Remote Perfluoroalkyl Substituents are Key to Living Aqueous Ethylene Polymerization

Schnitte Manuel; Scholliers Janine S.; Riedmiller Kai; Mecking Stefan

摘要

Abstract >In various nickel(II) salicylaldiminato ethylene polymerization catalysts, which are a versatile mechanistic probe for substituent effects, longer perfluoroalkyl groups exert a strong effect on catalytic activities and polymer microstructures compared to the trifluoromethyl group. This effect is accounted for by a reduced electron density on the active sites, and is also supported by electrochemical studies. Thus, β‐hydride elimination, the key step of chain transfer and branching pathways, is disfavored while chain‐growth rates are enhanced. This enhancement occurs to an extent that enables living polymerizations in aqueous systems to afford ultra‐high‐molecular‐weight polyethylene for various chelating salicylaldimine motifs. These findings are mechanistically instructive as well as practically useful for illustrating the potential of perfluoroalkyl groups in catalyst design. </abstract> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> <div class="translation abstracttxt"> <span class="zhankaihshouqi fivelineshidden" id="abstract"> <span>机译：</span><Abstract Type =“Main”XML：Lang =“en”> <标题类型=“main”>抽象</ title> 在各种镍（II）水杨酰基聚合乙烯聚合催化剂中，乙烯聚合催化剂是用于取代基的多功能机械探针，与三氟甲基相比，较长的全氟烷基对催化活性和聚合物微观结构产生强烈影响。通过活性位点上的电子密度降低，该效果占据了这种效果，并且还通过电化学研究支持。因此，β-氢化物消除，链转移和分支途径的关键步骤，而链增长率增强。这种增强发生在一定程度上，这使得在水性体系中的活性聚合以提供用于各种螯合水杨酰亚胺基序的超高分子量聚乙烯。这些发现是机械主义的有效性，并且实际上用于说明催化剂设计中全氟烷基的电位。</ p> </摘要> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> </div> <div class="record"> <h2 class="all_title" id="enpatent33" >著录项</h2> <ul> <li> <span class="lefttit">来源</span> <div style="width: 86%;vertical-align: text-top;display: inline-block;"> <a href='/journal-foreign-19011/'>《Angewandte Chemie》</a> <b style="margin: 0 2px;">|</b><span>2020年第8期</span><b style="margin: 0 2px;">|</b><span>共6页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Schnitte Manuel&option=202" target="_blank" rel="nofollow">Schnitte Manuel;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Scholliers Janine S.&option=202" target="_blank" rel="nofollow">Scholliers Janine S.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Riedmiller Kai&option=202" target="_blank" rel="nofollow">Riedmiller Kai;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mecking Stefan&option=202" target="_blank" rel="nofollow">Mecking Stefan;</a> </p> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zkzz" style="display: none;">展开▼</span> </div> </li> <li> <div style="display: flex;"> <span class="lefttit">作者单位</span> <div style="position: relative;margin-left: 3px;max-width: 639px;"> <div class="threelineshidden zhankaihshouqi" id="fOrgthree"> <p>Chair of Chemical Materials ScienceUniversity of Konstanz78457 Konstanz Germany;</p> <p>Chair of Chemical Materials ScienceUniversity of Konstanz78457 Konstanz Germany;</p> <p>Chair of Chemical Materials ScienceUniversity of Konstanz78457 Konstanz Germany;</p> <p>Chair of Chemical Materials ScienceUniversity of Konstanz78457 Konstanz Germany;</p> </div> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zhdw" style="display: none;">展开▼</span> </div> </div> </li> <li > <span class="lefttit">收录信息</span> <span style="width: 86%;vertical-align: text-top;display: inline-block;"></span> </li> <li> <span class="lefttit">原文格式</span> <span>PDF</span> </li> <li> <span class="lefttit">正文语种</span> <span>eng</span> </li> <li> <span class="lefttit">中图分类</span> <span><a href="https://www.zhangqiaokeyan.com/clc/1188.html" title="应用化学">应用化学;</a></span> </li> <li class="antistop"> <span class="lefttit">关键词</span> <p style="width: 86%;vertical-align: text-top;"> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=homogeneous catalysis&option=203" rel="nofollow">homogeneous catalysis;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=fluorine&option=203" rel="nofollow">fluorine;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=ligand design&option=203" rel="nofollow">ligand design;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=nickel&option=203" rel="nofollow">nickel;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=polymers&option=203" rel="nofollow">polymers;</a> </p> <div class="translation"> 机译：均匀催化;氟;配体设计;镍;聚合物; </div> </li> </ul> </div> </div> <div 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<span> <a href="/journal-cn-9182/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 日用化学工业 </a> </span> <span> . 2016</span><span>,第009期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-conference-cn_meeting-33553_thesis/02022889754.html">全氟(多氟)烷基磺酰叠氮R<,f>SO<,2>N<,3>与烯基硅醚的反应研究</a> <b>[C]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=许勇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 许勇</a> <span> <a href="/conference-cn-33553/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 第七届全国氟化学讨论会 </a> <span> <span> . 1998</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020313138329.html">过渡金属催化的(Z)-β-烷氧基全氟烷基烯酮和β-氟代全氟烷基烯酮的合成研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=罗强&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 罗强</a> <span> . 2016</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120104594953.html">在5位具有全氟代烷基取代基的萘吡喃,其制法和含该萘吡喃的组合物和基质</a> <b>[P]</b> . <span> 中国专利： CN1387524A </span> <span> . 2002-12-25</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120108105544.html">端基为全氟氧杂烷基的氟表面活性剂合成工艺</a> <b>[P]</b> . <span> 中国专利： CN105642187A </span> <span> . 2016-06-08</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130445739336.html">Naphthopyranes with a substituent perfluoroalkyl group in position 5, the preparation and compositions and matrices (co) polymers containing them,</a> <b>[P]</b> . <span> 外国专利：  FR2800738B1 </span> <span> . 2002-02-08</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：在5位带有全氟烷基取代基的萘并吡喃，其制备物和组合物以及含有它们的基质（共）聚合物， </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130446842994.html">Naphthopyranes with a substituent perfluoroalkyl group in position 5, the preparation and compositions and matrices (co) polymers containing them,</a> <b>[P]</b> . <span> 外国专利：  CL2000002997A1 </span> <span> . 2002-02-27</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：在5位带有全氟烷基取代基的萘并吡喃，其制备物和组合物以及含有它们的基质（共）聚合物， </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130433500763.html">Chitin derivatives, polymeric micelle type carrier and micelle-like aqueous composition consisting of the chitin derivative having a carboxyl lower alkyl group and a hydrophobic substituent as a hydrophilic substituent</a> <b>[P]</b> . <span> 外国专利：  JP4119482B2 </span> <span> . 2008-07-16</span> </div> <p class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：几丁质衍生物，聚合物胶束型载体和由具有羧基低级烷基和疏水取代基作为亲水取代基的几丁质衍生物组成的胶束状水性组合物 </span> </p> </li> </ul> </div> </div> </div> <div class="theme cardcommon" style="overflow: auto;display:none"> <h3 class="all_title" id="enpatent55">相关主题</h3> <ul id="subject"> </ul> </div> </div> </div> </div> <div class="right rightcon"> <div class="details_img cardcommon clearfix" style="margin-bottom: 10px;display:none;" > </div> </div> </div> <div id="thesis_get_original1" class="downloadBth" style="bottom: 19px;z-index: 999;" onclick="ywcd('0704028161250','4',7,2,1,'',this,24)" class="delivery" prompt="010401" title="通过人工服务将文献原文发送至邮箱" >获取原文</div> <div class="journalsub-pop-up" style="display: none"> <div class="journal-sub"> <h2>期刊订阅</h2> <img src="https://cdn.zhangqiaokeyan.com/img/loginclose.png" alt="关闭" 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