Characterization of CuO(y)/CuxCe1-xOδ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene

doi:10.16085/j.issn.1000-6613.2020-0315

Chemical Industry and Engineering Progress ›› 2020, Vol. 39 ›› Issue (12): 5104-5111.DOI: 10.16085/j.issn.1000-6613.2020-0315

• Industrial catalysis • Previous Articles Next Articles

Characterization of CuO(y)/Cu_xCe_1-_xO_δ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene

Huijie GU¹^,²(), Lei LI³^,⁴, Liping YE¹^,²^,⁴(), He HUANG³^,⁴, Yong LUO¹^,²^,⁴, Zhengwei JIN³^,⁴

^1.State Key Laboratory of Polyolefins and Catalysis, Shanghai 200062, China
^2.Shanghai Research Institute of Chemical Industry Co. , Ltd. , Shanghai 200062, China
^3.Institute of Coal Chemical Industry Technology, Ningxia Coal Industry Co. , Ltd. , CHN Energy Group, Yinchuan 750411, Ningxia, China
^4.Innovation Centre of Synergetic Technology of Coal-based Value-added Synthetic Resin Industry, Yinchuan 750411, Ningxia, China

Online:2020-12-02 Published:2020-12-05
Contact: Liping YE

低温深度脱除液相丙烯中微量CO的CuO(y)/Cu_xCe_1-_xO_δ催化剂表征分析及性能实验

顾慧劼¹^,²(), 李磊³^,⁴, 叶丽萍¹^,²^,⁴(), 黄河³^,⁴, 罗勇¹^,²^,⁴, 金政伟³^,⁴

^1.聚烯烃催化技术与高性能材料国家重点实验室，上海 200062
^2.上海化工研究院有限公司，上海 200062
^3.国家能源集团宁夏煤业有限责任公司煤炭化学工业技术研究院，宁夏银川 750411
^4.宁夏煤基合成树脂高值化产业技术协同创新中心，宁夏银川 750411

通讯作者: 叶丽萍
作者简介:顾慧劼（1990—），女，硕士，研究方向为工业催化净化。E-mail：ghjmianyang@126.com。
基金资助:
上海人才发展资金(2018019);宁夏煤基合成树脂高值化产业技术协同创新中心(2017DC57)

Abstract

Abstract:

Three CuO(y)/Cu_xCe_1-_xO_δcatalysts with different compositions were prepared and evaluated for the removal of trace CO in liquid-phase propylene at low temperature. The effects of the surface Cu species and Cu_xCe_1-_xO_δsolid solution on the structure, redox ability, surface state and CO oxidation activity were investigated, aiming to gain guide for further modification of the catalysts and finally to realize the industrial application. The catalysts were characterized by XRD, TEM, XPS, H₂-TPR, CO-TPD, etc. which showed that in the carrier Cu_xCe_1-_xO_δprepared by citric acid complexation, the copper particles could enter into the crystal lattice of cerium oxide, which enhanced the reducibility of the catalyst for oxygen activation. And the catalyst improved by impregnation method on this carrier, had more reduced and highly dispersed Cu species on the surface, which was beneficial to the chemisorption of CO. Therefore, the CO oxidation was promoted by the synergistic interaction. CuO(0.40)/Cu_0.1Ce_0.9O_δ_{exhibited the highest activity for CO conversion. Under the conditions of 50℃, LHSV=8h^-1 and 3.0MPa, the volume fraction of CO in liquid propylene decreased from 1.0×10^-5 to 2.65±0.27×10^-8 with good stability, which met the requirements of "polymer grade" propylene.}

Key words: catalyst, support, adsorption, carbon monoxide, deep removal, liquid propylene

摘要：

采用柠檬酸络合-浸渍的方法制备了CuO(y)/Cu_xCe_1-_xO_δ催化剂，重点研究了CuO的载体掺杂和表面负载对催化剂结构性质、氧化还原性能、吸附性能及CO净化性能等的影响，旨在指导催化剂进一步改性，实现低温下深度脱除液相丙烯中微量CO的工业化应用。采用X射线衍射（XRD）、透射电镜（TEM）、X射线光电子能谱分析仪（XPS）、拉曼光谱仪（Raman）和程序升温化学吸附仪（H₂-TPR、CO-TPD）等手段表征了催化剂的结构和性质，结果显示，CuO掺杂的载体，Cu进入CeO₂晶体形成固溶体，有利于催化剂氧化还原性能；浸渍法负载CuO制得的催化剂，表面具有更多的还原态、高分散的Cu物种，有利于表面对CO吸附性能；两者协同作用共同促进了CO催化氧化性能的提升。CuO(0.40)/Cu_0.1Ce_0.9O_δ催化剂具有优异的CO净化性能，在50℃、3.0MPa的工况条件下，可将液相丙烯中CO体积分数从1×10^-5脱除至2.65±0.27×10^-8，达到聚合级烯烃对CO脱除深度的要求，稳定性能良好。

关键词: 催化剂, 载体, 吸附作用, 一氧化碳, 深度脱除, 液相丙烯

CLC Number:

TQ032.41

Huijie GU, Lei LI, Liping YE, He HUANG, Yong LUO, Zhengwei JIN. Characterization of CuO(y)/Cu_xCe_1-_xO_δ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene[J]. Chemical Industry and Engineering Progress, 2020, 39(12): 5104-5111.

顾慧劼, 李磊, 叶丽萍, 黄河, 罗勇, 金政伟. 低温深度脱除液相丙烯中微量CO的CuO(y)/Cu_xCe_1-_xO_δ催化剂表征分析及性能实验[J]. 化工进展, 2020, 39(12): 5104-5111.

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Characterization of CuO(y)/Cu_xCe_1-_xO_δ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene

低温深度脱除液相丙烯中微量CO的CuO(y)/Cu_xCe_1-_xO_δ催化剂表征分析及性能实验

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Characterization of CuO(y)/CuxCe1-xOδ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene

低温深度脱除液相丙烯中微量CO的CuO(y)/CuxCe1-xOδ催化剂表征分析及性能实验

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Characterization of CuO(y)/Cu_xCe_1-_xO_δ mixed-oxide catalysts and their performance in deep removal of trace amount of CO in liquid-phase propylene

低温深度脱除液相丙烯中微量CO的CuO(y)/Cu_xCe_1-_xO_δ催化剂表征分析及性能实验