郑海龙(1989-),硕士研究生,主要研究方向为纳米锰氧化物选择性催化氧化小分子有机物.
网络首发:2017-03-09,
纸质出版:2017
移动端阅览
郑海龙, 廖菽欢, 余林. 介孔Cu-Mn复合氧化物催化氧化苯甲醇合成苯甲醛的研究[J]. 广东工业大学学报, 2017, 34(2): 28-33.
Zheng Hai-long, Liao Shu-huan, Yu Lin. A Research of Mesoporous Copper-Manganese Mixed Oxides for Selective Oxidation of Benzyl Alcohol to Benzaldehyde[J]. 2017, 34(2): 28-33.
郑海龙, 廖菽欢, 余林. 介孔Cu-Mn复合氧化物催化氧化苯甲醇合成苯甲醛的研究[J]. 广东工业大学学报, 2017, 34(2): 28-33. DOI: 10.12052/gdutxb.160025.
Zheng Hai-long, Liao Shu-huan, Yu Lin. A Research of Mesoporous Copper-Manganese Mixed Oxides for Selective Oxidation of Benzyl Alcohol to Benzaldehyde[J]. 2017, 34(2): 28-33. DOI: 10.12052/gdutxb.160025.
采用无模板共沉淀法合成介孔Cu-Mn复合氧化物,该氧化物具有很高的比表面积且可大量合成.该复合氧化物(Cu-Mn-
x
,
x
=1,2,4)作为催化剂应用在以O
2
为氧化剂,甲苯为溶剂的苯甲醇选择性氧化合成苯甲醛的研究中,发现该催化剂显示出很高的活性.当
n
(Cu):
n
(Mn)的设计比例为1:2时活性最高,在102℃的温度下,苯甲醇转化率达到90%时仅需20 min,选择性达到98%.催化剂的物理化学特性采用了XRD、SEM、TEM、BET、H
2
-TPR和EDS技术进行表征.结果表明,Cu和Mn具有协同促进作用,能够互相提高催化活性,但必须控制在一定的比例范围内;另外催化剂的活性与用量关系很大,量越大活性越高.
A novel template-free co-precipitation method was applied to synthesize mesoporous copper-manganese mixed oxides with high surface area
which can be obtained in large quantities. Catalytic activity of copper-manganese mixed oxides (Cu-Mn-
x
x
=1
2
4) has been studied in selective oxidation of benzyl alcohol using molecular oxygen as oxidizing agent and toluene as solvent. The catalysts exhibited highest activity
in which 90% conversion of the benzyl alcohol was achieved with 98% selectivity to benzaldehyde within a short reaction period only in 20 min at 102℃
when the design mole ratio of Cu/Mn was 1:2. The
physicochemical properties of the catalysts were characterized by XRD
SEM
TEM
BET
H2-TPR and EDS techniques. It shows that Cu and Mn can improve the catalytic performance each other effectively but there must be an appropriate mole ratio of Cu/Mn. In addition
there is a great relationship between the activity and the amount of catalysts
which shows that the higher activity the more catalysts.
张昕, 吴伟伟, 黄启权, 等. 苯甲醇液相氧化制苯甲醛催化剂的研究进展[J]. 石油化工, 2010, 02:215-223.ZHANG X, WU W W, HUANG Q Q, et al. Advance in catalysts for green liquid-phase oxidation of benzyl alcohol to benzaldehyde[J]. Electrochemical Technology, 2010, 02:215-223.
KCKRITZ A, SEBEK M, DITTMAR A, et al. Ru-catalyzed oxidation of primary alcohol[J]. J Mol Catal A:Chem, 2006, 246(1~2):85-99.
STUCHINSKAYA T L, KOZHEVNIKOV I V. Liquid-phase oxidation of alcohols with oxygen catalysed by modified palladium (Ⅱ) oxide[J]. Catal Commum, 2003, 4(8):417-422.
SU F Z, CHEN M, WANG L C, et al. Aerobic oxidation of alcohols catalyzed by gold nanoparticles supported on gallia[J]. Polymorphs Catal Commum, 2008, 9(6):1027-1032.
BEIER M J, HANSEN T W, GRUNWALDT J D. Selective liquid-phase oxidation of alcohols catalyzed by a silver-based catalyst promoted by the presence of ceria[J]. Journal of Catalysis, 2009, 266(2):320-330.
MENG X J, LIN K F, YANG X Y, et al. Catalytic oxidation of olefins and alcohols by molecular oxygen under air pressure over Cu 2 (OH)PO 4 and Cu 4 O(PO4) 2 catalysts[J ] . J Catal, 2003, 218(2):460-464.
CHOUDHARY V R, DUMBRE D K, UPHADE B S, et al. Solvent-free oxidation of benzyl alcohol to benzaldehyde by tert-butyl hydroper oxide using transition metal containing layered double hydroxides and/or mixed hydroxides[J]. J Mol Catal A:Chem, 2004, 215(1-2):129-135.
HU J, SUN K Q, HE D P, et al. Amorphous manganese oxide for catalytic selective oxidation of benzyl alcohol[J]. Chinese Journal of Catalysis, 2007, 28(12):1025-1027.
TANG Q H, HUANG X N, WU C M, et al. Structure and catalytic properties of K-doped manganese oxide supported on alumina[J]. J Mol Catal A:Chem, 2009, 306(1-2):48-53.
SHEN Y F, SUIB S L, O'YONG C L. Cu containing octahedral molecular sieves and octahedral layered materials[J]. J Catal, 1996, 161(1):115-122.
符志伟, 程高, 林婷, 等. 二氧化锰制备及催化燃烧甲苯性能研究[J ] . 广东工业大学学报, 2016, 33(02):85-90.FU Z W, CHENG G, LIN T, et al. The preparation of MnO 2 and application in catalytic combustion of toluene[J ] . Journal of Guangdong University of Technology, 2016, 33(02):85-90.
FANG D, XIE J L. Effect of CuMn 2 O 4 spinel in Cu-Mn oxide catalysts on selective catalytic reduction of NO x with NH 3 at low temperature[J ] . RSC Adv, 2014, 4(49):25540-25551.
TANG W X, WU X F, LI S D. Porous Mn-Co mixed oxide nanorod as a novel catalyst with enhanced catalytic activity for removal of VOCs[J]. Catalysis Communications, 2014, 56(56):134-138.
LI G N, LI L, SHI J J. One-pot pyrolytic synthesis of mesoporous MCo 2 O 4 (4.5)(M=Mn, Ni, Fe, Cu) spinels and its high efficient catalytic properties for CO oxidation at low temperature[J ] . Journal of Molecular Catalysis A-Chemical, 2014, 390(8):97-104.
TANG W X, WU X F, LI S D, et al. Co-nanocasting synthesis of mesoporous Cu-Mn composite oxides and their promoted catalytic activities for gaseous benzene removal[J]. Applied Catalysis B-Environmental, 2015, 162:110-121.
LIU X S, JIN Z N, LU J Q, et al. Highly active CuO/OMS-2 catalysts for low-temperature CO oxidation[J]. Chemical Engineering Journal, 2010, 162(1):151-157.
KRMER M, SCHMIDT T, STWE K, et al. Structural and catalytic aspects of sol-gel derived copper manganese oxides as low-temperature CO oxidation catalyst[J]. Applied Catalysis A:General, 2006, 302(2):257-263.
TANG Q H, GONG X N, ZHAO P Z, et al. Copper-manganese oxide catalysts supported on alumina:Physicochemical features and catalytic performances in the aerobic oxidation of benzyl alcohol[J]. Applied Catalysis A-General, 2010, 389(1-2):101-107.
TANG W X, WU X F, CHEN Y F, et al. Oxalate route for promoting activity of manganese oxide catalysts in total VOCs' oxidation:effect of calcination temperature and preparation method[J]. Mater Chem A, 2014, 2(8):2544-2554.
SHU Z, HUANG W M, SHI J L, et al. Template-free synthesis of mesoporous X-Mn (X=Co, Ni, Zn) bimetal oxides and catalytic application in the room temperature removal of low-concentration NO[J]. Mater Chem A, 2013, 1(35):10218-10227.
ALI R, SIDDIQUI M R, WARTHAN A A. Selective oxidation of benzyl alcohol with molecular oxygen over copper-manganese oxide catalyst[J]. Oxidation Communications, 2011, 34(4):778-787.
PAPAVASILIOU J, AVGOUROPOULOS G, IOANNIDES T. Combined steam reforming of methanol over Cu-Mn spinel oxide catalysts[J]. Journal of Catalysis, 2007, 251(1):7-20.
0
浏览量
0
下载量
0
CSCD
关联资源
相关文章
相关作者
相关机构
京公网安备11010802024621