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Particularly, coacervations of interfacial MAPs, foot protein type\u20103 fast variant (fp\u20103F) and type\u20105 (fp\u20105), are important in the initial mussel adhesion process due to the relationship between the easy secretion\/surface wetting properties of the coacervate and primer\u2010like surface adhesive role of interfacial MAPs, which directly contact the marine surface. To the best of the authors' knowledge, this is the first report on coacervate formation of major recombinant interfacial MAPs with high charge densities and the highest 3,4\u2010dihydroxyphenylalanine (Dopa) contents. Specifically, salt\u2010induced coacervation of fp\u20103F is observed at low pH values corresponding to the acidified environment of the distal depression during mussel secretion. In addition, it shows enthalpy driven upper critical solution temperature behavior, possibly relying on bridging interactions between like\u2010charged cationic fp\u20103Fs including salt\u2010bridge and cation\u2013\u03c0\/\u03c0\u2013\u03c0 interactions in the presence of specific counterions, supported by Raman spectroscopy. It is believed that this study has broadened the scope of the understanding of coacervation of MAPs and may provide new insight for responsive biomaterial design.<\/jats:p>","DOI":"10.1002\/smll.201803377","type":"journal-article","created":{"date-parts":[[2018,11,20]],"date-time":"2018-11-20T09:51:45Z","timestamp":1542707505000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":80,"title":["Coacervation of Interfacial Adhesive Proteins for Initial Mussel Adhesion to a Wet Surface"],"prefix":"10.1002","volume":"14","author":[{"given":"Byeongseon","family":"Yang","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering Pohang University of Science and Technology  Pohang 37673 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sila","family":"Jin","sequence":"additional","affiliation":[{"name":"Department of Chemistry Kangwon National University  Chunchon 24341 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yeonju","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemistry Kangwon National University  Chunchon 24341 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Young Mee","family":"Jung","sequence":"additional","affiliation":[{"name":"Department of Chemistry Kangwon National University  Chunchon 24341 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4640-189X","authenticated-orcid":false,"given":"Hyung Joon","family":"Cha","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Pohang University of Science and Technology  Pohang 37673 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2018,11,20]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1080\/00218460590944602"},{"key":"e_1_2_7_1_2","doi-asserted-by":"publisher","DOI":"10.1146\/annurev-matsci-062910-100429"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201000932"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1181044"},{"key":"e_1_2_7_2_3","doi-asserted-by":"publisher","DOI":"10.1080\/08927014.2012.719023"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aab0556"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6b03453"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchembio.630"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1002\/btpr.1810"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1007\/s10126-007-9053-x"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/biot.200700258"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.biomaterials.2015.08.055"},{"key":"e_1_2_7_6_3","doi-asserted-by":"publisher","DOI":"10.1039\/C4TB01496K"},{"key":"e_1_2_7_6_4","first-page":"1704806","volume":"29","author":"Jo Y. 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