Enhancement of Carbon Oxides Hydrogenation on Iron‐Based Nanoparticles by In‐Situ Water Removal

Bordet Alexis; Asensio Juan Manuel; Soulantica Katerina; Chaudret Bruno

摘要

Abstract > The carbidization of Fe(0) nanoparticles (NPs) under syngas (CO/H <sub>2</sub> ) produces crystalline Fe <sub>2.2</sub> C iron carbide NPs (ICNPs) displaying excellent hyperthermia properties, however, this transformation is significantly delayed by the concomitant water formation. Consequently, very long carbidization times (～140?h) are needed to obtain ICNPs with high specific absorption rate. In this paper, we show that the rate of the carbidization process can be greatly enhanced by the in‐situ removal of water using activated molecular sieves. As a result, ICNPs displaying very high heating power were obtained after only 40?h. Using this strategy, CO was successfully replaced by CO <sub>2</sub> as a carbon source in the carbidization process, resulting in the efficient conversion of Fe(0) NPs to ICNPs at relatively low temperature (230?°C). Without water removal, carbidization did not occur under these conditions, and the Fe(0) NPs were clearly oxidized. In addition, this approach was successfully applied to displace the equilibrium of CO <sub>2</sub> hydrogenation and accelerate the rate of the magnetically induced hydrogenation of CO <sub>2</sub> on ICNPs. Interestingly, the in‐situ water removal had also a strong influence on the product distribution and especially the chain growth process, leading to a higher selectivity towards the formation of C <sub>3</sub> H <sub>8</sub> (～11?%). </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> > 合成气下Fe（0）纳米颗粒（NPS）的碳化（CO / H. <sub> 2 </ sub> ）生产结晶Fe <sub> 2.2 </ sub> C铁碳化铁（ICNP）显示出优异的热疗性质，然而，这种转化被伴随的水形成显着延迟。因此，需要非常长的碳化时间（〜140μl）以获得具有高比吸收率的ICNP。在本文中，我们表明，通过使用活性分子筛的原位除去水，可以大大提高碳化过程的速率。结果，在仅40℃后获得了显示非常高的加热功率的ICNP。使用此策略，CO成功取代了CO <sub> 2 </ sub> 作为碳化过程中的碳源，导致在相对低的温度（230℃）下的Fe（0）NPS至ICNP的有效转化。没有去除除水，在这些条件下没有发生碳化，并且Fe（0）NPS明显氧化。此外，这种方法已成功应用于取代CO的均衡 <sub> 2 </ sub> 氢化并加速磁诱导的CO的氢化速率 <sub> 2 </ sub> 在ICNPS上。有趣的是，原位除水性对产品分布和尤其是链生长过程的影响也强烈影响，导致对C形成的较高选择性 <sub> 3 </ sub> H <sub> 8 </ sub> （〜11？％）。 </ 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>2018年第18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=Bordet Alexis&option=202" target="_blank" rel="nofollow">Bordet Alexis;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Asensio Juan Manuel&option=202" target="_blank" rel="nofollow">Asensio Juan Manuel;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Soulantica Katerina&option=202" target="_blank" rel="nofollow">Soulantica Katerina;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chaudret Bruno&option=202" target="_blank" rel="nofollow">Chaudret Bruno;</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>LPCNOUniversité de Toulouse CNRS INSA UPS135 avenue de Rangueil 31077 Toulouse France;</p> <p>LPCNOUniversité de Toulouse CNRS INSA UPS135 avenue de Rangueil 31077 Toulouse France;</p> <p>LPCNOUniversité de Toulouse CNRS INSA UPS135 avenue de Rangueil 31077 Toulouse France;</p> <p>LPCNOUniversité de Toulouse CNRS INSA UPS135 avenue de Rangueil 31077 Toulouse France;</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=CO 2 Hydrogenation&option=203" rel="nofollow">CO 2 Hydrogenation;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Iron Carbide&option=203" rel="nofollow">Iron Carbide;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Nanoparticles&option=203" rel="nofollow">Nanoparticles;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Magnetic Hyperthermia&option=203" rel="nofollow">Magnetic Hyperthermia;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Water Removal&option=203" rel="nofollow">Water Removal;</a> </p> <div class="translation"> 机译：二氧化碳氢化;碳化铁;纳米粒子;磁体热疗;除水; 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<b>[P]</b> . <span> 外国专利：  US2018118A </span> <span> . 1935-10-22</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：通过基于铁水蒸气反应的方法将制氢过程中产生的一氧化碳，氮气和氢气，残留气体和排放气体转化为混合物的方法 </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('0704022057382','4',7,2,1,'',this,24)" class="delivery" prompt="010401" title="通过人工服务将文献原文发送至邮箱" >获取原文</div> <div class="journalsub-pop-up" style="display: none"> <div class="journal-sub"> <h2>期刊订阅</h2> <img 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