以纺锤体状单晶氧化铜、片状单晶氧化镧和硝酸盐为金属源, 通过水热法并灼烧所得产物, 制备了具有纺锤体状、棒状和短链状类钙钛矿型氧化物 La2(xSrxCuO4 (x = 0, 1)单晶纳微米粒子. 采用 X 射线衍射、扫描电镜、透射电镜、X 射线光电子能谱、氢气程序升温还原、氧气程序升温脱附以及 N2 吸附等技术对所得催化剂的物化性质进行了表征, 考察了这些样品催化甲烷氧化反应的性能. 结果表明, 将 Sr 部分引入 La2CuO4 的晶格中可增加催化剂表面吸附氧量、Cu3+含量和还原能力. 在空速为 50 000 ml/(g·h) 和 CH4/O2 摩尔比为 1/10 的条件下, 以硝酸盐为金属源制得的 LaSrCuO4 表现出最高的催化活性, 在 675 ℃ 时甲烷反应速率高达 40.9 mmol/(g·h) . 这一优良的催化性能与其表面较高的氧空位浓度、独特的单晶结构和特定的表面形貌有关.
参考文献
[1] | Wang C H;Chen C L;Weng H S .[J].Chemosphere,2004,57:1131. |
[2] | Kaddouri, A;Ifrah, S;Gelin, P .A study of the influence of the synthesis conditions upon the catalytic properties of LaMnO3.15 in methane combustion in the absence and presence of H2S[J].Catalysis Letters,2007(3/4):237-244. |
[3] | Arendt E;Maione A;Klisinska A;Sanz O Montes M Suarez S Blanco J Ruiz P .[J].Applied Catalysis A:General,2008,339:1. |
[4] | Teng F;Han W;Liang S H;Gaugeu B Zong R L Zhu Y F .[J].Journal of Catalysis,2007,250:1. |
[5] | Banerjee S;Choudhary V R .[J].Proceedings-Indian Academy of Sciences Chemical Sciences,2000,112:535. |
[6] | Falcon H. .Defect LaCuO_(3-#delta#(#delta#=0.05-0.45)perovskites Bulk and surface structures and their relevance in CO oxidation[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2000(2):131-142. |
[7] | Spinicci R.;Tofanari A.;Delmastro A.;Mazza D.;Ronchetti S. .Catalytic properties of stoichiometric and non-stoichiometric LaFeO3 perovskite for total oxidation of methane[J].Materials Chemistry and Physics,2002(1):20-25. |
[8] | Nie HW;Wen TL;Wang SR;Wang YS;Guth U;Vashook V .Preparation, thermal expansion, chemical compatibility, electrical conductivity and polarization of A(2)-alpha A 'alpha MO4 (A = Pr, Sm; A ' = Sr; M = Mn, Ni; alpha = 0.3, 0.6) as a new cathode for SOFC[J].Solid state ionics,2006(19/25):1929-1932. |
[9] | 白雪,刘源,王晓燕,张通,于文国.La1-x-yBaxREyMnO3复合氧化物的制备及其对甲烷燃烧的催化性能[J].催化学报,2004(07):577-580. |
[10] | Gao LZ.;Au CT. .Studies on the redox behaviour of La1.867Th0.100CuO4 and its catalytic performance for NO decomposition[J].Catalysis Letters,2000(1/3):91-98. |
[11] | Urban J J;Yun W S;Gu Q;Park H .[J].Journal of the American Chemical Society,2002,124:1186. |
[12] | Miao J;Hu C G;Liu H;Xiong Y F .[J].Materials Letters,2008,62:235. |
[13] | Mao Y B;Banerjee S;Wong S S.[J].Chemical Communications,2003:408. |
[14] | Wang Y W;Xu H;Wang X B;Zhang X Jia H M Zhang L Z Qiu J R .[J].Journal of Physical Chemistry B,2006,110:13835. |
[15] | Chen C;Cheng JR;Yu SW;Che LJ;Meng ZY .Hydrothermal synthesis of perovskite bismuth ferrite crystallites[J].Journal of Crystal Growth,2006(1):135-139. |
[16] | Deng J G;Zhang L;Dai H X;He H Au C T .[J].Catalysis Letters,2008,123:294. |
[17] | Yang Z H;Xu J;Zhang W X;Liu A P Tang S P .[J].Journal of Solid State Chemistry,2007,180:1390. |
[18] | 姚超,马江权,林西平,汪信.纳米氧化镧的制备[J].高校化学工程学报,2003(06):685-688. |
[19] | He H;Dai H X;Au C T .[J].Applied Catalysis B:Environmental,2001,33:65. |
[20] | Wang P.;Yao L. .XPS and voltammetric studies on La_(1-x) Sr_xCoO_(3-#delta#) perovskite oxide electrodes[J].Journal of Alloys and Compounds: An Interdisciplinary Journal of Materials Science and Solid-state Chemistry and Physics,2000(1):53-56. |
[21] | Dai HX.;Au CT.;Ng CF. .Hole-doped La1.85Sr0.15CuO4-delta X sigma (X = F, Cl) and electron-doped Nd1.85Ce0.15Cu4-delta X sigma halo-oxide catalysts for the selective oxidation of ethane to ethene[J].Journal of Catalysis,2001(2):251-266. |
[22] | Zhu JJ;Zhao Z;Xiao DH;Li J;Yang XG;Wu Y .Study of La2-xSrxCuO4 (x=0.0, 0.5, 1.0) catalysts for NO plus CO reaction from the measurements of O-2-TPD, H-2-TPR and cyclic voltammetry[J].Journal of molecular catalysis, A. Chemical,2005(1/2):35-40. |
[23] | Liu J;Zhao Z;Xu CM;Duan AJ .Simultaneous removal of NOx and diesel soot over nanometer Ln-Na-Cu-O perovskite-like complex oxide catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(1/2):61-72. |
[24] | BULGAN G.,方滕飞,梁淑惠,姚文清,朱永法.Cu掺杂对LaMnO3催化剂的结构和催化氧化性能的影响[J].物理化学学报,2007(09):1387-1392. |
[25] | Teng F;Liang Sh H;Gauge B;Zhu Y F Xu J G Wen G D Tian Zh J Wang Zh M Yang X M Xiong G X .[J].Journal of Physical Chemistry C,2007,111:10941. |
[26] | Petrovic S;Karanovic L;Stefanov PK;Zdujic M;Terlecki-Baricevic A .Catalytic combustion of methane over Pd containing perovskite type oxides[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2005(1/2):133-141. |
[27] | Liang S H;Teng F;Gulgan G;Zhu Y F .[J].Journal of Physical Chemistry C,2007,111:16742. |
[28] | Kirchnerova J.;Klvana D. .Design criteria for high-temperature combustion catalysts[J].Catalysis Letters,2000(2/4):175-181. |
[29] | Alifanti M;Kirchnerova J;Delmon B .[J].Applied Catalysis A:General,2003,245:231. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%