Efficient Hydrogen Storage and Production Using a Catalyst with an Imidazoline‐Based, Proton‐Responsive Ligand

Wang Lin; Onishi Naoya; Murata Kazuhisa; Hirose Takuji; Muckerman James T.; Fujita Etsuko; Himeda Yuichiro

摘要

Abstract > A series of new imidazoline‐based iridium complexes has been developed for hydrogenation of CO <sub>2</sub> and dehydrogenation of formic acid. One of the proton‐responsive complexes bearing two ?OH groups at ortho and para positions on a coordinating pyridine ring ( 3?b ) can catalyze efficiently the chemical fixation of CO <sub>2</sub> and release H <sub>2</sub> under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO <sub>2</sub> can be efficiently carried out under CO <sub>2</sub> and H <sub>2</sub> at atmospheric pressure in basic water by 3?b , achieving a turnover frequency of 106?h ?1 and a turnover number of 7280 at 25?°C, which are higher than ever reported. Moreover, highly efficient CO‐free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H <sub>2</sub> ‐storage system in water. </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> > 已经开发了一系列基于咪唑啉的铱络合物，用于氢化CO <sub> 2 </ sub> 和甲酸的脱氢。轴承两组的质子响应复合物之一 ortho </ i> 和 para </ i> 在配位吡啶环上的位置（ 3？b </ b> ）可以有效地催化CO的化学固定 <sub> 2 </ sub> 并释放H. <sub> 2 </ sub> 在水性介质中的温和条件下，不使用有机添加剂/溶剂。值得注意的是，CO的氢化 <sub> 2 </ sub> 可以有效地进行CO <sub> 2 </ sub> 和H. <sub> 2 </ sub> 在基本水中的大气压下 3？b </ b> ，实现了106次的周转频率？1 </ sup> 和25°C的营业额7280，比曾经报告的高7280。此外，已经实现了在温和条件下采用相同催化剂的水溶液中甲酸的高效无氢氢产生，从而提供有希望的H. <sub> 2 </ sub> - 水中的古代系统。 </ 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-16185/'>《ChemSusChem 》</a> <b style="margin: 0 2px;">|</b><span>2017年第6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=Wang Lin&option=202" target="_blank" rel="nofollow">Wang Lin;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Onishi Naoya&option=202" target="_blank" rel="nofollow">Onishi Naoya;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Murata Kazuhisa&option=202" target="_blank" rel="nofollow">Murata Kazuhisa;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Hirose Takuji&option=202" target="_blank" rel="nofollow">Hirose Takuji;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Muckerman James T.&option=202" target="_blank" rel="nofollow">Muckerman James T.;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Fujita Etsuko&option=202" target="_blank" rel="nofollow">Fujita Etsuko;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Himeda Yuichiro&option=202" target="_blank" rel="nofollow">Himeda Yuichiro;</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>Research Institute of Energy FrontierNational Institute of Advanced Industrial Science and TechnologyTsukuba Central 5 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan;</p> <p>Research Institute of Energy FrontierNational Institute of Advanced Industrial Science and TechnologyTsukuba Central 5 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan;</p> <p>Research Institute of Energy FrontierNational Institute of Advanced Industrial Science and TechnologyTsukuba Central 5 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan;</p> <p>Graduate School of Science and EngineeringSaitama University255 Shimo-ohkubo Sakura-ku Saitama Japan;</p> <p>Chemistry DivisionBrookhaven National LaboratoryUpton NY 11973-5000 USA;</p> <p>Chemistry DivisionBrookhaven National LaboratoryUpton NY 11973-5000 USA;</p> <p>Research Institute of Energy FrontierNational Institute of Advanced Industrial Science and TechnologyTsukuba Central 5 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan;</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/159.html" title="化学">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=CO2 hydrogenation&option=203" rel="nofollow">CO2 hydrogenation;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=H2 storage&option=203" rel="nofollow">H2 storage;</a> <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=imidazoline&option=203" rel="nofollow">imidazoline;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=iridium complex&option=203" rel="nofollow">iridium complex;</a> </p> <div class="translation"> 机译：CO2氢化;H2储存;均匀催化;咪唑啉;铱络合物; </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/0704022092684.html">Efficient Hydrogen Storage and Production Using a Catalyst with an Imidazoline‐Based, Proton‐Responsive Ligand</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wang Lin&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">Wang Lin,</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Onishi Naoya&option=202" 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class="tuijian_authcolor"> . 第十七届全国化肥甲醇技术年会 </a> <span> <span> . 2008</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020313474672.html">可见光响应型金属纳米催化剂的设计合成及其在催化储氢材料放氢中的应用</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘鹏龙&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 刘鹏龙</a> <span> . 2017</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120112731922.html">储氢材料催化剂、含该催化剂的储氢材料及制备方法</a> <b>[P]</b> . <span> 中国专利： CN112755989A </span> <span> . 2021-05-07</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120970387.html">可见光响应型光催化剂粉末及使用了该粉末的可见光响应型光催化剂材料、光催化剂涂料及光催化剂产品</a> <b>[P]</b> . <span> 中国专利： CN101795767B </span> <span> . 2012.07.04</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130410437727.html">Metal-ligand concerted catalysis via nh arm deprotonation / pyridine dearomatization for efficient hydrogen production from formic acid</a> <b>[P]</b> . <span> 外国专利：  JP2016539793A </span> <span> . 2016-12-22</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：通过nh臂去质子化/吡啶脱芳香化作用的金属-配体协同催化，可有效地从甲酸生产氢 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130404574758.html">Metal-ligand cooperative catalysis through N-H arm deprotonation/pyridine dearomatiztion for efficient hydrogen generation from formic acid</a> <b>[P]</b> . <span> 外国专利：  US10300469B1 </span> <span> . 2019-05-28</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：N-H臂去质子化/吡啶脱芳香化作用的金属-配体协同催化，可有效地从甲酸生成氢 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130411791072.html">Metal-ligand cooperative catalysis through N-H arm deprotonation/pyridine dearomatiztion for efficient hydrogen generation from formic acid</a> <b>[P]</b> . <span> 外国专利：  AU2014358867A1 </span> <span> . 2016-06-23</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：N-H臂去质子化/吡啶脱芳香化作用的金属-配体协同催化，可有效地从甲酸生成氢 </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" 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