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A combination of catalysis, cell\u2010fractionation, and inhibitor experiments, supplemented with in\u2010cell solid\u2010state NMR spectroscopy, confirmed the in\u2010cell assembly. The ArM\u2010containing whole cells were active in the catalysis of the enantioselective Friedel\u2013Crafts alkylation of indoles and the Diels\u2013Alder reaction of azachalcone with cyclopentadiene. Directed evolution resulted in two different improved mutants for both reactions, LmrR_A92E_M8D and LmrR_A92E_V15A, respectively. The whole\u2010cell ArM system required no engineering of the microbial host, the protein scaffold, or the cofactor to achieve ArM assembly and catalysis. We consider this a key step towards integrating abiological catalysis with biosynthesis to generate a hybrid metabolism.\n                  <\/jats:p>","DOI":"10.1002\/anie.202014771","type":"journal-article","created":{"date-parts":[[2021,1,15]],"date-time":"2021-01-15T01:24:32Z","timestamp":1610673872000},"page":"5913-5920","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":94,"title":["In Vivo Assembly of Artificial Metalloenzymes and Application in Whole\u2010Cell Biocatalysis**"],"prefix":"10.1002","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6247-8446","authenticated-orcid":false,"given":"Shreyans","family":"Chordia","sequence":"first","affiliation":[{"name":"Stratingh Institute for Chemistry University of Groningen  Nijenborgh 4 9747 AG Groningen The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5712-2701","authenticated-orcid":false,"given":"Siddarth","family":"Narasimhan","sequence":"additional","affiliation":[{"name":"NMR Spectroscopy group Bijvoet Center for Biomolecular Research Utrecht University  Padualaan 8, 3584 CH Utrecht The Netherlands"},{"name":"Current address: Structural and Computational Biology Unit European Molecular Biology Laboratory  Meyerhofstra\u00dfe 1 69117 Heidelberg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6609-6672","authenticated-orcid":false,"given":"Alessandra","family":"Lucini Paioni","sequence":"additional","affiliation":[{"name":"NMR Spectroscopy group Bijvoet Center for Biomolecular Research Utrecht University  Padualaan 8, 3584 CH Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7068-5613","authenticated-orcid":false,"given":"Marc","family":"Baldus","sequence":"additional","affiliation":[{"name":"NMR Spectroscopy group Bijvoet Center for Biomolecular Research Utrecht University  Padualaan 8, 3584 CH Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0364-9564","authenticated-orcid":false,"given":"Gerard","family":"Roelfes","sequence":"additional","affiliation":[{"name":"Stratingh Institute for Chemistry University of Groningen  Nijenborgh 4 9747 AG Groningen The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2021,2]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.7b00014"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00469a064"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201508816"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201508816"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201811042"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201811042"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-019-0143-x"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.tibtech.2017.10.003"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja500613n"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2018.01.011"},{"key":"e_1_2_7_9_1","author":"Destito P.","year":"2020","journal-title":"Chem. 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