Article(id=1319232635239518428, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319232566922695375, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20220088, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1643299200000, receivedDateStr=2022-01-28, revisedDate=1646236800000, revisedDateStr=2022-03-03, acceptedDate=null, acceptedDateStr=null, onlineDate=1792459170397, onlineDateStr=2026-10-20, pubDate=1658246400000, pubDateStr=2022-07-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792459170397, onlineIssueDateStr=2026-10-20, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792459170397, creator=13701087609, updateTime=1792459170397, updator=13701087609, issue=Issue{id=1319232566922695375, tenantId=1146029695717560320, journalId=1263187385517883426, year='2022', volume='50', issue='7', pageStart='1775', pageEnd='2066', issueExtLink='null', onlineDate='null', pubDate='1658246400000', pubDateStr='2022-07-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792459154109, creator='13701087609', updateTime=1792460038980, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319236278420357264, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319232566922695375, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319236278420357265, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319232566922695375, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=1955, endPage=1963, ext={EN=ArticleExt(id=1319232636879491293, articleId=1319232635239518428, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Effect of Oxalic Acid Treatment on Mordenite Structure and Catalytic Performance of Dimethyl Ether Carbonylation, columnId=1263922769897599102, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Articles, runingTitle=null, highlight=null, articleAbstract=

Mordenite is highly active for the carbonylation of dimethyl ether reaction, and the regulation of its acid sites is an effective way to improve its catalytic performance. In this paper, a series of mordenite was subjected to the post-treatment of oxalic acid solution. The changes in the structure and acid sites were characterized by X-ray diffraction, N2 adsorption-desorption, scanning electron microscopy, NH3-temperature-programmed desorption and Py-infrared spectroscopy, respectively. The results show that the overall relative crystallinity and crystal phase of mordenite remain stable. However, the acid wash post-treatment can effectively remove parts of the acid sites through "etching" or complexation, especially those located in the twelve-membered ring channels. Meanwhile, it can create a certain amount of mesopores inside the particles, leading to an increase of the mesopore volume. The catalytic test results of dimethyl ether carbonylation reaction indicate that the sample treated with a suitable concentration of oxalic acid solution can effectively improve the dimethyl ether carbonylation activity. The dimethyl ether conversion significantly increases, despite the methyl acetate selectivity only slightly decreases. However, parts of the active sites responsible for the carbonylation reaction are removed when treated with high-concentration oxalic acid solution, resulting in a decrease in the catalytic activity. This research provides a simple and effective method for the regulation of the acid sites in mordenite and the improvement of its dimethyl ether carbonylation activity.

, authors=Xiaosheng WANG1, Shaoduo LIU1, Tao YANG1, Ranjia LI1, Changchun YU1, Yuxiang LIU2, Zhengqiu XIE3, Yongqiang WANG3, Xiaojiao LI4, 5, authorsList=Xiaosheng WANG, Shaoduo LIU, Tao YANG, Ranjia LI, Changchun YU, Yuxiang LIU, Zhengqiu XIE, Yongqiang WANG, Xiaojiao LI, authorCompany=null, correspAuthors=Changchun YU, Yuxiang LIU, authorNote=

WANG Xiaosheng(1988-), male, Ph.D., Lecturer. E-mail:

, correspAuthorsNote=
YU Changchun (1969-), male, Ph.D., Associate Professor; E-mail:
LIU Yuxiang (1989-), male, Ph.D., Associate Professor.
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丝光沸石是二甲醚羰基化反应的高活性催化剂,通过对其酸中心进行调控是进一步提高其催化性能的有效方法。采用不同浓度的草酸溶液对丝光沸石进行了酸处理,通过X射线粉末衍射、N2吸附-脱附、扫描电子显微镜、氨气-程序升温脱附、吡啶-红外等技术手段对草酸处理前后丝光沸石结构及酸中心的变化进行了表征。结果表明:草酸处理对丝光沸石的相对结晶度、晶型影响较小,但能够通过“蚀刻”或络合作用有效脱除部分酸中心,尤其是优先脱除十二元环孔道中的酸中心,同时能够在颗粒中制造出部分介孔、提升丝光沸石的介孔孔容。适当浓度的草酸处理能够有效提高丝光沸石的二甲醚羰基化反应活性,二甲醚转化率明显升高,乙酸甲酯选择性仅略有下降。草酸浓度过高时会脱除部分羰基化反应的活性中心,从而导致催化活性的降低。为丝光沸石的酸中心调控及其二甲醚羰基化反应活性的提高提供了简单有效的方法。

, authors=王晓胜1, 刘少铎1, 杨韬1, 李然家1, 余长春1, 刘毓翔2, 谢正求3, 王永强3, 李晓娇4, 5, authorsList=王晓胜, 刘少铎, 杨韬, 李然家, 余长春, 刘毓翔, 谢正求, 王永强, 李晓娇, authorCompany=null, correspAuthors=余长春, 刘毓翔, authorNote=

王晓胜(1988—),男,博士,讲师。

, correspAuthorsNote=
余长春(1969—),男,博士,副教授。
刘毓翔(1989—),男,博士,副教授。
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草酸处理对丝光沸石催化二甲醚羰化反应性能的影响
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王晓胜 1 , 刘少铎 1 , 杨韬 1 , 李然家 1 , 余长春 1 , 刘毓翔 2 , 谢正求 3 , 王永强 3 , 李晓娇 4, 5
硅酸盐学报 | 研究论文 2022,50(7): 1955-1963
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硅酸盐学报 |研究论文 2022 , 50 (7) : 1955 -1963
草酸处理对丝光沸石催化二甲醚羰化反应性能的影响
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王晓胜1 , 刘少铎1, 杨韬1, 李然家1, 余长春1 , 刘毓翔2 , 谢正求3, 王永强3, 李晓娇4, 5
作者信息
  • 1.中国石油大学(北京)新能源与材料学院,北京 102249
  • 2.青岛科技大学化学工程学院,山东 青岛 266042
  • 3.岳阳聚成化工有限公司,湖南 岳阳 414009
  • 4.中国石油化工股份有限公司炼油事业部,北京 100327
  • 5.中国石油大学(北京)经济管理学院,北京 102249
通讯作者:
余长春(1969—),男,博士,副教授。
刘毓翔(1989—),男,博士,副教授。
作者简介:

王晓胜(1988—),男,博士,讲师。

Effect of Oxalic Acid Treatment on Mordenite Structure and Catalytic Performance of Dimethyl Ether Carbonylation
Xiaosheng WANG1 , Shaoduo LIU1, Tao YANG1, Ranjia LI1, Changchun YU1 , Yuxiang LIU2 , Zhengqiu XIE3, Yongqiang WANG3, Xiaojiao LI4, 5
Affiliations
  • 1.College of New Energy and Materials, China University of Petroleum-Beijing, Beijing 102249, China
  • 2.College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
  • 3.Yueyang Jucheng Chemical Co. Ltd., Yueyang 414409, Hunan, China
  • 4.Refining Department, China Petroleum and Chemical Corporation, Beijing 100327, China
  • 5.College of Economics and Management, China University of Petroleum-Beijing, Beijing 102249, China
  • Corresponding Author:
    YU Changchun (1969-), male, Ph.D., Associate Professor; E-mail:
    LIU Yuxiang (1989-), male, Ph.D., Associate Professor.

    WANG Xiaosheng(1988-), male, Ph.D., Lecturer. E-mail:

出版时间: 2022-07-20 doi: 10.14062/j.issn.0454-5648.20220088
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丝光沸石是二甲醚羰基化反应的高活性催化剂,通过对其酸中心进行调控是进一步提高其催化性能的有效方法。采用不同浓度的草酸溶液对丝光沸石进行了酸处理,通过X射线粉末衍射、N2吸附-脱附、扫描电子显微镜、氨气-程序升温脱附、吡啶-红外等技术手段对草酸处理前后丝光沸石结构及酸中心的变化进行了表征。结果表明:草酸处理对丝光沸石的相对结晶度、晶型影响较小,但能够通过“蚀刻”或络合作用有效脱除部分酸中心,尤其是优先脱除十二元环孔道中的酸中心,同时能够在颗粒中制造出部分介孔、提升丝光沸石的介孔孔容。适当浓度的草酸处理能够有效提高丝光沸石的二甲醚羰基化反应活性,二甲醚转化率明显升高,乙酸甲酯选择性仅略有下降。草酸浓度过高时会脱除部分羰基化反应的活性中心,从而导致催化活性的降低。为丝光沸石的酸中心调控及其二甲醚羰基化反应活性的提高提供了简单有效的方法。

酸处理  /  丝光沸石  /  二甲醚  /  羰基化

Mordenite is highly active for the carbonylation of dimethyl ether reaction, and the regulation of its acid sites is an effective way to improve its catalytic performance. In this paper, a series of mordenite was subjected to the post-treatment of oxalic acid solution. The changes in the structure and acid sites were characterized by X-ray diffraction, N2 adsorption-desorption, scanning electron microscopy, NH3-temperature-programmed desorption and Py-infrared spectroscopy, respectively. The results show that the overall relative crystallinity and crystal phase of mordenite remain stable. However, the acid wash post-treatment can effectively remove parts of the acid sites through "etching" or complexation, especially those located in the twelve-membered ring channels. Meanwhile, it can create a certain amount of mesopores inside the particles, leading to an increase of the mesopore volume. The catalytic test results of dimethyl ether carbonylation reaction indicate that the sample treated with a suitable concentration of oxalic acid solution can effectively improve the dimethyl ether carbonylation activity. The dimethyl ether conversion significantly increases, despite the methyl acetate selectivity only slightly decreases. However, parts of the active sites responsible for the carbonylation reaction are removed when treated with high-concentration oxalic acid solution, resulting in a decrease in the catalytic activity. This research provides a simple and effective method for the regulation of the acid sites in mordenite and the improvement of its dimethyl ether carbonylation activity.

acid treatment  /  mordenite  /  dimethyl ether  /  carbonylation
王晓胜, 刘少铎, 杨韬, 李然家, 余长春, 刘毓翔, 谢正求, 王永强, 李晓娇. 草酸处理对丝光沸石催化二甲醚羰化反应性能的影响. 硅酸盐学报, 2022 , 50 (7) : 1955 -1963 . DOI: 10.14062/j.issn.0454-5648.20220088
Xiaosheng WANG, Shaoduo LIU, Tao YANG, Ranjia LI, Changchun YU, Yuxiang LIU, Zhengqiu XIE, Yongqiang WANG, Xiaojiao LI. Effect of Oxalic Acid Treatment on Mordenite Structure and Catalytic Performance of Dimethyl Ether Carbonylation[J]. Journal of the Chinese Ceramic Society, 2022 , 50 (7) : 1955 -1963 . DOI: 10.14062/j.issn.0454-5648.20220088
  • 国家自然科学基金(22008260)
  • 中国石油大学(北京)科研基金资助(2462021YJRC011)
  • 中国石油天然气集团有限公司-中国石油大学(北京)战略合作科技专项(ZLZX2020-04)
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2022年第50卷第7期
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doi: 10.14062/j.issn.0454-5648.20220088
  • 接收时间:2022-01-28
  • 首发时间:2026-10-20
  • 出版时间:2022-07-20
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  • 收稿日期:2022-01-28
  • 修回日期:2022-03-03
基金
国家自然科学基金(22008260)
中国石油大学(北京)科研基金资助(2462021YJRC011)
中国石油天然气集团有限公司-中国石油大学(北京)战略合作科技专项(ZLZX2020-04)
作者信息
    1.中国石油大学(北京)新能源与材料学院,北京 102249
    2.青岛科技大学化学工程学院,山东 青岛 266042
    3.岳阳聚成化工有限公司,湖南 岳阳 414009
    4.中国石油化工股份有限公司炼油事业部,北京 100327
    5.中国石油大学(北京)经济管理学院,北京 102249

通讯作者:

余长春(1969—),男,博士,副教授。
刘毓翔(1989—),男,博士,副教授。
参考文献
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2种不同金属材料的力学参数
科
Family
属数
Number of
genus
种数
Number of
species
占总种数比例
Percentage of
total species (%)
属
Genus
种数
Number of
species
占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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