Reaction mechanism and modeling study for the oxidation by SO        <sub >2</sub>2        of        <i >oo        ‐xylene and        <i >pp        ‐xylene in Claus process

Sinha Sourab; Raj Abhijeet

摘要

Abstract > Claus process, comprising of a furnace and a catalytic unit, is used to produce sulfur from H <sub>2</sub> S. The aromatic contaminants (benzene, toluene, and xylenes) in H <sub>2</sub> S feed form soot, and clog and deactivate the catalysts. Xylenes are known to be the most damaging ones. Therefore, there is a need to oxidize them in the furnace to enhance catalyst life. This article presents a kinetics study on the oxidation of o‐ and p‐ xylene radicals by SO <sub>2</sub> (an oxidant that is already present in the furnace) using density functional theory and a composite method. The mechanism begins with H‐abstraction from xylenes to form xylyl radicals, followed by exothermic addition of SO <sub>2</sub> to them. The breakage of O?S bond in the xylyl‐SO <sub>2</sub> adducts leads to the loss of SO molecule, while the remaining O atom on them helps in their oxidation. The isomerization study shows that less‐stable dimethylphenyl radicals have a high tendency to isomerize to resonantly stabilized methylbenzyl radicals. However, methylbenzyl radicals have lower reactivity toward SO <sub>2</sub> than dimethylphenyl radicals. The reaction rate constants were found using transition state theory. The reactor simulations reveal that p‐ xylene has lower reactivity toward SO <sub>2</sub> than o‐ xylene, and CO, SO, and CHO are the main by‐products of oxidation. </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”> <标题类型=“main”>摘要</标题> >条文方法，包括炉子和催化单元，用于产生H <sub> 2 </ sub的硫> S.在H <sub> 2 </ sup> S饲料中的芳族污染物（苯，甲苯和二甲苯）形成烟灰，并堵塞催化剂。已知二甲烯是最有害的。因此，需要在炉中氧化它们以增强催化剂寿命。本文介绍了通过SO <sub> 2 </ sub>（已经存在于中已经存在的氧化剂）的氧化的动力学研究。 2-</ i>二甲苯自由基炉子）采用密度泛函理论和复合方法。该机制从二甲苯的H-Abstach开始以形成Xylyl自由基，然后放热加入所以<sub> 2 </ sub>。 Xylyl-so <sub> 2 </ sub>加合物中的Oα键的破损导致所以分子的损失，而它们上的剩余O原子有助于它们氧化。异构化研究表明，较少稳定的二甲基苯基自由基具有高倾向于异构化以共振稳定甲基苄基。然而，甲基苄基的反应性比二甲基苯基与二甲基苯基较低。使用过渡状态理论发现反应速率常数。反应器模拟揭示了 p - </ i>二甲苯对SO <sub> 2 </ sup>的反应性低于 o - </ i>二甲苯，CO，SO和CHO是主要的副产品的氧化。 </ p> </ abstract> </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-21753/'>《International Journal of Quantum Chemistry》</a> <b style="margin: 0 2px;">|</b><span>2018年第14期</span><b style="margin: 0 2px;">|</b><span>共21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=Sinha Sourab&option=202" target="_blank" rel="nofollow">Sinha Sourab;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Raj Abhijeet&option=202" target="_blank" rel="nofollow">Raj Abhijeet;</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 Chemical EngineeringThe Petroleum InstituteAbu Dhabi 2533 United Arab Emirates;</p> <p>Department of Chemical EngineeringThe Petroleum InstituteAbu Dhabi 2533 United Arab Emirates;</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/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=Claus process&option=203" rel="nofollow">Claus process;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=DFT&option=203" rel="nofollow">DFT;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=oxidation&option=203" rel="nofollow">oxidation;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=reaction kinetics&option=203" rel="nofollow">reaction kinetics;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=sulfur dioxide&option=203" rel="nofollow">sulfur dioxide;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=xylene isomers&option=203" rel="nofollow">xylene isomers;</a> </p> <div class="translation"> 机译：克劳斯过程;DFT;氧化;反应动力学;二氧化硫;二甲苯异构体; 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target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 王春芳</a> <span> . 2007</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120101501014.html">通过二氧化硫选择性膜技术以及二氧化硫选择性吸收技术优化克劳斯尾气处理</a> <b>[P]</b> . <span> 中国专利： CN110621389A </span> <span> . 2019-12-27</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120104399668.html">通过氧化还原反应由丙烯醛生产丙烯酸的方法以及一种固体混合氧化物组合物作为所述反应中的氧化还原系统的应用</a> <b>[P]</b> . <span> 中国专利： CN1196974A </span> <span> . 1998-10-28</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130458971659.html">Process for the oxidation of at least one oxidizable reagent, selected from the group consisting of methanol, benzene, naphthalene, ortho xylene, cumene, methane, propylene, acrolein.Hydrogen and ammonia with oxidant and process for mixing at least one oxidizable reagent, which is susceptible to flammable or explosive reactions during the said mixture with oxidant</a> <b>[P]</b> . <span> 外国专利：  BR9304298A </span> <span> . 1995-03-28</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：氧化至少一种选自甲醇，苯，萘，邻二甲苯，枯烯，甲烷，丙烯，丙烯醛，氧化剂的氢和氨的方法以及将至少一种可氧化剂混合的方法在与氧化剂混合的过程中易燃或易爆反应 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130475047294.html">Process for the separation of phthalic anhydride contained in the reaction of the catalytic oxidation of the o - xylene or naphthalene</a> <b>[P]</b> . <span> 外国专利：  FR2444676B1 </span> <span> . 1983-04-22</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：邻二甲苯或萘催化氧化反应中所含邻苯二甲酸酐的分离方法 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130477285479.html">Process for continuously separating phthalic anhydride from the reaction gases of the catalytic oxidation of o-xylene and/or naphthalene</a> <b>[P]</b> . <span> 外国专利：  US4285870A </span> <span> . 1981-08-25</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：从邻二甲苯和/或萘的催化氧化反应气体中连续分离邻苯二甲酸酐的方法 </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> </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" style="bottom: 19px;z-index: 999;" onclick="ywcd('0704019755677','4',7,2,1,'',this,24)" class="delivery" prompt="010401" 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Reaction mechanism and modeling study for the oxidation by SO 22 of oo ‐xylene and pp ‐xylene in Claus process

摘要

Reaction mechanism and modeling study for the oxidation by SO ₂2 of oo ‐xylene and pp ‐xylene in Claus process