Inhibition by Inorganic Dopants of γ‐Alumina Chemical Weathering under Hydrothermal Conditions: Identification of Reactive Sites and their Influence in Fischer–Tropsch Synthesis

摘要

Abstract > Understanding how alumina degradation to boehmite AlOOH can be prevented under hydrothermal conditions is key to design more stable catalysts supported on alumina for Fischer–Tropsch synthesis. We compare the effect of four inorganic dopants to inhibit γ‐alumina chemical weathering under hydrothermal conditions: three metal ions: Mg 2+ , Zr 4+ , Ni 2+ , introduced by impregnation, and nonmetal Si, introduced by the grafting of tetraethyl orthosilicate. Boehmite is formed by a mechanism of dissolution–precipitation. A significant decrease of alumina weathering to boehmite is evidenced for all dopants. For metal ions, the thermal conversion of doped γ‐Al <sub>2</sub> O <sub>3</sub> into an alumina‐rich mixed oxide or the coverage of the alumina surface by particles of a poorly soluble oxide such as NiO contribute to the stabilization of the solid. Alumina dissolution and degradation are only inhibited fully through Si grafting. IR spectra in the OH stretching region suggest that the most reactive alumina sites toward dissolution are basic Al?OH sites located on lateral facets that are blocked upon Si introduction. Fischer–Tropsch reactivity shows that Co catalysts prepared on Mg 2+ ‐ and Si‐doped supports are less active or, at best, as active as a reference Co/γ‐Al <sub>2</sub> O <sub>3</sub> catalyst, which is explained by a lower reducibility of CoO on doped supports. The Co catalyst prepared on Mg 2+ ‐doped γ‐Al <sub>2</sub> O <sub>3</sub> calcined at 900?°C exhibits the best combination of catalytic activity, ease of preparation, and hydrothermal stability. </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> > 理解在水热条件下可以防止氧化铝可降解到Boehmite Alooh，是设计更稳定的催化剂的氧化铝，用于Fischer-Tropsch合成的关键。我们比较四种无机掺杂剂的效果在水热条件下抑制γ-氧化铝化学风化：三个金属离子：Mg 2 + </ sup> ，Zr. 4 + </ sup> ，你 2 + </ sup> 通过浸渍和非金属Si引入，通过嫁接四乙基硅酸盐引入。勃姆石由溶解沉淀机制形成。所有掺杂剂都证明了氧化铝向勃姆石的显着降低。对于金属离子，掺杂γ-Al的热转换 <sub> 2 </ sub> O. <sub> 3 </ sub> 通过诸如NIO的颗粒，通过诸如NIO的含量差的氧化铝表面的富含氧化铝的混合氧化物或氧化铝表面的覆盖范围有助于固体稳定。氧化铝溶解和降解仅通过Si嫁接完全抑制。 OH拉伸区域中的IR光谱表明，溶解的最活性氧化铝位点是位于横向小平面上的基本Alα，其被封闭在Si介绍上。 Fischer-Tropsch反应性表明，在Mg上制备的CO催化剂 2 + </ sup> - 并且Si-掺杂的支撑件较小，或者充其量是活性的，作为参考CO /γ-A1 <sub> 2 </ sub> O. <sub> 3 </ sub> 催化剂，其通过对掺杂载体的COO的降低来解释。在mg上制备的CO催化剂 2 + </ sup> - 致γ-al <sub> 2 </ sub> O. <sub> 3 </ sub> 在900℃下煅烧催化活性，易于制剂和水热稳定性的最佳组合。 </ 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12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=doping&option=203" rel="nofollow">doping;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=magnesium&option=203" rel="nofollow">magnesium;</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=silicon&option=203" rel="nofollow">silicon;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=zirconium&option=203" rel="nofollow">zirconium;</a> </p> <div class="translation"> 机译：掺杂;镁;镍;硅;锆; </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/0704022057200.html">Inhibition by Inorganic Dopants of γ‐Alumina Chemical Weathering under Hydrothermal Conditions: Identification of Reactive Sites and their Influence in Fischer–Tropsch Synthesis</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 class="zwjiyix translation" style="max-width: initial;height: auto;word-break: break-all;white-space: initial;text-overflow: initial;overflow: initial;"> <span>机译：在水热条件下γ-氧化铝化学风化的无机掺杂剂的抑制：鉴定反应性位点及其对费氏托合成的影响</span> </p> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/journal-foreign-detail/07040772267.html">Identification of the active species in the working alumina-supported cobalt catalyst under various conditions of Fischer-Tropsch synthesis</a> <b>[J]</b> . <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=M. 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tuijian_authcolor">,董光华</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘霞&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,刘霞</a> <span> <a href="/journal-cn-9180/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 燃料化学学报 </a> </span> <span> . 2018</span><span> ,第007期</span> </span> </div> </li> <li> <div> <b>6. </b><a class="enjiyixqcontent" href="/academic-conference-cn_meeting-19641_thesis/020222261123.html">锆助剂对钴基费托合成催化剂反应性能的影响</a> <b>[C]</b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=王月伦&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 王月伦</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=陈建刚&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,陈建刚</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=侯博&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,侯博</a> <span> <a href="/conference-cn-19641/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 中国化工学会2008年石油化工学术年会暨北京化工研究院建院50周年学术报告会 </a> <span> <span> . 2008</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020312469029.html">氧化铝负载的钴基催化剂费-托合成反应性能研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=刘成超&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 刘成超</a> <span> . 2017</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" href="/patent-detail/06120108188275.html">高水热稳定性钴基费托合成催化剂及制法和应用</a> <b>[P]</b> . <span> 中国专利： CN105688959A </span> <span> . 2016-06-22</span> </div> </li> <li> <div> <b>2. </b><a class="enjiyixqcontent" href="/patent-detail/06120113990724.html">费托合成循环气脱碳条件下获得催化剂二氧化碳选择性的方法</a> <b>[P]</b> . <span> 中国专利： CN114075445A </span> <span> . 2022-02-22</span> </div> </li> <li> <div> <b>3. </b><a class="enjiyixqcontent" href="/patent-detail/06130420382957.html">Catalyst of cobalt supported on alumina having improved stability and a high activity for the synthesis of Fischer Tropsch synthesis, and method of Fischer Tropsch hydrocarbon</a> <b>[P]</b> . <span> 外国专利：  BR0109337B1 </span> <span> . 2013-10-29</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：具有改善的稳定性和高活性的负载在氧化铝上的钴催化剂用于费-托合成以及费-托烃的合成方法 </span> </p> </li> <li> <div> <b>4. </b><a class="enjiyixqcontent" href="/patent-detail/06130426817470.html">Preparing catalyst, useful for Fischer-Tropsch synthesis, comprises depositing a precursor compound of a catalytically active element on an inorganic carrier material, where the deposition is carried out under basic and acidic conditions</a> <b>[P]</b> . <span> 外国专利：  DE102008025307A1 </span> <span> . 2009-12-03</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：制备用于费-托合成的催化剂，包括将催化活性元素的前体化合物沉积在无机载体材料上，其中在碱性和酸性条件下进行沉积 </span> </p> </li> <li> <div> <b>5. </b><a class="enjiyixqcontent" href="/patent-detail/06130439150439.html">METHOD FOR PRODUCING A catalyst support of stabilized transition alumina (optional), the manufacturing process Fischer-Tropsch catalyst and process for the synthesis of paraffinic hydrocarbons from synthesis gas</a> <b>[P]</b> . <span> 外国专利：  RU2005115063A </span> <span> . 2005-10-10</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：生产稳定化过渡氧化铝（可选）的催化剂载体的方法，费-托催化剂的生产方法以及由合成气合成链烷烃的方法 </span> </p> </li> </ul> </div> </div> </div> <div class="theme cardcommon" style="overflow: auto;display:none"> <h3 class="all_title" 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