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Selective Oxidation of Methacrolein over Crystalline Mo3VOx Catalysts and Comparison of Their Catalytic Properties with Heteropoly Acid Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-24 , DOI: 10.1021/acscatal.0c02530 Satoshi Ishikawa 1 , Nagisa Noda 1 , Masaki Wada 1 , Shota Tsurumi 1 , Wataru Ueda 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-24 , DOI: 10.1021/acscatal.0c02530 Satoshi Ishikawa 1 , Nagisa Noda 1 , Masaki Wada 1 , Shota Tsurumi 1 , Wataru Ueda 1
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Four distinct crystalline Mo3VOx catalysts comprising the same structural units were tested for the selective oxidation of methacrolein (MCR). Crystalline orthorhombic Mo3VOx (Orth-MoVO), trigonal Mo3VOx (Tri-MoVO), and amorphous Mo3VOx (Amor-MoVO) having pentagonal, hexagonal, and heptagonal channels in the crystal structure showed far better catalytic activity and selectivity to methacrylic acid (MAA) than those of various Mo–V-based mixed oxide catalysts. Tetragonal Mo3VOx (Tet-MoVO) having pentagonal and hexagonal but no heptagonal channels in the crystal structure provided minor MCR oxidation activity, and the MAA selectivity was lower than that of the other crystalline Mo3VOx catalysts with heptagonal channels. In situ Fourier transform infrared (FT-IR) measurements revealed that Orth-MoVO and Tri-MoVO were active with respect to MCR, forming methacrylate as a reaction intermediate, while no infrared (IR) bands related to surface compounds were observed over Tet-MoVO after the MCR injection. Based on these results, we concluded that the crystal structure of crystalline Mo3VOx catalysts significantly affects the catalytic MCR oxidation activity. Orth-MoVO catalyzed the MCR oxidation at low reaction temperatures (<240 °C), where the conventional catalyst used for the industrial MCR oxidation process, a heteropoly acid (HPA)-based catalyst, displayed poor catalytic activity.
中文翻译：
结晶Mo 3 VO x催化剂上甲基丙烯醛的选择性氧化及其与杂多酸催化剂的催化性能比较
测试了包含相同结构单元的四种不同的结晶Mo 3 VO x催化剂对甲基丙烯醛（MCR）的选择性氧化。晶体结构中具有五边形，六边形和七边形通道的正交晶体Mo 3 VO x（Orth-MoVO），三角形Mo 3 VO x（Tri-MoVO）和非晶Mo 3 VO x（Amor-MoVO）活性和对甲基丙烯酸（MAA）的选择性高于各种基于Mo-V的混合氧化物催化剂。四方Mo 3 VO x（Tet-MoVO）在晶体结构中具有五边形和六边形但没有七边形通道提供较小的MCR氧化活性，并且MAA选择性低于具有七边形通道的其他结晶Mo 3 VO x催化剂。原位傅立叶变换红外（FT-IR）测量表明，Orth-MoVO和Tri-MoVO对MCR具有活性，形成甲基丙烯酸酯作为反应中间体，而在Tet-上未观察到与表面化合物相关的红外（IR）谱带。 MCR注射后的MoVO。根据这些结果，我们得出结论，Mo 3 VO x晶体的晶体结构催化剂显着影响催化MCR的氧化活性。Orth-MoVO在低反应温度（<240°C）下催化了MCR氧化，其中用于工业MCR氧化过程的常规催化剂，基于杂多酸（HPA）的催化剂，显示出较差的催化活性。
更新日期：2020-09-20
中文翻译：
结晶Mo 3 VO x催化剂上甲基丙烯醛的选择性氧化及其与杂多酸催化剂的催化性能比较
测试了包含相同结构单元的四种不同的结晶Mo 3 VO x催化剂对甲基丙烯醛（MCR）的选择性氧化。晶体结构中具有五边形，六边形和七边形通道的正交晶体Mo 3 VO x（Orth-MoVO），三角形Mo 3 VO x（Tri-MoVO）和非晶Mo 3 VO x（Amor-MoVO）活性和对甲基丙烯酸（MAA）的选择性高于各种基于Mo-V的混合氧化物催化剂。四方Mo 3 VO x（Tet-MoVO）在晶体结构中具有五边形和六边形但没有七边形通道提供较小的MCR氧化活性，并且MAA选择性低于具有七边形通道的其他结晶Mo 3 VO x催化剂。原位傅立叶变换红外（FT-IR）测量表明，Orth-MoVO和Tri-MoVO对MCR具有活性，形成甲基丙烯酸酯作为反应中间体，而在Tet-上未观察到与表面化合物相关的红外（IR）谱带。 MCR注射后的MoVO。根据这些结果，我们得出结论，Mo 3 VO x晶体的晶体结构催化剂显着影响催化MCR的氧化活性。Orth-MoVO在低反应温度（<240°C）下催化了MCR氧化，其中用于工业MCR氧化过程的常规催化剂，基于杂多酸（HPA）的催化剂，显示出较差的催化活性。
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