OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

引用本文: 傅之丹, 臧佳欣, 叶青, 程水源, 康天放. OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能[J]. 物理化学学报, 2017, 33(9): 1855-1864. doi: 10.3866/PKU.WHXB201704282 shu

Citation: FU Zhi-Dan, ZANG Jia-Xin, YE Qing, CHENG Shui-Yuan, KANG Tian-Fang. Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate[J]. Acta Physico-Chimica Sinica, 2017, 33(9): 1855-1864. doi: 10.3866/PKU.WHXB201704282 shu

OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

北京工业大学区域大气复合污染防治北京市重点实验室, 北京 100124
基金项目:
国家自然科学基金（21277008，20777005），北京市自然科学基金（8082008）和北京市教委教师队伍建设（IDHT20140504）资助项目

摘要: 采用氧化还原法合成了层状锰氧化物（OL），并以OL为载体采用离子交换法制备了不同Cu负载量的Cu_x/OL催化剂。利用X射线衍射（XRD）、电子扫描电镜（SEM）、N₂吸附/脱附、H₂-程序升温还原（H₂-TPR）、TG（热重）、X射线光电子能谱（XPS）、O₂-程序升温脱附（O₂-TPD）等技术对所制催化剂进行结构和织构表征，并对其催化氧化CO及乙酸乙酯活性进行了评价。结果表明，OL具有典型的层状锰氧化物结构，适量掺杂Cu对OL的结构和织构影响不大，但Cu的掺杂明显影响Cu_x/OL的还原性、氧移动性及催化剂表面Cu²⁺/CuO、（Mn²⁺+Mn³⁺）/Mn⁴⁺和O_ads/O_latt的比例。Cu_x/OL的催化性能与以上因素密切相关。在Cu_x/OL样品中，Cu₅/OL催化剂具有最佳的催化活性（CO催化氧化，T₅₀=70 ℃和T₉₀=100 ℃；乙酸乙酯催化氧化T₅₀=160 ℃，T₉₀=200 ℃）。同时，Cu5/OL催化剂具有最佳的还原性能、氧移动性能和最多的Cu²⁺、（Mn²⁺+Mn³⁺）和表面吸附氧浓度。Cu_x/OL催化性能与铜锰之间相互作用、还原性和氧移动性能密切相关。

关键词:

English

Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing 100124, P. R. China
Received Date: 17 March 2017
Revised Date: 20 April 2017
Available Online: 28 April 2017
Fund Project:
The project was supported by the National Natural Science Foundation of China (21277008, 20777005) and Natural Science Foundation of Beijing, China (8082008) and Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality (IDHT20140504)

Abstract: Octahedral layered birnessite (denoted as OL) was synthesized by the oxidation-reduction method and a series of Cu_x/OL catalysts were prepared by the ion exchange method with various Cu loadings. The materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N₂ adsorption-desorption, hydrogen temperature-programmed reduction (H₂-TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric (TG) and.oxygen temperature-programmed desorption (O₂-TPD) techniques, and their catalytic activities for CO and ethyl acetate oxidation were evaluated. The results show that OL is a typical octahedral layered structure, and the doping of Cu hardly affects the structure of OL. Moreover, Cu_x/OL samples had different reducibility, oxygen mobility, and atomic ratio of Cu²⁺/CuO, (Mn²⁺+Mn³⁺)/Mn⁴⁺, and O_ads/O_latt after the addition of Cu to OL. Among the Cu_x/OL samples, the Cu₅/OL sample showed the best activity for the catalytic oxidation of CO and ethyl acetate (T₅₀=70 and T₉₀=100℃ for CO oxidation; T₅₀=160℃ and T₉₀=200℃ for ethyl acetate oxidation). Cu₅/OL showed the best reducibility, most isolated Cu²⁺ species, highest surface (Mn²⁺+Mn³⁺)/Mn⁴⁺ atomic ratio, highest chemisorbed oxygen species, and lowest O₂ desorption temperature. Hence, factors such as the strong interaction between copper and manganese, good reducibility, and oxygen mobility were responsible for the excellent catalytic activity of Cu₅/OL.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

English

Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

English

Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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