Highly efficient bromine capture and storage using N-containing porous organic cages
Highly volatile and toxic bromine (Br 2 ) molecules can be utilized safely in various chemical processes when coupled with efficient separation systems. Herein, we present two different N-containing porous organic cages (POCs), covalent cage 3-R (CC3-R) and formaldehyde tied-reduced covalent cage 3...
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| Veröffentlicht in: | Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2022-11, Vol.1 (46), p.2482-24812 |
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| creator | Lee, Sunggyu Kevlishvili, Ilia Kulik, Heather J Kim, Hee-Tak Chung, Yongchul G Koh, Dong-Yeun |
| description | Highly volatile and toxic bromine (Br
2
) molecules can be utilized safely in various chemical processes when coupled with efficient separation systems. Herein, we present two different N-containing porous organic cages (POCs), covalent cage 3-R (CC3-R) and formaldehyde tied-reduced covalent cage 3 (FT-RCC3), for vapor Br
2
capture under ambient conditions. They show outstanding sorption capacities (11.02 mmol g
−1
and 11.64 mmol g
−1
, respectively) compared with previously reported adsorbents. Reversibility of the Br
2
sorption process has been elucidated experimentally and computationally by identifying bromine species adsorbed at POCs and calculating their binding energies. The strong charge-transfer interactions between adsorbed Br
2
and abundant N atomic sites of the host cages led to the dominant formation of polybromide species (Br
3
−
and Br
5
−
). Further host-guest interaction between POCs and polybromides determined the reversibility of the Br
2
sorption process-showing partially reversible (>70% recovery) behavior for CC3-R and irreversible ( |
| doi_str_mv | 10.1039/d2ta05420e |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_rsc_p</sourceid><recordid>TN_cdi_proquest_journals_2740821990</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2740821990</sourcerecordid><originalsourceid>FETCH-LOGICAL-c281t-1ad8f9477caff07d1fb73e73cff2ef34e5e275ff16523d703d93cca90bee7e223</originalsourceid><addsrcrecordid>eNpFkEFLAzEQRoMoWGov3oWAN2F1kuw2m2Op1QpFL_W8pNnJmtIma7J76L93a6XOZeaDNzPwCLll8MhAqKeadxqKnANekBGHAjKZq-nleS7LazJJaQtDlQBTpUZkvXTN1-5A0VpnHPqObmLYO4_U6LbrI1Lta5q6EHWDtE_ON_Q9M8F32vljaEMMfaIhNto7M2w1mG7IldW7hJO_PiafL4v1fJmtPl7f5rNVZnjJuozpurQql9Joa0HWzG6kQCmMtRytyLFALgtr2bTgopYgaiWM0Qo2iBI5F2Nyf7rbxvDdY-qqbeijH15WXOZQcqYUDNTDiTIxpBTRVm10ex0PFYPqKK565uvZr7jFAN-d4JjMmfsXK34AeEprFw</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2740821990</pqid></control><display><type>article</type><title>Highly efficient bromine capture and storage using N-containing porous organic cages</title><source>Royal Society Of Chemistry Journals 2008-</source><creator>Lee, Sunggyu ; Kevlishvili, Ilia ; Kulik, Heather J ; Kim, Hee-Tak ; Chung, Yongchul G ; Koh, Dong-Yeun</creator><creatorcontrib>Lee, Sunggyu ; Kevlishvili, Ilia ; Kulik, Heather J ; Kim, Hee-Tak ; Chung, Yongchul G ; Koh, Dong-Yeun</creatorcontrib><description>Highly volatile and toxic bromine (Br
2
) molecules can be utilized safely in various chemical processes when coupled with efficient separation systems. Herein, we present two different N-containing porous organic cages (POCs), covalent cage 3-R (CC3-R) and formaldehyde tied-reduced covalent cage 3 (FT-RCC3), for vapor Br
2
capture under ambient conditions. They show outstanding sorption capacities (11.02 mmol g
−1
and 11.64 mmol g
−1
, respectively) compared with previously reported adsorbents. Reversibility of the Br
2
sorption process has been elucidated experimentally and computationally by identifying bromine species adsorbed at POCs and calculating their binding energies. The strong charge-transfer interactions between adsorbed Br
2
and abundant N atomic sites of the host cages led to the dominant formation of polybromide species (Br
3
−
and Br
5
−
). Further host-guest interaction between POCs and polybromides determined the reversibility of the Br
2
sorption process-showing partially reversible (>70% recovery) behavior for CC3-R and irreversible (<10% recovery) behavior for FT-RCC3, both of which were affected by the chemical and structural nature of different POCs. DFT calculations further indicate that the formation of carbocationic species (Br
3
−
and Br
5
−
) and HBr is energetically favorable within the cage, which is in good agreement with the experimental results. This work demonstrates that strong host-guest interactions are essential for highly efficient Br
2
capture and storage performance.
Two distinct N-containing POCs show exceptional Br
2
vapor adsorption ability and different reversibility of adsorption by forming charge-transfer complexes with polybromide species, as demonstrated by experimental investigations and DFT calculations.</description><identifier>ISSN: 2050-7488</identifier><identifier>EISSN: 2050-7496</identifier><identifier>DOI: 10.1039/d2ta05420e</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Bromine ; Cages ; Charge transfer ; Chemical reactions ; Mathematical analysis ; Recovery ; Sorption</subject><ispartof>Journal of materials chemistry. A, Materials for energy and sustainability, 2022-11, Vol.1 (46), p.2482-24812</ispartof><rights>Copyright Royal Society of Chemistry 2022</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c281t-1ad8f9477caff07d1fb73e73cff2ef34e5e275ff16523d703d93cca90bee7e223</citedby><cites>FETCH-LOGICAL-c281t-1ad8f9477caff07d1fb73e73cff2ef34e5e275ff16523d703d93cca90bee7e223</cites><orcidid>0000-0001-9342-0191 ; 0000-0001-8133-4165 ; 0000-0003-4578-5422 ; 0000-0002-6049-9371 ; 0000-0001-9841-2529 ; 0000-0002-7756-0589</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,777,781,27905,27906</link.rule.ids></links><search><creatorcontrib>Lee, Sunggyu</creatorcontrib><creatorcontrib>Kevlishvili, Ilia</creatorcontrib><creatorcontrib>Kulik, Heather J</creatorcontrib><creatorcontrib>Kim, Hee-Tak</creatorcontrib><creatorcontrib>Chung, Yongchul G</creatorcontrib><creatorcontrib>Koh, Dong-Yeun</creatorcontrib><title>Highly efficient bromine capture and storage using N-containing porous organic cages</title><title>Journal of materials chemistry. A, Materials for energy and sustainability</title><description>Highly volatile and toxic bromine (Br
2
) molecules can be utilized safely in various chemical processes when coupled with efficient separation systems. Herein, we present two different N-containing porous organic cages (POCs), covalent cage 3-R (CC3-R) and formaldehyde tied-reduced covalent cage 3 (FT-RCC3), for vapor Br
2
capture under ambient conditions. They show outstanding sorption capacities (11.02 mmol g
−1
and 11.64 mmol g
−1
, respectively) compared with previously reported adsorbents. Reversibility of the Br
2
sorption process has been elucidated experimentally and computationally by identifying bromine species adsorbed at POCs and calculating their binding energies. The strong charge-transfer interactions between adsorbed Br
2
and abundant N atomic sites of the host cages led to the dominant formation of polybromide species (Br
3
−
and Br
5
−
). Further host-guest interaction between POCs and polybromides determined the reversibility of the Br
2
sorption process-showing partially reversible (>70% recovery) behavior for CC3-R and irreversible (<10% recovery) behavior for FT-RCC3, both of which were affected by the chemical and structural nature of different POCs. DFT calculations further indicate that the formation of carbocationic species (Br
3
−
and Br
5
−
) and HBr is energetically favorable within the cage, which is in good agreement with the experimental results. This work demonstrates that strong host-guest interactions are essential for highly efficient Br
2
capture and storage performance.
Two distinct N-containing POCs show exceptional Br
2
vapor adsorption ability and different reversibility of adsorption by forming charge-transfer complexes with polybromide species, as demonstrated by experimental investigations and DFT calculations.</description><subject>Bromine</subject><subject>Cages</subject><subject>Charge transfer</subject><subject>Chemical reactions</subject><subject>Mathematical analysis</subject><subject>Recovery</subject><subject>Sorption</subject><issn>2050-7488</issn><issn>2050-7496</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNpFkEFLAzEQRoMoWGov3oWAN2F1kuw2m2Op1QpFL_W8pNnJmtIma7J76L93a6XOZeaDNzPwCLll8MhAqKeadxqKnANekBGHAjKZq-nleS7LazJJaQtDlQBTpUZkvXTN1-5A0VpnHPqObmLYO4_U6LbrI1Lta5q6EHWDtE_ON_Q9M8F32vljaEMMfaIhNto7M2w1mG7IldW7hJO_PiafL4v1fJmtPl7f5rNVZnjJuozpurQql9Joa0HWzG6kQCmMtRytyLFALgtr2bTgopYgaiWM0Qo2iBI5F2Nyf7rbxvDdY-qqbeijH15WXOZQcqYUDNTDiTIxpBTRVm10ex0PFYPqKK565uvZr7jFAN-d4JjMmfsXK34AeEprFw</recordid><startdate>20221129</startdate><enddate>20221129</enddate><creator>Lee, Sunggyu</creator><creator>Kevlishvili, Ilia</creator><creator>Kulik, Heather J</creator><creator>Kim, Hee-Tak</creator><creator>Chung, Yongchul G</creator><creator>Koh, Dong-Yeun</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>JG9</scope><scope>L7M</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0001-9342-0191</orcidid><orcidid>https://orcid.org/0000-0001-8133-4165</orcidid><orcidid>https://orcid.org/0000-0003-4578-5422</orcidid><orcidid>https://orcid.org/0000-0002-6049-9371</orcidid><orcidid>https://orcid.org/0000-0001-9841-2529</orcidid><orcidid>https://orcid.org/0000-0002-7756-0589</orcidid></search><sort><creationdate>20221129</creationdate><title>Highly efficient bromine capture and storage using N-containing porous organic cages</title><author>Lee, Sunggyu ; Kevlishvili, Ilia ; Kulik, Heather J ; Kim, Hee-Tak ; Chung, Yongchul G ; Koh, Dong-Yeun</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c281t-1ad8f9477caff07d1fb73e73cff2ef34e5e275ff16523d703d93cca90bee7e223</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Bromine</topic><topic>Cages</topic><topic>Charge transfer</topic><topic>Chemical reactions</topic><topic>Mathematical analysis</topic><topic>Recovery</topic><topic>Sorption</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lee, Sunggyu</creatorcontrib><creatorcontrib>Kevlishvili, Ilia</creatorcontrib><creatorcontrib>Kulik, Heather J</creatorcontrib><creatorcontrib>Kim, Hee-Tak</creatorcontrib><creatorcontrib>Chung, Yongchul G</creatorcontrib><creatorcontrib>Koh, Dong-Yeun</creatorcontrib><collection>CrossRef</collection><collection>Electronics & Communications Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lee, Sunggyu</au><au>Kevlishvili, Ilia</au><au>Kulik, Heather J</au><au>Kim, Hee-Tak</au><au>Chung, Yongchul G</au><au>Koh, Dong-Yeun</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Highly efficient bromine capture and storage using N-containing porous organic cages</atitle><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle><date>2022-11-29</date><risdate>2022</risdate><volume>1</volume><issue>46</issue><spage>2482</spage><epage>24812</epage><pages>2482-24812</pages><issn>2050-7488</issn><eissn>2050-7496</eissn><abstract>Highly volatile and toxic bromine (Br
2
) molecules can be utilized safely in various chemical processes when coupled with efficient separation systems. Herein, we present two different N-containing porous organic cages (POCs), covalent cage 3-R (CC3-R) and formaldehyde tied-reduced covalent cage 3 (FT-RCC3), for vapor Br
2
capture under ambient conditions. They show outstanding sorption capacities (11.02 mmol g
−1
and 11.64 mmol g
−1
, respectively) compared with previously reported adsorbents. Reversibility of the Br
2
sorption process has been elucidated experimentally and computationally by identifying bromine species adsorbed at POCs and calculating their binding energies. The strong charge-transfer interactions between adsorbed Br
2
and abundant N atomic sites of the host cages led to the dominant formation of polybromide species (Br
3
−
and Br
5
−
). Further host-guest interaction between POCs and polybromides determined the reversibility of the Br
2
sorption process-showing partially reversible (>70% recovery) behavior for CC3-R and irreversible (<10% recovery) behavior for FT-RCC3, both of which were affected by the chemical and structural nature of different POCs. DFT calculations further indicate that the formation of carbocationic species (Br
3
−
and Br
5
−
) and HBr is energetically favorable within the cage, which is in good agreement with the experimental results. This work demonstrates that strong host-guest interactions are essential for highly efficient Br
2
capture and storage performance.
Two distinct N-containing POCs show exceptional Br
2
vapor adsorption ability and different reversibility of adsorption by forming charge-transfer complexes with polybromide species, as demonstrated by experimental investigations and DFT calculations.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d2ta05420e</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0001-9342-0191</orcidid><orcidid>https://orcid.org/0000-0001-8133-4165</orcidid><orcidid>https://orcid.org/0000-0003-4578-5422</orcidid><orcidid>https://orcid.org/0000-0002-6049-9371</orcidid><orcidid>https://orcid.org/0000-0001-9841-2529</orcidid><orcidid>https://orcid.org/0000-0002-7756-0589</orcidid></addata></record> |
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| identifier | ISSN: 2050-7488 |
| ispartof | Journal of materials chemistry. A, Materials for energy and sustainability, 2022-11, Vol.1 (46), p.2482-24812 |
| issn | 2050-7488 2050-7496 |
| language | eng |
| recordid | cdi_proquest_journals_2740821990 |
| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Bromine Cages Charge transfer Chemical reactions Mathematical analysis Recovery Sorption |
| title | Highly efficient bromine capture and storage using N-containing porous organic cages |
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