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Hydrogen Evolution of a Unique DNAzyme Composed of Cobalt-Protoporphyrin IX and G-Quadruplex DNA
Molecular hydrogen (H ) is a clean and renewable fuel that has garnered significant interest in the search for alternatives to fossil fuels. Here, we constructed an artificial DNAzyme composed of cobalt-protoporphyrin IX (CoPP) and G-quadruplex DNA, possessing a unique H O ligand between the CoPP an...
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| Published in: | ChemSusChem 2024-01, Vol.17 (1), p.e202301244-e202301244 |
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| Main Authors: | , , , , , , , , |
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| cites | cdi_FETCH-LOGICAL-c318t-fa90b5cea2dd0ce85c9905d6e0360b4d981b1d0c9ecf8a7bcc3db72d190b8d283 |
| container_end_page | e202301244 |
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| container_start_page | e202301244 |
| container_title | ChemSusChem |
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| creator | Cui, Yue Zhang, Li Liu, Jing Zhang, Taozhe Sugahara, Aya Momotake, Atsuya Yamamoto, Yasuhiko Mao, Zong-Wan Tai, Hulin |
| description | Molecular hydrogen (H
) is a clean and renewable fuel that has garnered significant interest in the search for alternatives to fossil fuels. Here, we constructed an artificial DNAzyme composed of cobalt-protoporphyrin IX (CoPP) and G-quadruplex DNA, possessing a unique H
O
ligand between the CoPP and G-quartet planes. We show for the first time that CoPP-DNAzyme catalyzes photo-induced H
production under anaerobic conditions with a turnover number (TON) of 1229 ± 51 over 12 h at pH 6.05 and 10 °C. Compared with free-CoPP, complexation with G-quadruplex DNA resulted in a 4.7-fold increase in H
production activity. The TON of the CoPP-DNAzyme revealed an optimal acid-base equilibrium with a pK
value of 7.60 ± 0.05, apparently originating from the equilibrium between Co(III)-H
and Co(I) states. Our results demonstrate that the H
O
ligand can augment and modulate the intrinsic catalytic activity of H
production catalysts. These systems pave the way to using DNAzymes for H
evolution in the direct conversion of solar energy to H
from water. |
| doi_str_mv | 10.1002/cssc.202301244 |
| format | article |
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) is a clean and renewable fuel that has garnered significant interest in the search for alternatives to fossil fuels. Here, we constructed an artificial DNAzyme composed of cobalt-protoporphyrin IX (CoPP) and G-quadruplex DNA, possessing a unique H
O
ligand between the CoPP and G-quartet planes. We show for the first time that CoPP-DNAzyme catalyzes photo-induced H
production under anaerobic conditions with a turnover number (TON) of 1229 ± 51 over 12 h at pH 6.05 and 10 °C. Compared with free-CoPP, complexation with G-quadruplex DNA resulted in a 4.7-fold increase in H
production activity. The TON of the CoPP-DNAzyme revealed an optimal acid-base equilibrium with a pK
value of 7.60 ± 0.05, apparently originating from the equilibrium between Co(III)-H
and Co(I) states. Our results demonstrate that the H
O
ligand can augment and modulate the intrinsic catalytic activity of H
production catalysts. These systems pave the way to using DNAzymes for H
evolution in the direct conversion of solar energy to H
from water.</description><identifier>ISSN: 1864-5631</identifier><identifier>EISSN: 1864-564X</identifier><identifier>DOI: 10.1002/cssc.202301244</identifier><identifier>PMID: 37681481</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Acid base equilibrium ; Alternative fuels ; Anaerobic conditions ; Catalytic activity ; Cobalt ; Direct conversion ; DNA ; DNA, Catalytic - metabolism ; G-Quadruplexes ; Hydrogen ; Hydrogen evolution ; Hydrogen production ; Ligands ; Solar energy conversion</subject><ispartof>ChemSusChem, 2024-01, Vol.17 (1), p.e202301244-e202301244</ispartof><rights>2023 Wiley-VCH GmbH.</rights><rights>2024 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c318t-fa90b5cea2dd0ce85c9905d6e0360b4d981b1d0c9ecf8a7bcc3db72d190b8d283</cites><orcidid>0000-0003-0844-1022</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37681481$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Cui, Yue</creatorcontrib><creatorcontrib>Zhang, Li</creatorcontrib><creatorcontrib>Liu, Jing</creatorcontrib><creatorcontrib>Zhang, Taozhe</creatorcontrib><creatorcontrib>Sugahara, Aya</creatorcontrib><creatorcontrib>Momotake, Atsuya</creatorcontrib><creatorcontrib>Yamamoto, Yasuhiko</creatorcontrib><creatorcontrib>Mao, Zong-Wan</creatorcontrib><creatorcontrib>Tai, Hulin</creatorcontrib><title>Hydrogen Evolution of a Unique DNAzyme Composed of Cobalt-Protoporphyrin IX and G-Quadruplex DNA</title><title>ChemSusChem</title><addtitle>ChemSusChem</addtitle><description>Molecular hydrogen (H
) is a clean and renewable fuel that has garnered significant interest in the search for alternatives to fossil fuels. Here, we constructed an artificial DNAzyme composed of cobalt-protoporphyrin IX (CoPP) and G-quadruplex DNA, possessing a unique H
O
ligand between the CoPP and G-quartet planes. We show for the first time that CoPP-DNAzyme catalyzes photo-induced H
production under anaerobic conditions with a turnover number (TON) of 1229 ± 51 over 12 h at pH 6.05 and 10 °C. Compared with free-CoPP, complexation with G-quadruplex DNA resulted in a 4.7-fold increase in H
production activity. The TON of the CoPP-DNAzyme revealed an optimal acid-base equilibrium with a pK
value of 7.60 ± 0.05, apparently originating from the equilibrium between Co(III)-H
and Co(I) states. Our results demonstrate that the H
O
ligand can augment and modulate the intrinsic catalytic activity of H
production catalysts. These systems pave the way to using DNAzymes for H
evolution in the direct conversion of solar energy to H
from water.</description><subject>Acid base equilibrium</subject><subject>Alternative fuels</subject><subject>Anaerobic conditions</subject><subject>Catalytic activity</subject><subject>Cobalt</subject><subject>Direct conversion</subject><subject>DNA</subject><subject>DNA, Catalytic - metabolism</subject><subject>G-Quadruplexes</subject><subject>Hydrogen</subject><subject>Hydrogen evolution</subject><subject>Hydrogen production</subject><subject>Ligands</subject><subject>Solar energy conversion</subject><issn>1864-5631</issn><issn>1864-564X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNpdkM9LwzAcxYMobk6vHiXgxUtnfrRpehxzboPhD3CwW02TVDvapiatWP96Wzd38PT9wvu8x-MBcInRGCNEbqVzckwQoQgT3z8CQ8yZ7wXM3xwffooH4My5LUIMRYydggENGcc-x0PwumiVNW-6hLNPkzd1ZkpoUijgusw-Gg3vHibfbaHh1BSVcVr14tQkIq-9J2tqUxlbvbc2K-FyA0Wp4Nx7boSyTZXrr959Dk5SkTt9sb8jsL6fvUwX3upxvpxOVp6kmNdeKiKUBFILohSSmgcyilCgmEaUocRXEccJ7pRIy5SLMJGSqiQkCnc2rginI3Czy62s6Yq7Oi4yJ3Wei1KbxsWEM0oRwSjq0Ot_6NY0tuzaxSTCBAck_A0c7yhpjXNWp3Fls0LYNsYo7reP--3jw_ad4Wof2ySFVgf8b2z6AyKLf3s</recordid><startdate>20240108</startdate><enddate>20240108</enddate><creator>Cui, Yue</creator><creator>Zhang, Li</creator><creator>Liu, Jing</creator><creator>Zhang, Taozhe</creator><creator>Sugahara, Aya</creator><creator>Momotake, Atsuya</creator><creator>Yamamoto, Yasuhiko</creator><creator>Mao, Zong-Wan</creator><creator>Tai, Hulin</creator><general>Wiley Subscription Services, Inc</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0003-0844-1022</orcidid></search><sort><creationdate>20240108</creationdate><title>Hydrogen Evolution of a Unique DNAzyme Composed of Cobalt-Protoporphyrin IX and G-Quadruplex DNA</title><author>Cui, Yue ; Zhang, Li ; Liu, Jing ; Zhang, Taozhe ; Sugahara, Aya ; Momotake, Atsuya ; Yamamoto, Yasuhiko ; Mao, Zong-Wan ; Tai, Hulin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c318t-fa90b5cea2dd0ce85c9905d6e0360b4d981b1d0c9ecf8a7bcc3db72d190b8d283</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Acid base equilibrium</topic><topic>Alternative fuels</topic><topic>Anaerobic conditions</topic><topic>Catalytic activity</topic><topic>Cobalt</topic><topic>Direct conversion</topic><topic>DNA</topic><topic>DNA, Catalytic - metabolism</topic><topic>G-Quadruplexes</topic><topic>Hydrogen</topic><topic>Hydrogen evolution</topic><topic>Hydrogen production</topic><topic>Ligands</topic><topic>Solar energy conversion</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cui, Yue</creatorcontrib><creatorcontrib>Zhang, Li</creatorcontrib><creatorcontrib>Liu, Jing</creatorcontrib><creatorcontrib>Zhang, Taozhe</creatorcontrib><creatorcontrib>Sugahara, Aya</creatorcontrib><creatorcontrib>Momotake, Atsuya</creatorcontrib><creatorcontrib>Yamamoto, Yasuhiko</creatorcontrib><creatorcontrib>Mao, Zong-Wan</creatorcontrib><creatorcontrib>Tai, Hulin</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>ChemSusChem</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Cui, Yue</au><au>Zhang, Li</au><au>Liu, Jing</au><au>Zhang, Taozhe</au><au>Sugahara, Aya</au><au>Momotake, Atsuya</au><au>Yamamoto, Yasuhiko</au><au>Mao, Zong-Wan</au><au>Tai, Hulin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Hydrogen Evolution of a Unique DNAzyme Composed of Cobalt-Protoporphyrin IX and G-Quadruplex DNA</atitle><jtitle>ChemSusChem</jtitle><addtitle>ChemSusChem</addtitle><date>2024-01-08</date><risdate>2024</risdate><volume>17</volume><issue>1</issue><spage>e202301244</spage><epage>e202301244</epage><pages>e202301244-e202301244</pages><issn>1864-5631</issn><eissn>1864-564X</eissn><abstract>Molecular hydrogen (H
) is a clean and renewable fuel that has garnered significant interest in the search for alternatives to fossil fuels. Here, we constructed an artificial DNAzyme composed of cobalt-protoporphyrin IX (CoPP) and G-quadruplex DNA, possessing a unique H
O
ligand between the CoPP and G-quartet planes. We show for the first time that CoPP-DNAzyme catalyzes photo-induced H
production under anaerobic conditions with a turnover number (TON) of 1229 ± 51 over 12 h at pH 6.05 and 10 °C. Compared with free-CoPP, complexation with G-quadruplex DNA resulted in a 4.7-fold increase in H
production activity. The TON of the CoPP-DNAzyme revealed an optimal acid-base equilibrium with a pK
value of 7.60 ± 0.05, apparently originating from the equilibrium between Co(III)-H
and Co(I) states. Our results demonstrate that the H
O
ligand can augment and modulate the intrinsic catalytic activity of H
production catalysts. These systems pave the way to using DNAzymes for H
evolution in the direct conversion of solar energy to H
from water.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>37681481</pmid><doi>10.1002/cssc.202301244</doi><orcidid>https://orcid.org/0000-0003-0844-1022</orcidid><oa>free_for_read</oa></addata></record> |
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| language | eng |
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| subjects | Acid base equilibrium Alternative fuels Anaerobic conditions Catalytic activity Cobalt Direct conversion DNA DNA, Catalytic - metabolism G-Quadruplexes Hydrogen Hydrogen evolution Hydrogen production Ligands Solar energy conversion |
| title | Hydrogen Evolution of a Unique DNAzyme Composed of Cobalt-Protoporphyrin IX and G-Quadruplex DNA |
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