Carbon Dioxide Activation at Metal Centers: Evolution of Charge Transfer from Mg?.+ to CO2 in [MgCO2(H2O)n].+ ,n=  0–8

Barwa Erik; Pascher Tobias F.; On?ák Milan; Linde Christian; Beyer Martin K.

摘要

Abstract > We investigate activation of carbon dioxide by singly charged hydrated magnesium cations Mg? .+ (H <sub>2</sub> O) <sub> n </sub> , through infrared multiple photon dissociation (IRMPD) spectroscopy combined with quantum chemical calculations. The spectra of [MgCO <sub>2</sub> (H <sub>2</sub> O) <sub> n </sub> ] .+ in the 1250–4000?cm ?1 region show a sharp transition from n= 2 to n= 3 for the position of the CO <sub>2</sub> antisymmetric stretching mode. This is evidence for the activation of CO <sub>2</sub> via charge transfer from Mg? .+ to CO <sub>2</sub> for n ≥3, while smaller clusters feature linear CO <sub>2</sub> coordinated end‐on to the metal center. Starting with n= 5, we see a further conformational change, with CO <sub>2</sub> .? coordination to Mg 2+ gradually shifting from bidentate to monodentate, consistent with preferential hexa‐coordination of Mg 2+ . Our results reveal in detail how hydration promotes CO <sub>2</sub> activation by charge transfer at metal centers. </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> > 我们通过单电荷的水合镁阳离子Mg调查二氧化碳的激活？。+ </ sup> （H <sub> 2 </ sub> o） <sub> n </ i> </ sub> ，通过红外线多光子解离（IRMPD）光谱与量子化学计算结合。 [mgco的光谱 <sub> 2 </ sub> （H <sub> 2 </ sub> o） <sub> n </ i> </ sub> ] 。+ </ sup> 在1250-4000？cm ？1 </ sup> 区域显示出急剧过渡 n = </ i> 2到 n = </ i> 3对于CO的位置 <sub> 2 </ sub> 反对称拉伸模式。这是CO的激活的证据 <sub> 2 </ sub> 通过MG的电荷转移？。+ </ sup> 合作 <sub> 2 </ sub> 为了 n </ i> ≥3，较小的簇具有线性CO <sub> 2 </ sub> 协调为金属中心的终端。从...开始 n = </ i> 5，我们看到进一步的构象变化，与CO <sub> 2 </ sub> 。？</ sup> 协调到MG. 2 + </ sup> 逐渐从二齿到单怡特，符合优先的六巴 - 协调mg 2 + </ sup> 。我们的结果详细揭示了水合如何促进CO <sub> 2 </ sub> 金属中心电荷转移激活。 </ 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19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=Barwa Erik&option=202" target="_blank" rel="nofollow">Barwa Erik;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Pascher Tobias F.&option=202" target="_blank" rel="nofollow">Pascher Tobias F.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=On?ák Milan&option=202" target="_blank" rel="nofollow">On?ák Milan;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Linde Christian&option=202" target="_blank" rel="nofollow">Linde Christian;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Beyer Martin K.&option=202" target="_blank" rel="nofollow">Beyer Martin K.;</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 für Ionenphysik und Angewandte PhysikUniversit?t InnsbruckTechnikerstra?e 25 6020 Innsbruck Austria;</p> <p>Institut für Ionenphysik und Angewandte PhysikUniversit?t InnsbruckTechnikerstra?e 25 6020 Innsbruck Austria;</p> <p>Institut für Ionenphysik und Angewandte PhysikUniversit?t InnsbruckTechnikerstra?e 25 6020 Innsbruck Austria;</p> <p>Institut für Ionenphysik und Angewandte PhysikUniversit?t InnsbruckTechnikerstra?e 25 6020 Innsbruck Austria;</p> <p>Institut für Ionenphysik und Angewandte PhysikUniversit?t InnsbruckTechnikerstra?e 25 6020 Innsbruck Austria;</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=ab initio calculations&option=203" rel="nofollow">ab initio calculations;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=CO2 activation&option=203" rel="nofollow">CO2 activation;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=hydration&option=203" rel="nofollow">hydration;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=IR spectroscopy&option=203" rel="nofollow">IR spectroscopy;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=mass spectrometry&option=203" rel="nofollow">mass spectrometry;</a> </p> <div class="translation"> 机译：AB Initio计算;CO2激活;水合;IR光谱;质谱; </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" 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href="/academic-journal-cn_detail_thesis/0201296942772.html">二氧化碳与环氧烷加成反应的金属配合物催化剂及活化机理研究进展</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=王浩&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 王浩</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘定华&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,刘定华</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=沈文彬&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,沈文彬</a> <span> <a href="/journal-cn-56821/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 现代化工 </a> </span> <span> . 2011</span><span>,第S1期</span> </span> </div> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/academic-journal-cn_progress-in-chemistry_thesis/0201286804522.html">过渡金属络合物与二氧化碳活化</a> <b>[J]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=翟纬绪&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 翟纬绪</a> <span> <a href="/journal-cn-12018/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 化学进展 </a> </span> <span> . 1990</span><span>,第001期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-conference-cn_meeting-60604_thesis/020222680575.html">普适性建筑既有空间的保护与再生——从食堂浴室、活动中心到实训基地的进化与活化实验</a> <b>[C]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=尹雷&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 尹雷</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=张俊发&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,张俊发</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=鹿鹏&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,鹿鹏</a> <span> <a href="/conference-cn-60604/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 2015年中国第6届工业建筑遗产学术研讨会 </a> <span> <span> . 2015</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020315755963.html">过渡金属/离子液体协同活化的二氧化碳常压转化反应</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=宋丹丹&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 宋丹丹</a> <span> . 2019</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/061204750891.html">一种碱活化皮革固定短小芽孢杆菌/H2O2净化印染废水的方法</a> <b>[P]</b> . <span> 中国专利： CN110642461B </span> <span> . 2021.11.02</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120113571951.html">一种非共轭连接的空间电荷转移热活化延迟荧光材料及其电致发光应用</a> <b>[P]</b> . <span> 中国专利： CN113603628A </span> <span> . 2021-11-05</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130461839959.html">flare gun equipped to blow up charges of canisters of co2 (carbon dioxide) to launch into the air fustelle paper goffrata and metalizate and bright colored</a> <b>[P]</b> . <span> 外国专利：  ITBO920017A1 </span> <span> . 1993-07-17</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：火炬枪，用于吹散二氧化碳（二氧化碳）罐中的杂物，以将空气中的烟头纸goffrata和金属化金属喷出，并且色泽鲜艳 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130463299332.html">flare gun equipped to blow up charges of canisters of co2 (carbon dioxide) to launch into the air fustelle paper goffrata and metalizate and bright colored</a> <b>[P]</b> . <span> 外国专利：  ITBO920017D0 </span> <span> . 1992-01-16</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：火炬枪，用于吹散二氧化碳（二氧化碳）罐中的杂物，以将空气中的烟头纸goffrata和金属化金属喷出，并且色泽鲜艳 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130422095450.html">COMPLEX COMPOUND CAPABLE OF TAKING DIVALENT OR MORE FORMAL CHARGE OF METAL CENTER BY SYNTHESIZE FROM LIGAND INCLUDING AMMONIUM SALT, AND MANUFACTURING METHOD OF POLYCARBONATE THROUGH COPOLYMERIZATION OF EPOXIDE AND CARBON DIOXIDE USING THE SAME AS CATALYST</a> <b>[P]</b> . <span> 外国专利：  KR20120004372A </span> <span> . 2012-01-12</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：能够通过包含铵盐的配体合成来获得金属中心相同或更多形式电荷的复杂化合物，以及通过使用相同的催化剂将环氧乙烷和二氧化碳共聚合制备聚碳酸酯的方法 </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> 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