Stabilization of the Oxidation State +IV in Siloxide‐Supported Terbium Compounds

Willauer Aurélien R.; Palumbo Chad T.; Scopelliti Rosario; Zivkovic Ivica; Douair Iskander; Maron Laurent; Mazzanti Marinella

摘要

Abstract > The synthesis of lanthanides other than cerium in the oxidation state +IV has remained a desirable but unmet target until recently, when two examples of Tb IV with saturated coordination spheres were isolated. Here we report the third example of an isolated molecular complex of terbium(IV), where the supporting siloxide ligands do not saturate the coordination sphere. The fully characterized six‐coordinate complex [Tb IV (OSiPh <sub>3</sub> ) <sub>4</sub> (MeCN) <sub>2</sub> ], 2 ‐Tb Ph , shows high stability and the labile MeCN ligands can be replaced by phosphinoxide ligands. Computational studies suggest that the stability is due to a strong π(O?Tb) interaction which is stronger than in the previously reported Tb IV complexes. Cyclic‐voltammetry experiments demonstrate that non‐binding counterions contribute to the stability of Tb IV in solution by destabilizing the +III oxidation state, while alkali ions promote Tb IV /Tb III electron transfer. </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> > 除氧化态+ IV中的锡镧的合成仍然是理想的但未掩盖的靶标，直到最近，当TB的两个例子 iv </ sup> 分离饱和的协调球。在这里，我们报告了铽（IV）的分离的分子复合物的第三个例子，其中支持的硅氧烷配体不饱和配位球。完全表征六坐标复杂[TB iv </ sup> （osip. <sub> 3 </ sub> 的） <sub> 4 </ sub> （mecn） <sub> 2 </ sub> ]， 2 </ b> -TB. pH </ sup> ，显示出高稳定性，并且不稳定的Mecn配体可以被膦醛配体代替。计算研究表明，稳定性是由于比以前报道的结核病更强的强烈π（O→TB）相互作用 iv </ sup> 复合物。循环伏安法实验表明，非结合抗衡抵抗有助于TB的稳定性 iv </ sup> 通过破坏+ III氧化态的溶液，而碱离子促进TB iv </ sup> / TB. iii </ sup> 电子转移。 </ 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9期</span><b style="margin: 0 2px;">|</b><span>共5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=Willauer Aurélien R.&option=202" target="_blank" rel="nofollow">Willauer Aurélien R.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Palumbo Chad T.&option=202" target="_blank" rel="nofollow">Palumbo Chad T.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Scopelliti Rosario&option=202" target="_blank" rel="nofollow">Scopelliti Rosario;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Zivkovic Ivica&option=202" target="_blank" rel="nofollow">Zivkovic Ivica;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Douair Iskander&option=202" target="_blank" rel="nofollow">Douair Iskander;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Maron Laurent&option=202" target="_blank" rel="nofollow">Maron Laurent;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Mazzanti Marinella&option=202" target="_blank" rel="nofollow">Mazzanti Marinella;</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>Institut des Sciences et Ingénierie ChimiquesEcole Polytechnique Fédérale de Lausanne (EPFL)1015 Lausanne Switzerland;</p> <p>Institut des Sciences et Ingénierie ChimiquesEcole Polytechnique Fédérale de Lausanne (EPFL)1015 Lausanne Switzerland;</p> <p>Institut des Sciences et Ingénierie ChimiquesEcole Polytechnique Fédérale de Lausanne (EPFL)1015 Lausanne Switzerland;</p> <p>Laboratory for Quantum MagnetismEPFL1015 Lausanne Switzerland;</p> <p>Laboratoire de Physique et Chimie des Nano-objetsInstitut National des Sciences Appliquées31077 Toulouse Cedex 4 France;</p> <p>Laboratoire de Physique et Chimie des Nano-objetsInstitut National des Sciences Appliquées31077 Toulouse Cedex 4 France;</p> <p>Institut des Sciences et Ingénierie ChimiquesEcole Polytechnique Fédérale de Lausanne (EPFL)1015 Lausanne Switzerland;</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=lanthanides&option=203" rel="nofollow">lanthanides;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=metal-ion-coupled electron transfer&option=203" rel="nofollow">metal-ion-coupled electron transfer;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=rare earths&option=203" rel="nofollow">rare earths;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=siloxides&option=203" rel="nofollow">siloxides;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=terbium&option=203" rel="nofollow">terbium;</a> </p> <div class="translation"> 机译：镧系元素;金属离子耦合电子转移;稀土;硅氧化物;铽; </div> </li> </ul> </div> </div> <div class="literature cardcommon"> <div class="similarity "> <h3 class="all_title" id="enpatent66">相似文献</h3> <div class="similaritytab clearfix"> <ul> <li class="active" >外文文献</li> <li >中文文献</li> <li >专利</li> </ul> </div> <div class="similarity_details"> <ul > <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/0704028161257.html">Stabilization of the Oxidation State +IV in Siloxide‐Supported Terbium Compounds</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Willauer Aurélien R.&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Willauer Aurélien R.,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Palumbo Chad T.&option=202" target="_blank" rel="nofollow" class="tuijian_auth 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href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=曹少魁&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 曹少魁</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=单锦宇&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,单锦宇</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=石军&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,石军</a> <span> <a href="/conference-cn-33266/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 中国化学会'99高分子学术论文报告会 </a> <span> <span> . 1999</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020315841246.html">铽功能化二氧化硅复合材料在乳铁蛋白分离纯化中的应用</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=宋顺粉&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 宋顺粉</a> <span> . 2017</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120100953487.html">包含苯并D1,3氧硫杂环戊烯、苯并D1,3氧硫杂环戊烯3-氧化物或苯并D1,3氧硫杂环戊烯3,3-二氧化物的化合物及其作为G蛋白偶联受体119的激动剂的方法/用途</a> <b>[P]</b> . <span> 中国专利： CN109890814A </span> <span> . 2019-06-14</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/061202074721.html">含有进行了稳定化的4-氧代-2,2,6,6-四甲基哌啶-1-氧基的组合物、乙烯基化合物的阻聚剂组合物、及使用其的乙烯基化合物的阻聚方法</a> <b>[P]</b> . <span> 中国专利： CN104039835B </span> <span> . 2016.06.08</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130407410400.html">Separation of terbium(III,IV) oxide</a> <b>[P]</b> . <span> 外国专利：  US10029920B2 </span> <span> . 2018-07-24</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：分离三氧化二（ </span> </p> </li> <li> <div> <b>4. </b><a 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