Delocalization Engineering of Heme‐Mimetic Artificial Enzymes for Augmented Reactive Oxygen Catalysis
Developing artificial enzymes based on organic molecules or polymers for reactive oxygen species (ROS)‐related catalysis has broad applicability. Herein, inspired by porphyrin‐based heme mimics, we report the synthesis of polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) as a new porphyrin‐ev...
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| creator | Li, Qian Zhao, Zhenyang Chen, Fan Xu, Xiaohui Xu, Lizhi Cheng, Liang Adeli, Mohsen Luo, Xianglin Cheng, Chong |
| description | Developing artificial enzymes based on organic molecules or polymers for reactive oxygen species (ROS)‐related catalysis has broad applicability. Herein, inspired by porphyrin‐based heme mimics, we report the synthesis of polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) as a new porphyrin‐evolving structure to serve as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to the structural advantages, such as enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS‐production activity in terms of Vmax and turnover numbers as compared with porphyrin‐based conjugated polymers (Fe‐PPor‐AE), which also surpassed reported state‐of‐the‐art artificial enzymes in their activity. More interestingly, by changing the reaction medium and substrates, Fe‐PPc‐AE also revealed significantly improved activity and environmental adaptivity in many other ROS‐related biocatalytic processes, validating the potential of Fe‐PPc‐AE to replace conventional (poly)porphyrin‐based heme mimics for ROS‐related catalysis, biosensors, or biotherapeutics. It is suggested that this study will offer essential guidance for designing artificial enzymes based on organic molecules or polymers.
Inspired by porphyrin‐based heme mimics, polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) were synthesized as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS production even than the reported state‐of‐the‐art biocatalysts. |
| doi_str_mv | 10.1002/anie.202400838 |
| format | Article |
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Inspired by porphyrin‐based heme mimics, polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) were synthesized as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS production even than the reported state‐of‐the‐art biocatalysts.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>ISSN: 1521-3773</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202400838</identifier><identifier>PMID: 38372011</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>artificial enzymes ; biocatalysts ; Biosensors ; Catalysis ; Chemical synthesis ; Conjugation ; Electron transfer ; Enzymes ; Heme ; Heme - chemistry ; heme-mimetic materials ; Organic chemistry ; Oxygen ; Oxygen - chemistry ; peroxidase-like activity ; Polymers ; Porphyrins ; Porphyrins - chemistry ; Reactive Oxygen Species ; Substrates</subject><ispartof>Angewandte Chemie International Edition, 2024-04, Vol.63 (15), p.e202400838-n/a</ispartof><rights>2024 Wiley‐VCH GmbH</rights><rights>2024 Wiley‐VCH GmbH.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3738-e1efb9bb8bb6b241f78bc27d2980dad1cb240cef39fd5122a1a9d974870be1713</citedby><cites>FETCH-LOGICAL-c3738-e1efb9bb8bb6b241f78bc27d2980dad1cb240cef39fd5122a1a9d974870be1713</cites><orcidid>0000-0002-6872-2240 ; 0000-0003-3328-1147</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.202400838$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202400838$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,776,780,1411,27901,27902,45550,45551</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38372011$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Li, Qian</creatorcontrib><creatorcontrib>Zhao, Zhenyang</creatorcontrib><creatorcontrib>Chen, Fan</creatorcontrib><creatorcontrib>Xu, Xiaohui</creatorcontrib><creatorcontrib>Xu, Lizhi</creatorcontrib><creatorcontrib>Cheng, Liang</creatorcontrib><creatorcontrib>Adeli, Mohsen</creatorcontrib><creatorcontrib>Luo, Xianglin</creatorcontrib><creatorcontrib>Cheng, Chong</creatorcontrib><title>Delocalization Engineering of Heme‐Mimetic Artificial Enzymes for Augmented Reactive Oxygen Catalysis</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Developing artificial enzymes based on organic molecules or polymers for reactive oxygen species (ROS)‐related catalysis has broad applicability. Herein, inspired by porphyrin‐based heme mimics, we report the synthesis of polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) as a new porphyrin‐evolving structure to serve as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to the structural advantages, such as enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS‐production activity in terms of Vmax and turnover numbers as compared with porphyrin‐based conjugated polymers (Fe‐PPor‐AE), which also surpassed reported state‐of‐the‐art artificial enzymes in their activity. More interestingly, by changing the reaction medium and substrates, Fe‐PPc‐AE also revealed significantly improved activity and environmental adaptivity in many other ROS‐related biocatalytic processes, validating the potential of Fe‐PPc‐AE to replace conventional (poly)porphyrin‐based heme mimics for ROS‐related catalysis, biosensors, or biotherapeutics. It is suggested that this study will offer essential guidance for designing artificial enzymes based on organic molecules or polymers.
Inspired by porphyrin‐based heme mimics, polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) were synthesized as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS production even than the reported state‐of‐the‐art biocatalysts.</description><subject>artificial enzymes</subject><subject>biocatalysts</subject><subject>Biosensors</subject><subject>Catalysis</subject><subject>Chemical synthesis</subject><subject>Conjugation</subject><subject>Electron transfer</subject><subject>Enzymes</subject><subject>Heme</subject><subject>Heme - chemistry</subject><subject>heme-mimetic materials</subject><subject>Organic chemistry</subject><subject>Oxygen</subject><subject>Oxygen - chemistry</subject><subject>peroxidase-like activity</subject><subject>Polymers</subject><subject>Porphyrins</subject><subject>Porphyrins - chemistry</subject><subject>Reactive Oxygen Species</subject><subject>Substrates</subject><issn>1433-7851</issn><issn>1521-3773</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqF0UFvFCEYBmBiNLZWrx4NiRcvs_LB7MIcN-tqm1SbGD0TYD4mNDNMhRl1eupP6G_0l0iztSZevAAhD2--8BLyEtgKGONvTQy44ozXjCmhHpFjWHOohJTicTnXQlRSreGIPMv5snil2OYpORJKSM4Ajkn3DvvRmT5cmymMke5jFyJiCrGjo6enOOCvm9uPYcApOLpNU_DBBdMXeL0MmKkfE93O3YBxwpZ-RuOm8B3pxc-lw0h3ZjL9kkN-Tp5402d8cb-fkK_v9192p9X5xYez3fa8ckIKVSGgt421ytqN5TV4qazjsuWNYq1pwZVL5tCLxrdr4NyAadpG1koyiyBBnJA3h9yrNH6bMU96CNlh35uI45w1b7haKwn1ptDX_9DLcU6xTKcF47ApC2dFrQ7KpTHnhF5fpTCYtGhg-q4CfVeBfqigPHh1HzvbAdsH_ufPC2gO4EfocflPnN5-Otv_Df8NNuCUXQ</recordid><startdate>20240408</startdate><enddate>20240408</enddate><creator>Li, Qian</creator><creator>Zhao, Zhenyang</creator><creator>Chen, Fan</creator><creator>Xu, Xiaohui</creator><creator>Xu, Lizhi</creator><creator>Cheng, Liang</creator><creator>Adeli, Mohsen</creator><creator>Luo, Xianglin</creator><creator>Cheng, Chong</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>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-6872-2240</orcidid><orcidid>https://orcid.org/0000-0003-3328-1147</orcidid></search><sort><creationdate>20240408</creationdate><title>Delocalization Engineering of Heme‐Mimetic Artificial Enzymes for Augmented Reactive Oxygen Catalysis</title><author>Li, Qian ; Zhao, Zhenyang ; Chen, Fan ; Xu, Xiaohui ; Xu, Lizhi ; Cheng, Liang ; Adeli, Mohsen ; Luo, Xianglin ; Cheng, Chong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3738-e1efb9bb8bb6b241f78bc27d2980dad1cb240cef39fd5122a1a9d974870be1713</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>artificial enzymes</topic><topic>biocatalysts</topic><topic>Biosensors</topic><topic>Catalysis</topic><topic>Chemical synthesis</topic><topic>Conjugation</topic><topic>Electron transfer</topic><topic>Enzymes</topic><topic>Heme</topic><topic>Heme - chemistry</topic><topic>heme-mimetic materials</topic><topic>Organic chemistry</topic><topic>Oxygen</topic><topic>Oxygen - chemistry</topic><topic>peroxidase-like activity</topic><topic>Polymers</topic><topic>Porphyrins</topic><topic>Porphyrins - chemistry</topic><topic>Reactive Oxygen Species</topic><topic>Substrates</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Qian</creatorcontrib><creatorcontrib>Zhao, Zhenyang</creatorcontrib><creatorcontrib>Chen, Fan</creatorcontrib><creatorcontrib>Xu, Xiaohui</creatorcontrib><creatorcontrib>Xu, Lizhi</creatorcontrib><creatorcontrib>Cheng, Liang</creatorcontrib><creatorcontrib>Adeli, Mohsen</creatorcontrib><creatorcontrib>Luo, Xianglin</creatorcontrib><creatorcontrib>Cheng, Chong</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Qian</au><au>Zhao, Zhenyang</au><au>Chen, Fan</au><au>Xu, Xiaohui</au><au>Xu, Lizhi</au><au>Cheng, Liang</au><au>Adeli, Mohsen</au><au>Luo, Xianglin</au><au>Cheng, Chong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Delocalization Engineering of Heme‐Mimetic Artificial Enzymes for Augmented Reactive Oxygen Catalysis</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2024-04-08</date><risdate>2024</risdate><volume>63</volume><issue>15</issue><spage>e202400838</spage><epage>n/a</epage><pages>e202400838-n/a</pages><issn>1433-7851</issn><issn>1521-3773</issn><eissn>1521-3773</eissn><abstract>Developing artificial enzymes based on organic molecules or polymers for reactive oxygen species (ROS)‐related catalysis has broad applicability. Herein, inspired by porphyrin‐based heme mimics, we report the synthesis of polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) as a new porphyrin‐evolving structure to serve as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to the structural advantages, such as enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS‐production activity in terms of Vmax and turnover numbers as compared with porphyrin‐based conjugated polymers (Fe‐PPor‐AE), which also surpassed reported state‐of‐the‐art artificial enzymes in their activity. More interestingly, by changing the reaction medium and substrates, Fe‐PPc‐AE also revealed significantly improved activity and environmental adaptivity in many other ROS‐related biocatalytic processes, validating the potential of Fe‐PPc‐AE to replace conventional (poly)porphyrin‐based heme mimics for ROS‐related catalysis, biosensors, or biotherapeutics. It is suggested that this study will offer essential guidance for designing artificial enzymes based on organic molecules or polymers.
Inspired by porphyrin‐based heme mimics, polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) were synthesized as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe−N coordination centers, Fe‐PPc‐AE showed more efficient ROS production even than the reported state‐of‐the‐art biocatalysts.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>38372011</pmid><doi>10.1002/anie.202400838</doi><tpages>12</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-6872-2240</orcidid><orcidid>https://orcid.org/0000-0003-3328-1147</orcidid></addata></record> |
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| subjects | artificial enzymes biocatalysts Biosensors Catalysis Chemical synthesis Conjugation Electron transfer Enzymes Heme Heme - chemistry heme-mimetic materials Organic chemistry Oxygen Oxygen - chemistry peroxidase-like activity Polymers Porphyrins Porphyrins - chemistry Reactive Oxygen Species Substrates |
| title | Delocalization Engineering of Heme‐Mimetic Artificial Enzymes for Augmented Reactive Oxygen Catalysis |
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