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The Immobilization of Pd(II) on Porous Organic Polymers for Semihydrogenation of Terminal Alkynes

文献类型：期刊论文

作者Liu, Jianguo1,2,3,4; Wang, Nan1,2,3,5; Liu, Jianan1,2,3; Li, Ming1,2,3; Xu, Ying1,2,3; Wang, Chenguang1,2,3; Wang, Yanzhi6; Zheng, Haoquan6; Ma, Longlong1,2,3,5
刊名ACS APPLIED MATERIALS & INTERFACES
出版日期2020-11-18
卷号12期号:46页码:51428-51436
ISSN号1944-8244
关键词porous organic polymers facile synthesis Pd catalysis semihydrogenation terminal alkynes
DOI10.1021/acsami.0c14486
通讯作者Ma, Longlong(mall@ms.giec.ac.cn)
英文摘要Highly selective catalytic hydrogenation of alkynes to alkenes is a highly important reaction owing to its industrial and commercial application. Specifically, semi-hydrogenation of terminal alkynes has been more challenging than internal alkenes even using Lindlar catalysts. Also, the high reduction degree state metal-supported catalysts like Pd-0/C, Pt-0/C, and Ru-0/C have been well-known to be used widely in hydrogenation due to their super activity. However, charcoal can absorb a large amount of water; Pd/C with 50% water is convenient on a large-scale synthesis. Charcoal generally bears oxygen groups on its surface, which are responsible for low selectivity and undesired products. Even typically, only 10-60% of the Pd metal atoms are exposed, they still suffer from poor stability in acids owing to leaching. Herein, we intend to design active and stable metal catalysts with features as the following to avoid leaching: having strong interaction with the support and coordinatively unsaturated metal sites or low valence state metals physically isolated from the acid environment. Herein, a highly efficient semihydrogenation of terminal alkynes to produce alkenes has been realized using a heterogeneous Pd(II)/POP-GIEC catalyst, imine-linked, crystalline, and porous organic polymer supporter modified by coordination of Pd(OAc)(2) to its walls under mild conditions. Surprisingly, for the first time, modified POP-supported low reduction degree Pd" catalysts were synthesized efficiently, and they were successfully used in semihydrogenation of terminal allcynes. The substrate scope was studied and included both unfunctionalized as well as functionalized substituents on the para, ortho, and meta position of aromatic alkynes. The substrate having a substituent with the functionality of fluoro protected at the meta position was semihydrogenated with a high alkyne conversion of 100% and olefin selectivity (up to 99 %) .
资助项目National Natural Science Foundation of China[51976225] ; Dalian National Laboratory Cooperation Foundation, Chinese Academy of Sciences[DNL201916]
WOS研究方向Science & Technology - Other Topics ; Materials Science
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000592923100027
资助机构National Natural Science Foundation of China ; Dalian National Laboratory Cooperation Foundation, Chinese Academy of Sciences
源URL[http://ir.giec.ac.cn/handle/344007/32513]  
专题中国科学院广州能源研究所
通讯作者Ma, Longlong
作者单位1.Chinese Acad Sci, Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
3.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China
4.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
5.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China
6.Shaanxi Normal Univ, Sch Chem & Chem Engn, Xian 710062, Peoples R China
推荐引用方式
GB/T 7714		 Liu, Jianguo,Wang, Nan,Liu, Jianan,et al. The Immobilization of Pd(II) on Porous Organic Polymers for Semihydrogenation of Terminal Alkynes[J]. ACS APPLIED MATERIALS & INTERFACES,2020,12(46):51428-51436.
APA Liu, Jianguo.,Wang, Nan.,Liu, Jianan.,Li, Ming.,Xu, Ying.,...&Ma, Longlong.(2020).The Immobilization of Pd(II) on Porous Organic Polymers for Semihydrogenation of Terminal Alkynes.ACS APPLIED MATERIALS & INTERFACES,12(46),51428-51436.
MLA Liu, Jianguo,et al."The Immobilization of Pd(II) on Porous Organic Polymers for Semihydrogenation of Terminal Alkynes".ACS APPLIED MATERIALS & INTERFACES 12.46(2020):51428-51436.

入库方式： OAI收割

来源：广州能源研究所

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