采用沉积.沉淀法和氨水络合法制备了Al_2O_3,TiO_2,CeO_2和SiO_2负载的纳米金催化剂,利用元素分析、x射线衍射、氮气物理吸附、程序升温还原、透射电镜和拉曼光谱等技术对催化剂进行了表征,并考察了其低温催化甲醛氧化活性.结果表明,Au/CeO_2的催化性能最佳,在40℃时甲醛转化率仍能保持在80%以上.催化剂的活性同时受Au的化学状态和载体性质的影响.Au/CeO_2催化剂较高的低温活性可能与离子态的Au物种有关,同时AuxCe_(1-x)O_(2-δ)固溶体的形成产生了大量的氧缺位,提高了氧的活化能力,也有助于提高催化剂的低温活性.
A series of gold catalysts were prepared by a deposition-precipitation method and an ammonia-complex method on different metal oxides (Al_2O_3, TiO_2, CeO_2, and SiO_2) and tested for low temperature HCHO oxidation. The Au/CeO_2 catalyst exhibited the highest activity with 80% of conversion obtained even at 40℃. The catalysts were characterized by inductively coupled plasma, X-ray diffraction, N2 adsorption, temperature-programmed reduction, transmission electron microscopy, and Raman spectroscopy. The results show that the reactivity of HCHO oxidation is influenced by the chemical state of Au species and the properties of the supports. The high activity obtained on the Au/CeO_2 catalyst was probably due to the presence of cationic Au species (Au~(3+)) in the catalyst and the formation of AuxCe_(1-x)O_(2-δ) solid solution, which generates oxygen vacancies and activates the oxygen species and consequently enhance the activity.
参考文献
| [1] | Tang X F;Li Y G;Huang X M;Xu Y D Zhu H Q Wang J G Shen W J .[J].Applied Catalysis B:Environmental,2006,62:265. |
| [2] | Zhang CB;He H;Tanaka K .Catalytic performance and mechanism of a Pt/TiO2 catalyst for the oxidation of formaldehyde at room temperature[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(1/2):37-43. |
| [3] | Collins JJ;Ness R;Tyl RW;Krivanek N;Esmen NA;Hall TA .A review of adverse pregnancy outcomes and formaldehyde exposure in human and animal studies.[J].Regulatory Toxicology and Pharmacology: RTP,2001(1):17-34. |
| [4] | Shen Y N;Yang X Z;Wang Y Z;Zhang Y B Zhu H Y Gao L Jia M L .[J].Applied Catalysis B:Environmental,2008,79:142. |
| [5] | Li C Y;Shen Y N;Jia M L;Sheng S S Adebajo M O Zhu H Y .[J].Catalysis Communications,2008,9:355. |
| [6] | Sekine Y;Nishimura A .[J].Atom Spher Environ,2001,35:2001. |
| [7] | Alvarez-Galvan M C;de la Pefta O'Shea V A;Fierro J L G;Arias P L .[J].Catalysis Communications,2003,4:223. |
| [8] | Tang X F;Chen J L;Li Y G;Xu Y D Shen W J .[J].Chemical Engineering Journal,2006,118:119. |
| [9] | 廖卫平;董园园;金明善;何涛 索掌怀 .[J].催化学报,2008,29:1 34. |
| [10] | 李锦卫,詹瑛瑛,张凤利,林性贻,郑起.改性沉积-沉淀法制备Au/Fe2O3水煤气变换反应催化剂[J].催化学报,2008(04):346-350. |
| [11] | 王东辉,董同欣,史喜成,郝郑平.纳米金催化剂的存放失活[J].催化学报,2007(02):148-152. |
| [12] | Haruta M .[J].Catalysis Today,1997,36:153. |
| [13] | Haruta M;Yamada N;Kobayshi T;Iijima S .[J].Journal of Catalysis,1989,115:301. |
| [14] | Chen M S;Goodman D W .[J].Catalysis Today,2006,111:22. |
| [15] | Haruta M .[J].Cattech,2002,6:102. |
| [16] | Tabakova T;Boccuzzi F;Manzoli M;Andreeva D .[J].Applied Catalysis A:General,2003,252:385. |
| [17] | Guzman J;Gates B C .[J].Journal of the American Chemical Society,2004,126:2672. |
| [18] | Qian K;Huang W X;Jiang Z Q;Sun H X .[J].Journal of Catalysis,2007,248:137. |
| [19] | Lai S Y;Qiu Y F;Wang S J .[J].Journal of Catalysis,2006,237:303. |
| [20] | Weiher N;Bus E;Delannoy L;Louis C;Ramaker DE;Miller JT;van Bokhoven JA .Structure and oxidation state of gold on different supports under various CO oxidation conditions[J].Journal of Catalysis,2006(2):100-107. |
| [21] | Pillai UR;Deevi S .Highly active gold-ceria catalyst for the room temperature oxidation of carbon monoxide[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):266-273. |
| [22] | Fu Q.;Saltsburg H.;Flytzani-Stephanopoulos M. .Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts[J].Science,2003(5635):935-938. |
| [23] | Calla J T;Davis R J .[J].Journal of Physical Chemistry B,2005,109:2307. |
| [24] | Luo MF.;Zheng XM.;Zhong YJ.;Wu TH.;Lu GL. .Redox properties of CexZr1-xO2 mixed oxides prepared by the sol-gel method[J].Journal of Materials Science Letters,1998(18):1553-1557. |
| [25] | Yao HC;YuYYF .[J].Journal of Catalysis,1984,86:254. |
| [26] | Guzman J;Carrettin S;Corma A .[J].Journal of the American Chemical Society,2005,127:3286. |
| [27] | Bond G C;Louis C;Thompson D T.Catalysis by Gold[M].London:Imperial College Press,2006:185. |
| [28] | Bera P;Hegde M S .[J].Catalysis Letters,2002,79:75. |
| [29] | Venezia A M;Pantaleo G;Longo A;Carlo G D Casaletto M P Liotta F L Deganello G .[J].Journal of Physical Chemistry B,2005,109:2821. |
| [30] | McBride J R;Hass K C;Poindexter B D;Weber W H .[J].Journal of Applied Physics,1994,76:2435. |
| [31] | Pu Z Y;Liu X S;Jia A P;Xie Y L Lu J Q Luo M F .[J].Journal of Physical Chemistry C,2008,112:15045. |
| [32] | Zhang X;Wang H;Xu B Q .[J].Journal of Physical Chemistry B,2005,109:9678. |
| [33] | Carrettin S;Concepci6n P;Corma A;Nieto J M L,Puntes V F .[J].Angewandte Chemie International Edition,2004,43:2538. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%