Citation:
WANG Rui-yu, BAI Si-yu, ZHENG Chuan-yue, LI Zhong. Effect of oxidative/reductive pretreatment on the performance of Cu2O/AC catalyst for oxidative carbonylation of methnol[J]. Journal of Fuel Chemistry and Technology,
;2015, 43(10): 1245-1251.
-
The Cu2O/AC catalyst prepared by pyrolysis of copper acetate supported on activatede carbon was pretreated under oxidative (O2/N2) or reductive (H2/N2 and CO/N2) atmospheres. The oxidation/reduction of Cu2O was completed through pretreatment at 350 ℃ for 4 h, the Cu2O in catalyst could be completely oxidized to CuO by oxidative atmosphere, or reduced to metallic copper by reductive atmosphere. The catalyst activities were evaluated in a continuous fixed-bed tubular micro reactor under atmospheric pressure at 140 ℃. The catalyst pretreated by CO/N2 had good Cu0 dispersion on its surface and exhibited the highest activity. The space-time yield and selectivity of DMC reached 261.9 mg/(g·h) and 74.7%, respectively. After 58 h reaction, the valence state of copper species and the catalytic activity of catalysts pretreated by reductive atmosphere were found to be close to that of the Cu2O/AC catalyst. Comparing the catalytic performance, the characterization of surface and bulk copper species before and after reaction, it was obvious that metallic copper exhibited a high initial activity, while Cu2O was stable in catalytic activity and valence state, and CuO was low in activity.
-
-
-
[1]
[1] KELLER N, REBMANN G, KELLER V. Catalysts, mechanisms and industrial processes for the dimethyl carbonate synthesis[J]. J Mol Catal A: Chem, 2010, 317(1/2): 1-18.
-
[2]
[2] 宋一兵, 罗爱国, 杜玉海, 方奕文. 甲醇直接气相氧化羰基化合成碳酸二甲酯[J]. 化学进展, 2008, 20(2/3): 221-226. (SONG Yi-bin, LUO Ai-guo, DU Yu-hai, FANG Yi-wen. Synthesis of dimethyl carbonate by direct vapor-phase oxycarbonylation of methanol[J]. Prog Chem, 2008, 20(2/3): 221-226.)
-
[3]
[3] RICHTER M, FAIT M J G, ECKELT R, SCHNEIDER M, RADNIK J, HEIDEMANN D, FRICKE R. Gas-phase carbonylation of methanol to dimethyl carbonate on chloride-free Cu-precipitated zeolite Y at normal pressure[J]. J Catal, 2007, 245(1): 11-24.
-
[4]
[4] RICHTER M, FAIT M J G, ECKELT R, SCHREIER E, SCHNEIDER M, POHL M-M, FRICKE R. Oxidative gas phase carbonylation of methanol to dimethyl carbonate over chloride-free Cu-impregnated zeolite Y catalysts at elevated pressure[J]. Appl Catal B: Environ, 2007, 73(3/4): 269-281.
-
[5]
[5] 张海涛, 王淑芳, 赵新强, 王延吉. 负载型CuO催化剂上甲醇气相氧化羰基化合成碳酸二甲酯反应研究[J]. 河北工业大学学报, 2004, 33(4): 36-40. (ZHANG Hai-tao,WANG Shu-fang,ZHAO Xin-qiang,WANG Yan-ji. Study of synthesis of dimethyl carbonate by gas-phase oxidative carbonylation of methanol over supported copper catalysts[J]. J Hebei Univ Techol, 2004, 33(4): 36-40.)
-
[6]
[6] 李忠, 文春梅, 王瑞玉, 郑华艳, 谢克昌. 醋酸铜热解制备无氯Cu2O/AC催化剂及其催化氧化羰基化[J]. 高等学校化学学报, 2009, 30(10): 2024-2031. (LI Zhong,WEN Chun-mei, WANG Rui-yu, ZHENG Hua-yan, XIE Ke-chang. Chloride-free Cu2O/AC catalyst prepared by pyrolysis of copper acetate and catalytic oxycarbonylation[J]. Chem J Chin Univ, 2009, 30(10): 2024-2031.)
-
[7]
[7] 李忠, 文春梅, 郑华艳, 谢克昌. 载体表面性质对Cu2O/AC催化剂结构和活性的影响[J]. 高等学校化学学报, 2010, 31(1): 145-152. (LI Zhong, WEN Chun-mei, ZHENG Hua-yan, XIE Ke-chang. Effects of the active carbon surface properties on the structure and catalytic activity of Cu2O/AC catalyst[J]. Chem J Chin Univ, 2010, 31(1): 145-152.)
-
[8]
[8] 章日光, 郑华艳, 王宝俊, 李忠. CO和CH3O在Cu2O (Ш)表面吸附特性及共吸附的理论研究[J]. 高等学校化学学报, 2010, 31(6): 1246-1251. (ZHANG Ri-guang, ZHENG Hua-yan, WANG Bao-jun, LI Zhong. Theoretical study on the properties of CO and CH3O adsorption on Cu2O(111) surface and co-adsorption[J]. Chem J Chin Univ, 2010, 31(6): 1246-1251.)
-
[9]
[9] YAN B, HUANG S Y, WANG S P, MA X B. Catalytic oxidative carbonylation over Cu2O nanoclusters supported on carbon materials: The role of the carbon support[J]. Chem Cat Chem, 2014, 6(9): 2671-2679.
-
[10]
[10] 王瑞玉, 李忠, 郑华艳, 谢克昌. 无氯Cu/AC催化剂的制备及其催化气相甲醇氧化羰基化反应性能[J]. 催化学报, 2010, 31(7): 851-856. (WANG Rui-yu, LI Zhong, ZHENG Hua-yan, XIE Ke-chang. Preparation of chlorine-free Cu/AC catalyst and its catalytic properties for vapor phase oxidative carbonylation of methanol[J]. Chin J Catal, 2010, 31(7): 851-856.)
-
[11]
[11] 任军, 郭长江, 杨雷雷, 李忠. 淀粉基炭负载纳米铜催化合成碳酸二甲酯[J]. 催化学报, 2013, 34(9): 1734-1744. (REN Jun, GUO Chang-jiang, YANG Lei-lei, LI Zhong. Synthesis of dimethyl carbonate over starch-based carbon-supported Cu nanoparticles catalysts[J]. Chin J Catal, 2013, 34(9): 1734-1744.)
-
[12]
[12] REN J, WANG W, WANG D l, ZUO Z J, LIN J Y, LI Z. A theoretical investigation on the mechanism of dimethyl carbonate formation on Cu/AC catalyst[J]. Appl Catal A: Gen, 2014, 472: 47-52.
-
[13]
[13] WANG L C, HE L, LIU Y M, CAO Y, HE H Y, FAN K N, ZHUANG J H. Effect of pretreatment atmosphere on CO oxidation over α-Mn2O3 supported gold catalysts[J]. J Catal, 2009, 264(2): 145-157.
-
[14]
[14] 邹汉波, 陈胜洲, 林维明. Cu1Zr1Ce9Oδ催化剂选择性氧化CO性能的研究[J]. 工业催化, 2008, 16(2): 23-27. (ZOU Han-bo, CHEN Sheng-zhou, LIN Wei-ming. Effect of reaction conditions on the performance of Cu1Zr1Ce9Oδ catalyst for selective oxidation of CO[J]. Ind Catal, 2008, 16(2): 23-27.)
-
[15]
[15] 张丽萍, 万海勤, 朱捷, 宋春燕, 刘斌, 李丹, 董林. CO预处理对CuO/γ-Al 2O3催化剂性能的影响[J]. 无机化学学报, 2007, 23(3): 427-431. (ZHANG Li-ping, WAN Hai-qin, ZHU Jie, SONG Chun-yan, LIU Bin, LI Dan, DONG Lin. Effect of CO pretreatment on properties of CuO/γ-Al 2O3 catalyst[J]. Chin J Inorg Chem, 2007, 23(3): 427-431.)
-
[16]
[16] WAN H Q, LI D, DAI Y, HU Y H, ZHANG Y H, LIU L J, ZHAO B, LIU B, SUN K Q, DONG L, CHEN Y. Effect of CO pretreatment on the performance of CuO/CeO2/γ-Al2O3 catalysts in CO+O2 reactions[J]. Appl Catal A: Gen, 2009, 360(1): 26-32.
-
[17]
[17] BUKUR D B, LANG X S, DING Y J. Pretreatment effect studies with a precipitated iron Fischer-Tropsch catalyst in a slurry reactor[J]. Appl Catal A: Gen, 1999, 186(1/2): 255-275.
-
[18]
[18] ZHANG Y C, TANG J Y, WANG G L, ZHANG M, HU X Y. Facile synthesis of submicron Cu2O and CuO crystallites from a solid metalorganic molecular precursor[J]. J Cryst Growth, 2006, 294(2): 278-282.
-
[19]
[19] HUANG L, PENG F, YU H, WANG H J. Preparation of cuprous oxides with different sizes and their behaviors of adsorption, visible-light driven photocatalysis and photocorrosion[J]. Solid State Sci, 2009, 11(1): 129-138.
-
[20]
[20] CHEN A P, LONG H, LI X C, LI Y H, YANG G, LU P X. Controlled growth and characteristics of single-phase Cu2O and CuO films by pulsed laser deposition[J]. Vacuum, 2009, 83(6): 927-930.
-
[21]
[21] WANG L C, LIU Y M, CHEN M, CAO Y, HE H Y, WU G S, DAI W L, FAN K N. Production of hydrogen by steam reforming of methanol over Cu/ZnO catalysts prepared via a practical soft reactive grinding route based on dry oxalate-precursor synthesis[J]. J Catal, 2007, 246(1): 193-204.
-
[22]
[22] GVNTER M M, RESSLER T, JENTOFT R E, BEMS B.Redox behavior of copper oxide/zinc oxide catalysts in the steam reforming of methanol studied by in situ X-ray diffraction and adsorption spectroscopy[J]. J Catal, 2001, 203(1): 133-149.
-
[23]
[23] LUO M F, FANG P, HE M, XIE Y L. In situ XRD, Raman, and TPR studies of CuO/Al2O3 catalysts for CO oxidation[J]. J Mol Catal A: Chem, 2005, 239(1/2): 243-248.
-
[24]
[24] 李忠, 黄海彬, 谢克昌. Cu(I)/SO42-/ZnO和Cu(I)/S28O2-/ZnO催化剂的制备与表征[J]. 高等学校化学学报, 2008, 29(8): 1609-1615. (LI Zhong, HUANG Hai-bin, XIE Ke-chang. Preparation and characterization of Cu(I)/SO42-/ZnO and Cu(I)/S28O2-/ZnO catalysts[J]. Chem J Chin Univ, 2008, 29(8): 1609-1615.)
-
[25]
[25] LEE C Y, HA B H. Reduction behavior of copper oxide in copper/mordenites[J]. Stud Surf Sci Catal, 1994, 84: 1563-1570.
-
[26]
[26] WAN Y, MA J X, WANG Z, ZHOU W, KALIAGUINE S. Selective catalytic reduction of NO over Cu-Al-MCM-41[J]. J Catal, 2004, 227(1): 242-252.
-
[27]
[27] YANG P, CAO Y, DAI W L, DENG J F, FAN K N. Effect of chemical treatment of activated carbon as a support for promoted dimethyl carbonate synthesis by vapor phase oxidative carbonylation of methanol over Wacker-type catalysts[J]. Appl Catal A: Gen, 2003, 243(2): 323-331.
-
[28]
[28] 姜瑞霞, 宋兴涛, 陈大伟, 畅延青, 谢在库. 高温氢气处理对活性炭及钯炭催化剂性能的影响[J]. 化学反应工程与技术, 2007, 23(4): 375-379. (JIANG Rui-xia, SONG Xing-tao, CHEN Da-wei, CHANG Yan-qing, XIE Zai-ku. Effects of hydrogen treatment on the properties of activated carbon and Pd/C catalysts[J]. Chem React Eng Technol, 2007, 23(4): 375-379.)
-
[1]
-
-
-
[1]
Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-Based Photocatalysts for CO2 Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2406029-0. doi: 10.3866/PKU.WHXB202406029
-
[2]
Honghong Zhang , Zhen Wei , Derek Hao , Lin Jing , Yuxi Liu , Hongxing Dai , Weiqin Wei , Jiguang Deng . 非均相催化CO2与烃类协同催化转化的最新进展. Acta Physico-Chimica Sinica, 2025, 41(7): 100073-0. doi: 10.1016/j.actphy.2025.100073
-
[3]
Jiapei Zou , Junyang Zhang , Xuming Wu , Cong Wei , Simin Fang , Yuxi Wang . A Comprehensive Experiment Based on Electrocatalytic Nitrate Reduction into Ammonia: Synthesis, Characterization, Performance Exploration, and Applicable Design of Copper-based Catalysts. University Chemistry, 2024, 39(6): 373-382. doi: 10.3866/PKU.DXHX202312081
-
[4]
Xiting Zhou , Zhipeng Han , Xinlei Zhang , Shixuan Zhu , Cheng Che , Liang Xu , Zhenyu Sun , Leiduan Hao , Zhiyu Yang . Dual Modulation via Ag-Doped CuO Catalyst and Iodide-Containing Electrolyte for Enhanced Electrocatalytic CO2 Reduction to Multi-Carbon Products: A Comprehensive Chemistry Experiment. University Chemistry, 2025, 40(7): 336-344. doi: 10.12461/PKU.DXHX202412070
-
[5]
Qiqi Li , Su Zhang , Yuting Jiang , Linna Zhu , Nannan Guo , Jing Zhang , Yutong Li , Tong Wei , Zhuangjun Fan . Preparation of High Density Activated Carbon by Mechanical Compression of Precursors for Compact Capacitive Energy Storage. Acta Physico-Chimica Sinica, 2025, 41(3): 2406009-0. doi: 10.3866/PKU.WHXB202406009
-
[6]
Jianjun LI , Mingjie REN , Lili ZHANG , Lingling ZENG , Huiling WANG , Xiangwu MENG . UV-assisted degradation of tetracycline hydrochloride by MnFe2O4@activated carbon activated persulfate. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1869-1880. doi: 10.11862/CJIC.20240187
-
[7]
Yajin Li , Huimin Liu , Lan Ma , Jiaxiong Liu , Dehua He . Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO2 over Au/Co3O4-ZnO Catalyst. Acta Physico-Chimica Sinica, 2024, 40(9): 2308005-0. doi: 10.3866/PKU.WHXB202308005
-
[8]
Guanghui SUI , Yanyan CHENG . Application of rice husk-based activated carbon-loaded MgO composite for symmetric supercapacitors. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 521-530. doi: 10.11862/CJIC.20240221
-
[9]
Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH2 supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317
-
[10]
Hailang JIA , Pengcheng JI , Hongcheng LI . Preparation and performance of nickel doped ruthenium dioxide electrocatalyst for oxygen evolution. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1632-1640. doi: 10.11862/CJIC.20240398
-
[11]
Wentao Xu , Xuyan Mo , Yang Zhou , Zuxian Weng , Kunling Mo , Yanhua Wu , Xinlin Jiang , Dan Li , Tangqi Lan , Huan Wen , Fuqin Zheng , Youjun Fan , Wei Chen . Bimetal Leaching Induced Reconstruction of Water Oxidation Electrocatalyst for Enhanced Activity and Stability. Acta Physico-Chimica Sinica, 2024, 40(8): 2308003-0. doi: 10.3866/PKU.WHXB202308003
-
[12]
Dong Xiang , Kunzhen Li , Kanghua Miao , Ran Long , Yujie Xiong , Xiongwu Kang . Amine-Functionalized Copper Catalysts: Hydrogen Bonding Mediated Electrochemical CO2 Reduction to C2 Products and Superior Rechargeable Zn-CO2 Battery Performance. Acta Physico-Chimica Sinica, 2024, 40(8): 2308027-0. doi: 10.3866/PKU.WHXB202308027
-
[13]
Bing WEI , Jianfan ZHANG , Zhe CHEN . Research progress in fine tuning of bimetallic nanocatalysts for electrocatalytic carbon dioxide reduction. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 425-439. doi: 10.11862/CJIC.20240201
-
[14]
Xuejie Wang , Guoqing Cui , Congkai Wang , Yang Yang , Guiyuan Jiang , Chunming Xu . Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers. Acta Physico-Chimica Sinica, 2025, 41(5): 100044-0. doi: 10.1016/j.actphy.2024.100044
-
[15]
Ping Song , Nan Zhang , Jie Wang , Rui Yan , Zhiqiang Wang , Yingxue Jin . Experimental Teaching Design on Synthesis and Antitumor Activity Study of Cu-Pyropheophorbide-a Methyl Ester. University Chemistry, 2024, 39(6): 278-286. doi: 10.3866/PKU.DXHX202310087
-
[16]
Yuchen Zhou , Huanmin Liu , Hongxing Li , Xinyu Song , Yonghua Tang , Peng Zhou . Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde. Acta Physico-Chimica Sinica, 2025, 41(6): 100067-0. doi: 10.1016/j.actphy.2025.100067
-
[17]
Dan Li , Hui Xin , Xiaofeng Yi . Comprehensive Experimental Design on Ni-based Catalyst for Biofuel Production. University Chemistry, 2024, 39(8): 204-211. doi: 10.3866/PKU.DXHX202312046
-
[18]
Huiwei Ding , Bo Peng , Zhihao Wang , Qiaofeng Han . Advances in Metal or Nonmetal Modification of Bismuth-Based Photocatalysts. Acta Physico-Chimica Sinica, 2024, 40(4): 2305048-0. doi: 10.3866/PKU.WHXB202305048
-
[19]
Yushan Cai , Fang-Xing Xiao . Revisiting MXenes-based Photocatalysis Landscape: Progress, Challenges, and Future Perspectives. Acta Physico-Chimica Sinica, 2024, 40(8): 2306048-0. doi: 10.3866/PKU.WHXB202306048
-
[20]
Yuanyin Cui , Jinfeng Zhang , Hailiang Chu , Lixian Sun , Kai Dai . Rational Design of Bismuth Based Photocatalysts for Solar Energy Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2405016-0. doi: 10.3866/PKU.WHXB202405016
-
[1]
Metrics
- PDF Downloads(0)
- Abstract views(757)
- HTML views(86)