effectively by the diameters of SiO_2 microspheres. Compared to the solid microsphere Au@ZrO_2, the Au@ZrO_2 hollow microspheres showed good catalytic performance in reduction of p-nitroaniline, and p-nitroaniline was completely reduced to pphenylenediamine in 7 min at 45 ℃.
SiO_2 microspheres with different diameters were prepared by Stober method, and the SiO_2 microspheres were uniformly coated with ZrO_2 by adsorption and hydrolysis of Zr OCl2. The ZrO_2 hollow microspheres were then obtained after SiO_2 was removed by hydrofluoric acid, and Au@ZrO_2 hollow microspheres were finally prepared by deposition-precipitation(DP) method. Catalytic properties of Au@ZrO_2 hollow microspheres in reduction of paranitroaniline were studied carefully. The research results indicate that the SiO_2 microspheres have regular shape and good dispersity. The sizes and the surface areas of the ZrO_2 hollow microspheres could be controlled effectively by the diameters of SiO_2 microspheres. Compared to the solid microsphere Au@ZrO_2, the Au@ZrO_2 hollow microspheres showed good catalytic performance in reduction of p-nitroaniline, and p-nitroaniline was completely reduced to pphenylenediamine in 7 min at 45 ℃.
引文
[1]Elmalem E,Saunders A E,Costi R,et al.Adv.Mater.,2008,20:4312-4317
[2]Zhai C Y,Zhu M S,Pang F Z,et al.ACS Appl.Mater.Interfaces,2016,8:5972-5980
[3]Zhai C Y,Zhu M S,Duan B,et al.J.Power Sources,2015,275:483-488
[4]Zhu M S,Zhai C Y,Sun M J,et al.Appl.Catal.B:Environ.,2017,203:108-115
[5]Wang X,Perret N,Keane M A.Appl.Catal.A:Gen.,2013,467:575-584
[6]Kuroda K,Ishida T,Haruta M.J.Mol.Catal.A:Chem.,2009,298(1):7-11
[7]Ismail A A,Hakki A,Bahnemann D W.J.Mol.Catal.A:Chem.,2012,358(6):145-151
[8]Evangelista V,Acosta B,Miridonov S,et al.Appl.Catal.B:Environ.,2015,166-167:518-528
[9]Zhu J,Zoltan Kónya,Puntus V F,et al.Langmuir,2003,19(10):4396-4401
[10]Tuzovskaya I,Bogdanchikova N,Simakov A,et al.Chem.Phys.,2007,338(1):23-32
[11]Zanella R,Rodríguezgonzález V,Arzola Y,et al.ACS Catal.,2011,2(1):1-11
[12]Smolentseva E,Kusema B T,Beloshapkin S,et al.Appl.Catal.A:Gen.,2011,392(1/2):69-79
[13]Sandoval A,Aguilar A,Louis C,et al.J.Catal.,2011,281(1):40-49
[14]WANG Jing(王晶),XU Ji-Tai(许吉泰),GONG Nian(龚念).Bull.Chinese Ceram.Soc.(硅酸盐通报),2013,32(5):936-940
[15]Wang C,Le Y,Cheng B J.Ceram.Int.,2014,40(7):10847-10856
[16]Xiao M,Li Y G,Lu Y F,et al.J.Mater.Chem.A,2015,3(6):2701-2706
[17]Yang X,Zhao N,Zhou Q,et al.J.Mater.Chem.C,2013,1(1):3359-3366
[18]Lin Y F,Liang F L.Cryst Eng Comm,2015,17:678-685
[19]Kumar P N.RSC Adv.,2014,4:29946-29956
[20]YANG Shu-Mei(杨淑梅),DENG Shu-Hua(邓淑华),HUANG Hui-Min(黄惠民),et al.Ind.Catal.(工业催化),2003,11(10):39-43
[21]Lin F Q,Dong W S,Liu C L,et al.J.Colloid Interface Sci.,2008,323(2):365-71
[22]JIANG Feng(江峰),LI Sa(李洒),PENG Zhi-Jian(彭志坚).Bull.Chinese Ceram.Soc.(硅酸盐通报),2014,42(9):1087-1091
[23]CHEN Guo-Hong(陈国红),ZHOU Fang-Ling(周芳玲),LI Qiao-Ling(李巧玲),et al.Chinese J.Inorg.Chem.(无机化学学报),2015,31(11):2181-2187
[24]WANG Wen-Juan(王文娟),ZHANG Hai-Peng(张海鹏),HAN Yu-Xiang(韩玉香),et al.Chinese J.Inorg.Chem.(无机化学学报),2014,30(12):2726-2732
[25]Tahir M N,Ragg R,Natalio F,et al.J.Mater.Chem.B,2015,3(11):2371-2377
[26]MA Tian(马天),YANG Jin-Long(杨金龙),ZHANG Li-Ming(张立明),et al.Chinese J.Inorg.Chem.(无机化学学报),2004,20(2):121-127
[27]Guo C,Hu P,Yu L,et al.J.Mater.Lett.,2009,63(12):1013-1015
[28]Jiang Y,Yang S,Ding X,et al.J.Mater.Chem.,2005,15(20):2041-2046
[29]Kuroda Y,Sakamoto Y,Kuroda K.J.Am.Chem.Soc.,2012,134(20):8684-8692
[30]Guo D,Lu Y,Zhao Y,et al.RSC Adv.,2015,5(16):11738-11744
[31]Zhu S,Xue Y,Guo J,et al.ACS Catal.,2016,6(3):2035-2042
[32]Ma J,Guo S,Guo X,et al.Ceram.Int.,2015,41(9):705-708
[2]Zhai C Y,Zhu M S,Pang F Z,et al.ACS Appl.Mater.Interfaces,2016,8:5972-5980
[3]Zhai C Y,Zhu M S,Duan B,et al.J.Power Sources,2015,275:483-488
[4]Zhu M S,Zhai C Y,Sun M J,et al.Appl.Catal.B:Environ.,2017,203:108-115
[5]Wang X,Perret N,Keane M A.Appl.Catal.A:Gen.,2013,467:575-584
[6]Kuroda K,Ishida T,Haruta M.J.Mol.Catal.A:Chem.,2009,298(1):7-11
[7]Ismail A A,Hakki A,Bahnemann D W.J.Mol.Catal.A:Chem.,2012,358(6):145-151
[8]Evangelista V,Acosta B,Miridonov S,et al.Appl.Catal.B:Environ.,2015,166-167:518-528
[9]Zhu J,Zoltan Kónya,Puntus V F,et al.Langmuir,2003,19(10):4396-4401
[10]Tuzovskaya I,Bogdanchikova N,Simakov A,et al.Chem.Phys.,2007,338(1):23-32
[11]Zanella R,Rodríguezgonzález V,Arzola Y,et al.ACS Catal.,2011,2(1):1-11
[12]Smolentseva E,Kusema B T,Beloshapkin S,et al.Appl.Catal.A:Gen.,2011,392(1/2):69-79
[13]Sandoval A,Aguilar A,Louis C,et al.J.Catal.,2011,281(1):40-49
[14]WANG Jing(王晶),XU Ji-Tai(许吉泰),GONG Nian(龚念).Bull.Chinese Ceram.Soc.(硅酸盐通报),2013,32(5):936-940
[15]Wang C,Le Y,Cheng B J.Ceram.Int.,2014,40(7):10847-10856
[16]Xiao M,Li Y G,Lu Y F,et al.J.Mater.Chem.A,2015,3(6):2701-2706
[17]Yang X,Zhao N,Zhou Q,et al.J.Mater.Chem.C,2013,1(1):3359-3366
[18]Lin Y F,Liang F L.Cryst Eng Comm,2015,17:678-685
[19]Kumar P N.RSC Adv.,2014,4:29946-29956
[20]YANG Shu-Mei(杨淑梅),DENG Shu-Hua(邓淑华),HUANG Hui-Min(黄惠民),et al.Ind.Catal.(工业催化),2003,11(10):39-43
[21]Lin F Q,Dong W S,Liu C L,et al.J.Colloid Interface Sci.,2008,323(2):365-71
[22]JIANG Feng(江峰),LI Sa(李洒),PENG Zhi-Jian(彭志坚).Bull.Chinese Ceram.Soc.(硅酸盐通报),2014,42(9):1087-1091
[23]CHEN Guo-Hong(陈国红),ZHOU Fang-Ling(周芳玲),LI Qiao-Ling(李巧玲),et al.Chinese J.Inorg.Chem.(无机化学学报),2015,31(11):2181-2187
[24]WANG Wen-Juan(王文娟),ZHANG Hai-Peng(张海鹏),HAN Yu-Xiang(韩玉香),et al.Chinese J.Inorg.Chem.(无机化学学报),2014,30(12):2726-2732
[25]Tahir M N,Ragg R,Natalio F,et al.J.Mater.Chem.B,2015,3(11):2371-2377
[26]MA Tian(马天),YANG Jin-Long(杨金龙),ZHANG Li-Ming(张立明),et al.Chinese J.Inorg.Chem.(无机化学学报),2004,20(2):121-127
[27]Guo C,Hu P,Yu L,et al.J.Mater.Lett.,2009,63(12):1013-1015
[28]Jiang Y,Yang S,Ding X,et al.J.Mater.Chem.,2005,15(20):2041-2046
[29]Kuroda Y,Sakamoto Y,Kuroda K.J.Am.Chem.Soc.,2012,134(20):8684-8692
[30]Guo D,Lu Y,Zhao Y,et al.RSC Adv.,2015,5(16):11738-11744
[31]Zhu S,Xue Y,Guo J,et al.ACS Catal.,2016,6(3):2035-2042
[32]Ma J,Guo S,Guo X,et al.Ceram.Int.,2015,41(9):705-708