Metal‐Templated, Tight Loop Conformation of a Cys‐X‐Cys Biomimetic Assembles a Dimanganese Complex

Le Trung; Nguyen Hao; Perez Lisa M.; Darensbourg Donald J.; Darensbourg Marcetta Y.

摘要

Abstract > With the goal of generating anionic analogues to MN <sub>2</sub> S <sub>2</sub> ? Mn(CO) <sub>3</sub> Br we introduced metallodithiolate ligands, MN <sub>2</sub> S <sub>2</sub> 2? prepared from the Cys‐X‐Cys biomimetic, ema 4? ligand (ema=N,N′‐ethylenebis(mercaptoacetamide); M=Ni II , [V IV ≡O] 2+ and Fe III ) to Mn(CO) <sub>5</sub> Br. An unexpected, remarkably stable dimanganese product, (H <sub>2</sub> N <sub>2</sub> (CH <sub>2</sub> C=O(μ‐S)) <sub>2</sub> )[Mn(CO) <sub>3</sub> ] <sub>2</sub> resulted from loss of M originally residing in the N <sub>2</sub> S <sub>2</sub> 4? pocket, replaced by protonation at the amido nitrogens, generating H <sub>2</sub> ema 2? . Accordingly, the ema ligand has switched its coordination mode from an N <sub>2</sub> S <sub>2</sub> 4? cavity holding a single metal, to a binucleating H <sub>2</sub> ema 2? with bridging sulfurs and carboxamide oxygens within Mn‐μ‐S‐CH <sub>2</sub> ‐C‐O, 5‐membered rings. In situ metal‐templating by zinc ions gives quantitative yields of the Mn <sub>2</sub> product. By computational studies we compared the conformations of “linear” ema 4? to ema 4? frozen in the “tight‐loop” around single metals, and to the “looser” fold possible for H <sub>2</sub> ema 2? that is the optimal arrangement for binucleation. XRD molecular structures show extensive H‐bonding at the amido‐nitrogen protons in the solid state. </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> > 目的是产生到Mn的阴离子类似物 <sub> 2 </ sub> S. <sub> 2 </ sub> ？</ b> MN（CO） <sub> 3 </ sub> BR我们介绍了金属二硫酸盐配体，Mn <sub> 2 </ sub> S. <sub> 2 </ sub> 2？</ sup> 从Cys-X-Cys Biomimic，EMA准备 4？</ sup> 配体（Ema = N，N'-乙基脲（巯基乙酰胺）; m = ni ii </ sup> ，[V. iv </ sup> ≡o] 2 + </ sup> 和fe. iii </ sup> ）到Mn（CO） <sub> 5 </ sub> 布尔。一个意想不到的，非常稳定的Dimanganese产品，（H <sub> 2 </ sub> N. <sub> 2 </ sub> （CH. <sub> 2 </ sub> C = O（μ-s）） <sub> 2 </ sub> [Mn（CO） <sub> 3 </ sub> ] <sub> 2 </ sub> 由于损失最初居住在n <sub> 2 </ sub> S. <sub> 2 </ sub> 4？</ sup> 口袋，替换在氨基氮的质子化，产生h <sub> 2 </ sub> EMA. 2？</ sup> 。因此，EMA配体已从n切换其协调模式 <sub> 2 </ sub> S. <sub> 2 </ sub> 4？</ sup> 持有单个金属的腔，到一个binuclating h <sub> 2 </ sub> EMA. 2？</ sup> 在Mn-μ-S-CH中桥接硫磺和羧酰胺氧氧气 <sub> 2 </ sub> -C-O，5元环。原位金属 - 锌离子模板赋予Mn的定量产量 <sub> 2 </ sub> 产品。通过计算研究，我们比较了“线性”EMA的构象 4？</ sup> 到EMA. 4？</ sup> 在单个金属周围的“紧循环”中冷冻，并为H的“宽松”折叠 <sub> 2 </ sub> EMA. 2？</ sup> 这是Binucleation的最佳布置。 XRD分子结构显示在固态的酰胺 - 氮质子中广泛的H键合。 </ 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=Le Trung&option=202" target="_blank" rel="nofollow">Le Trung;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Nguyen Hao&option=202" target="_blank" rel="nofollow">Nguyen Hao;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Perez Lisa M.&option=202" target="_blank" rel="nofollow">Perez Lisa M.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Darensbourg Donald J.&option=202" target="_blank" rel="nofollow">Darensbourg Donald J.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Darensbourg Marcetta Y.&option=202" target="_blank" rel="nofollow">Darensbourg Marcetta Y.;</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>Department of ChemistryTexas A&</p> <p>M University3255 TAMU College Station TX 77843 USA;</p> <p>Department of ChemistryTexas A&</p> <p>M University3255 TAMU College Station TX 77843 USA;</p> <p>Department of ChemistryTexas A&</p> <p>M University3255 TAMU College Station TX 77843 USA;</p> <p>Department of ChemistryTexas A&</p> <p>M University3255 TAMU College Station TX 77843 USA;</p> <p>Department of ChemistryTexas A&</p> <p>M University3255 TAMU College Station TX 77843 USA;</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=bimetallic complexes&option=203" rel="nofollow">bimetallic complexes;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydrogen bonds&option=203" rel="nofollow">hydrogen bonds;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=manganese&option=203" rel="nofollow">manganese;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=N2S2&option=203" rel="nofollow">N2S2;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=transition metals&option=203" rel="nofollow">transition metals;</a> </p> <div class="translation"> 机译：双金属配合物;氢键;锰;N2S2;过渡金属; </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 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