Homogeneous and Heterogeneous Nickel‐Catalyzed Olefin Oligomerization: Experimental Investigation for a Common Mechanistic Proposition and Catalyst Optimization

摘要

Abstract >Only a few catalytic transformations can be efficiently catalyzed by both homogeneous or heterogeneous technologies, with short olefin oligomerization promoted by a nickel‐based catalysts among them. Homogeneous and heterogeneous catalysis are often opposed in terms of activity, active‐site description or recyclability, traditionally mentioned as “homogeneous versus. heterogeneous”. Unlike previous studies, we propose to emphasize the similarities between both catalysis by comparing industrially representative results obtained in continuous flow‐mode under similar mild conditions. A detailed analysis of both primary products of olefins oligomerization, and a set of secondary products obtained in experimental assays completed with recently published results of DFT calculations prompted us to postulate a common mechanistic pathway for nickel‐catalyzed ethylene oligomerization. Heterogeneous metallic ethylene oligomerization, for which nickel active sites identification has indeed long been under debate, seems to follow the Cossee–Arlman mechanism, well accepted as major mechanism in the homogeneous counterpart. This analysis allowed us to design an unprecedented heterogeneous catalyst active for ethylene and butene oligomerization. </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> 均匀或异质技术只能有效地催化少数催化转化，其中镍基催化剂促进了短的烯烃低聚。均匀和异质催化通常在活性，有源部位描述或可回收性方面相反，传统上提到为“均匀与相反。异质”。与以往的研究不同，我们建议通过在相似的温和条件下在连续流动模式下获得的工业代表性结果进行比较来强调催化作用之间的相似性。对烯烃寡聚化初级产物的详细分析，以及在最近公布的DFT计算结果中获得的一组二次产物，促使我们假设用于镍催化的乙烯低聚的共同机制途径。异质金属乙烯低聚，其中镍活性地点鉴定确实是在辩论中遵循Cossee-Arlman机制，良好地被接受为均匀对应物的主要机制。该分析使我们允许我们设计一个前所未有的异质催化剂，其活性为乙烯和丁烯寡聚化。</ 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-16041/'>《ChemCatChem 》</a> <b style="margin: 0 2px;">|</b><span>2017年第12期</span><b style="margin: 0 2px;">|</b> <span>共10页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> </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"> </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/1186.html" title="物理化学（理论化学）、化学物理学">物理化学（理论化学）、化学物理学 ;</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 and heterogeneous catalysis&option=203" rel="nofollow">homogeneous and heterogeneous catalysis;</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=NiSiF 6&option=203" rel="nofollow">NiSiF 6;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=oligomerization&option=203" rel="nofollow">oligomerization;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=reaction mechanisms&option=203" rel="nofollow">reaction mechanisms;</a> </p> <div class="translation"> 机译：均匀和异质催化;镍;Nisif 6;寡聚化;反应机制; </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/0704022058383.html">Homogeneous and Heterogeneous Nickel‐Catalyzed Olefin Oligomerization: Experimental Investigation for a Common Mechanistic Proposition and Catalyst Optimization</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> </a> <a href="/journal-foreign-16041/" target="_blank" rel="nofollow" class="tuijian_authcolor">ChemCatChem .</a> <span>2017</span> <span>,第12期</span> </span> </div> <p 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href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=周志宏&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,周志宏</a> <span> <a href="/conference-cn-27104/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 中国石化中国石油催化裂化协作组第十届年会 </a> <span> <span> . 2004</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020314628698.html">茂金属及后过渡金属均相烯烃聚合催化剂的研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=罗爽&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 罗爽</a> <span> . 2010</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120290841.html">在多个连续的非均相催化剂区中进行烯烃低聚反应的方法</a> <b>[P]</b> . <span> 中国专利： CN1295199C </span> <span> . 2007.01.17</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120104865206.html">在多个连续的非均相催化剂区中进行烯烃低聚反应的方法</a> <b>[P]</b> . <span> 中国专利： CN1665762A </span> <span> . 2005-09-07</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130501363865.html">Nickel-Based Oligomerization Catalysts and Method for Oligomerizing Light Olefins Using the Same</a> <b>[P]</b> . <span> 外国专利：  US2022008900A1 </span> <span> . 2022-01-13</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：基于镍的寡聚化催化剂和使用相同的轻烯烃的方法 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130440135970.html">Mixed heteroatomic ligand for olefin catalyst oligomerization, olefin catalyst system oligomerization, catalyst system, and process for olefin oligomerization</a> <b>[P]</b> . <span> 外国专利：  BR0215088A </span> <span> . 2004-11-16</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：用于烯烃催化剂低聚的混合杂原子配体，烯烃催化剂体系的低聚，催化剂体系和烯烃低聚的方法 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130431718895.html">Nickel complexes of 2-amino and 2-hydroxy-2-phosphinoalkanoic acid derivatives, processes for the preparation of these nickel complexes and their use as catalysts for the oligomerization or polymerization of olefins</a> <b>[P]</b> . <span> 外国专利：  DE102004029698B4 </span> <span> . 2008-01-31</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：2-氨基和2-羟基-2-膦基链烷酸衍生物的镍配合物，这些镍配合物的制备方法及其在烯烃低聚或聚合反应中的催化剂用途 </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 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