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Bimetallic nickel complexes containing imidazole-based phenolate ligands as efficient catalysts for the copolymerization of carbon dioxide with epoxides
The utilization of hexadentate imidazole-derived diamine-bisphenolate ligands to construct structurally well-defined bimetallic nickel catalysts that enable the mediation of the copolymerization of carbon dioxide with alicyclic epoxides was reported for the first time. A series of dinickel carboxyla...
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| Published in: | Dalton transactions : an international journal of inorganic chemistry 2023-12, Vol.53 (1), p.299-314 |
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| container_end_page | 314 |
| container_issue | 1 |
| container_start_page | 299 |
| container_title | Dalton transactions : an international journal of inorganic chemistry |
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| creator | Hsu, Han-Fang Liu, Guan-Lin Su, Yu-Chia Ko, Bao-Tsan |
| description | The utilization of hexadentate imidazole-derived diamine-bisphenolate ligands to construct structurally well-defined bimetallic nickel catalysts that enable the mediation of the copolymerization of carbon dioxide with alicyclic epoxides was reported for the first time. A series of dinickel carboxylate/nitrophenolate complexes were facilely prepared through a one-pot procedure and their structures were fully determined by single crystal X-ray structural analysis. Dinickel complexes
1-10
were used as single-component catalysts, and were evaluated for the copolymerization of CO
2
and cyclohexene oxide (CHO), for which acetato-incorporated complex
1
was proved to exhibit the best activity. Not only has the controllability of binickel catalyst
1
for CO
2
/CHO copolymerization been demonstrated, but also an "immortal" character for the same polymerization has been realized. Furthermore, detailed kinetic studies of polymerization catalysis of this type were undertaken, and the kinetics results revealed a first-order dependence on both Ni complex
1
and CHO concentrations. This is a successful example of the introduction of the easily accessible nitrogen-heterocycle group, the imidazole moiety, into phenolate ligands for the development of high-performance homogeneous catalysts towards the bimetallic complex-catalyzed copolymerization of CO
2
and epoxides.
In this study, a series of new structurally well-defined dinickel complexes containing imidazole-based diamine-bisphenolate ligands were found to effectively catalyze the ring-opening copolymerization (ROCOP) of CO
2
and cyclohexene oxide. |
| doi_str_mv | 10.1039/d3dt03084a |
| format | article |
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1-10
were used as single-component catalysts, and were evaluated for the copolymerization of CO
2
and cyclohexene oxide (CHO), for which acetato-incorporated complex
1
was proved to exhibit the best activity. Not only has the controllability of binickel catalyst
1
for CO
2
/CHO copolymerization been demonstrated, but also an "immortal" character for the same polymerization has been realized. Furthermore, detailed kinetic studies of polymerization catalysis of this type were undertaken, and the kinetics results revealed a first-order dependence on both Ni complex
1
and CHO concentrations. This is a successful example of the introduction of the easily accessible nitrogen-heterocycle group, the imidazole moiety, into phenolate ligands for the development of high-performance homogeneous catalysts towards the bimetallic complex-catalyzed copolymerization of CO
2
and epoxides.
In this study, a series of new structurally well-defined dinickel complexes containing imidazole-based diamine-bisphenolate ligands were found to effectively catalyze the ring-opening copolymerization (ROCOP) of CO
2
and cyclohexene oxide.</description><identifier>ISSN: 1477-9226</identifier><identifier>EISSN: 1477-9234</identifier><identifier>DOI: 10.1039/d3dt03084a</identifier><identifier>PMID: 38047477</identifier><language>eng</language><publisher>England: Royal Society of Chemistry</publisher><subject>Bimetals ; Carbon dioxide ; Catalysis ; Catalysts ; Copolymerization ; Diamines ; Imidazole ; Ligands ; Nickel ; Polymerization ; Single crystals ; Structural analysis</subject><ispartof>Dalton transactions : an international journal of inorganic chemistry, 2023-12, Vol.53 (1), p.299-314</ispartof><rights>Copyright Royal Society of Chemistry 2024</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c296t-f9ad856894e2cb5bc6ea07954a9a128f4b7444523e034afeb5c5a3a9b42dbd423</cites><orcidid>0000-0001-8404-6265</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,783,787,27936,27937</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38047477$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Hsu, Han-Fang</creatorcontrib><creatorcontrib>Liu, Guan-Lin</creatorcontrib><creatorcontrib>Su, Yu-Chia</creatorcontrib><creatorcontrib>Ko, Bao-Tsan</creatorcontrib><title>Bimetallic nickel complexes containing imidazole-based phenolate ligands as efficient catalysts for the copolymerization of carbon dioxide with epoxides</title><title>Dalton transactions : an international journal of inorganic chemistry</title><addtitle>Dalton Trans</addtitle><description>The utilization of hexadentate imidazole-derived diamine-bisphenolate ligands to construct structurally well-defined bimetallic nickel catalysts that enable the mediation of the copolymerization of carbon dioxide with alicyclic epoxides was reported for the first time. A series of dinickel carboxylate/nitrophenolate complexes were facilely prepared through a one-pot procedure and their structures were fully determined by single crystal X-ray structural analysis. Dinickel complexes
1-10
were used as single-component catalysts, and were evaluated for the copolymerization of CO
2
and cyclohexene oxide (CHO), for which acetato-incorporated complex
1
was proved to exhibit the best activity. Not only has the controllability of binickel catalyst
1
for CO
2
/CHO copolymerization been demonstrated, but also an "immortal" character for the same polymerization has been realized. Furthermore, detailed kinetic studies of polymerization catalysis of this type were undertaken, and the kinetics results revealed a first-order dependence on both Ni complex
1
and CHO concentrations. This is a successful example of the introduction of the easily accessible nitrogen-heterocycle group, the imidazole moiety, into phenolate ligands for the development of high-performance homogeneous catalysts towards the bimetallic complex-catalyzed copolymerization of CO
2
and epoxides.
In this study, a series of new structurally well-defined dinickel complexes containing imidazole-based diamine-bisphenolate ligands were found to effectively catalyze the ring-opening copolymerization (ROCOP) of CO
2
and cyclohexene oxide.</description><subject>Bimetals</subject><subject>Carbon dioxide</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Copolymerization</subject><subject>Diamines</subject><subject>Imidazole</subject><subject>Ligands</subject><subject>Nickel</subject><subject>Polymerization</subject><subject>Single crystals</subject><subject>Structural analysis</subject><issn>1477-9226</issn><issn>1477-9234</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpdkU1rFTEUhgex2FrduFcCbkSYmsnHncmytn4UCm7qejhJzvSmZpIxycXe_hJ_bmNvvYKr8x7Ow8uBp2ledfSko1x9sNwWyukg4Elz1Im-bxXj4uk-s9Vh8zznG0oZo5I9aw75QEVfj0fN749uxgLeO0OCMz_QExPnxeMt5ppCARdcuCZudhbuosdWQ0ZLljWG6KEg8e4ags0EMsFpcsZhKMRA7dzmkskUEylrrF1L9NsZk7uD4mIgcapU0jVZF2-dRfLLlTXB5WHJL5qDCXzGl4_zuPn--dPV2df28tuXi7PTy9YwtSrtpMAOcjUogcxoqc0KgfZKClDQsWESuhdCSMaRcgETamkkcFBaMKutYPy4ebfrXVL8ucFcxtllg95DwLjJIxtUL4aeclnRt_-hN3GTQv1uZIpyNkguu0q931EmxZwTTuOS3AxpO3Z0_ONrPOfnVw--Tiv85rFyo2e0e_SvoAq83gEpm_31n3B-DxUJneY</recordid><startdate>20231219</startdate><enddate>20231219</enddate><creator>Hsu, Han-Fang</creator><creator>Liu, Guan-Lin</creator><creator>Su, Yu-Chia</creator><creator>Ko, Bao-Tsan</creator><general>Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-8404-6265</orcidid></search><sort><creationdate>20231219</creationdate><title>Bimetallic nickel complexes containing imidazole-based phenolate ligands as efficient catalysts for the copolymerization of carbon dioxide with epoxides</title><author>Hsu, Han-Fang ; Liu, Guan-Lin ; Su, Yu-Chia ; Ko, Bao-Tsan</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c296t-f9ad856894e2cb5bc6ea07954a9a128f4b7444523e034afeb5c5a3a9b42dbd423</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Bimetals</topic><topic>Carbon dioxide</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Copolymerization</topic><topic>Diamines</topic><topic>Imidazole</topic><topic>Ligands</topic><topic>Nickel</topic><topic>Polymerization</topic><topic>Single crystals</topic><topic>Structural analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Hsu, Han-Fang</creatorcontrib><creatorcontrib>Liu, Guan-Lin</creatorcontrib><creatorcontrib>Su, Yu-Chia</creatorcontrib><creatorcontrib>Ko, Bao-Tsan</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Hsu, Han-Fang</au><au>Liu, Guan-Lin</au><au>Su, Yu-Chia</au><au>Ko, Bao-Tsan</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Bimetallic nickel complexes containing imidazole-based phenolate ligands as efficient catalysts for the copolymerization of carbon dioxide with epoxides</atitle><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle><addtitle>Dalton Trans</addtitle><date>2023-12-19</date><risdate>2023</risdate><volume>53</volume><issue>1</issue><spage>299</spage><epage>314</epage><pages>299-314</pages><issn>1477-9226</issn><eissn>1477-9234</eissn><abstract>The utilization of hexadentate imidazole-derived diamine-bisphenolate ligands to construct structurally well-defined bimetallic nickel catalysts that enable the mediation of the copolymerization of carbon dioxide with alicyclic epoxides was reported for the first time. A series of dinickel carboxylate/nitrophenolate complexes were facilely prepared through a one-pot procedure and their structures were fully determined by single crystal X-ray structural analysis. Dinickel complexes
1-10
were used as single-component catalysts, and were evaluated for the copolymerization of CO
2
and cyclohexene oxide (CHO), for which acetato-incorporated complex
1
was proved to exhibit the best activity. Not only has the controllability of binickel catalyst
1
for CO
2
/CHO copolymerization been demonstrated, but also an "immortal" character for the same polymerization has been realized. Furthermore, detailed kinetic studies of polymerization catalysis of this type were undertaken, and the kinetics results revealed a first-order dependence on both Ni complex
1
and CHO concentrations. This is a successful example of the introduction of the easily accessible nitrogen-heterocycle group, the imidazole moiety, into phenolate ligands for the development of high-performance homogeneous catalysts towards the bimetallic complex-catalyzed copolymerization of CO
2
and epoxides.
In this study, a series of new structurally well-defined dinickel complexes containing imidazole-based diamine-bisphenolate ligands were found to effectively catalyze the ring-opening copolymerization (ROCOP) of CO
2
and cyclohexene oxide.</abstract><cop>England</cop><pub>Royal Society of Chemistry</pub><pmid>38047477</pmid><doi>10.1039/d3dt03084a</doi><tpages>16</tpages><orcidid>https://orcid.org/0000-0001-8404-6265</orcidid></addata></record> |
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| identifier | ISSN: 1477-9226 |
| ispartof | Dalton transactions : an international journal of inorganic chemistry, 2023-12, Vol.53 (1), p.299-314 |
| issn | 1477-9226 1477-9234 |
| language | eng |
| recordid | cdi_proquest_miscellaneous_2897487035 |
| source | Royal Society of Chemistry:Jisc Collections:Royal Society of Chemistry Read and Publish 2022-2024 (reading list) |
| subjects | Bimetals Carbon dioxide Catalysis Catalysts Copolymerization Diamines Imidazole Ligands Nickel Polymerization Single crystals Structural analysis |
| title | Bimetallic nickel complexes containing imidazole-based phenolate ligands as efficient catalysts for the copolymerization of carbon dioxide with epoxides |
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