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Surface Organometallic Chemistry on Zeolites: Synthesis of Group IV Metal Alkyls and Metal Hydrides on Hierarchical Mesoporous H-ZSM-5
Chemistry of Materials ( IF 7.2 ) Pub Date : 2022-09-21 , DOI: 10.1021/acs.chemmater.2c02033
Manoj Kumar Gangwar 1 , Swechchha Pandey 1 , Rajesh Kumar Parsapur 1 , Moussab Harb 1 , Sathiyamoorthy Murugesan 1 , Abdul-Hamid Emwas 2 , Omer Refa Koseoglu 3 , Robert Peter Hodgkins 4 , Anissa Bendjeriou-Sedjerari 1 , Magnus Rueping 1 , Kuo-Wei Huang 1 , Jean-Marie Basset 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2022-09-21 , DOI: 10.1021/acs.chemmater.2c02033
Manoj Kumar Gangwar 1 , Swechchha Pandey 1 , Rajesh Kumar Parsapur 1 , Moussab Harb 1 , Sathiyamoorthy Murugesan 1 , Abdul-Hamid Emwas 2 , Omer Refa Koseoglu 3 , Robert Peter Hodgkins 4 , Anissa Bendjeriou-Sedjerari 1 , Magnus Rueping 1 , Kuo-Wei Huang 1 , Jean-Marie Basset 1
Affiliation
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Surface organometallic chemistry (SOMC) has mainly been devoted to the reaction of organometallics with surfaces comprising highly divided and dehydroxylated oxides. The field has been extended to SOMC on metal nanoparticles. However, to the best of our knowledge, SOMC has not been extended to hierarchical fibrous zeolites, although zeolitic materials are a particular class of oxides. Zeolite catalysis is important in hydrocarbon industrial chemistry. However, having an optimum balance between the activity and selectivity of the zeolitic catalysts remains a major challenge in the field. The main difficultly is the plethora of surface sites, only some of which are catalytically active. Given that the acido–basic properties and porosity of zeolites are especially important to the refining and petrochemical industries, we decided to explore this rather unexplored area. Here, three novel well-defined single-site materials [(Np)3M@ZSM-5, M = Ti, Zr, and Hf] supported on a hierarchical mesoporous H-ZSM-5 material (1) are reported. They are prepared using the concepts and tools of SOMC. They are further converted to their corresponding metal hydride [(H)nM@ZSM-5, M = Ti, Zr, and Hf, (n = 1–2)] materials (5–7) through controlled hydrogenolysis of [(≡Si–O−)M(Np)3, M = Ti, Zr, and Hf] materials (2–4) under H2 (1 atm) at 150 °C for 16 h. All these surface catalysts are characterized by various spectroscopic techniques including Fourier transform infrared spectroscopy, elemental analysis, solid-state NMR spectroscopy, powder X-ray diffraction, Brunauer–Emmett–Teller surface area measurements, and scanning electron microscopy and high-resolution transmission electron microscopy analyses and are supported by density functional theory calculations. The catalytic activity of these well-defined single-site novel materials will be tested for the catalytic applications in petrochemistry for refinery processes such as hydrocracking of distillates from crude oil or intermediate refinery process streams to useful petroleum value-added products for the society.
中文翻译：
沸石上的表面有机金属化学：在分级介孔 H-ZSM-5 上合成第 IV 族金属烷基和金属氢化物
表面有机金属化学 (SOMC) 主要致力于有机金属与包含高度分裂和脱羟基氧化物的表面的反应。该领域已扩展到金属纳米颗粒上的 SOMC。然而，据我们所知，SOMC 尚未扩展到分级纤维沸石，尽管沸石材料是一类特殊的氧化物。沸石催化在烃类工业化学中很重要。然而，在沸石催化剂的活性和选择性之间取得最佳平衡仍然是该领域的主要挑战。主要的困难是过多的表面位点，其中只有一些具有催化活性。鉴于沸石的酸碱性和孔隙率对炼油和石化工业尤为重要，我们决定探索这个相当未开发的领域。在这里，三种新颖的定义明确的单点材料[（Np）3 M@ZSM-5，M = Ti、Zr 和 Hf]被报道支持在分级介孔 H-ZSM-5 材料 ( 1 ) 上。它们是使用 SOMC 的概念和工具准备的。它们通过[ （≡ _ _ Si-O-)M(Np) 3 , M = Ti, Zr, and Hf] 材料 ( 2-4 ) 在 H 2下(1 atm) 在 150 °C 下 16 小时。所有这些表面催化剂都通过各种光谱技术进行表征，包括傅里叶变换红外光谱、元素分析、固态核磁共振光谱、粉末 X 射线衍射、布鲁诺-埃米特-泰勒表面积测量、扫描电子显微镜和高分辨率透射电子显微镜分析并得到密度泛函理论计算的支持。这些定义明确的单中心新型材料的催化活性将在炼油工艺的石油化学催化应用中进行测试，例如将原油或中间炼油工艺流中的馏分加氢裂化为社会有用的石油增值产品。
更新日期：2022-09-21
中文翻译：
沸石上的表面有机金属化学：在分级介孔 H-ZSM-5 上合成第 IV 族金属烷基和金属氢化物
表面有机金属化学 (SOMC) 主要致力于有机金属与包含高度分裂和脱羟基氧化物的表面的反应。该领域已扩展到金属纳米颗粒上的 SOMC。然而，据我们所知，SOMC 尚未扩展到分级纤维沸石，尽管沸石材料是一类特殊的氧化物。沸石催化在烃类工业化学中很重要。然而，在沸石催化剂的活性和选择性之间取得最佳平衡仍然是该领域的主要挑战。主要的困难是过多的表面位点，其中只有一些具有催化活性。鉴于沸石的酸碱性和孔隙率对炼油和石化工业尤为重要，我们决定探索这个相当未开发的领域。在这里，三种新颖的定义明确的单点材料[（Np）3 M@ZSM-5，M = Ti、Zr 和 Hf]被报道支持在分级介孔 H-ZSM-5 材料 ( 1 ) 上。它们是使用 SOMC 的概念和工具准备的。它们通过[ （≡ _ _ Si-O-)M(Np) 3 , M = Ti, Zr, and Hf] 材料 ( 2-4 ) 在 H 2下(1 atm) 在 150 °C 下 16 小时。所有这些表面催化剂都通过各种光谱技术进行表征，包括傅里叶变换红外光谱、元素分析、固态核磁共振光谱、粉末 X 射线衍射、布鲁诺-埃米特-泰勒表面积测量、扫描电子显微镜和高分辨率透射电子显微镜分析并得到密度泛函理论计算的支持。这些定义明确的单中心新型材料的催化活性将在炼油工艺的石油化学催化应用中进行测试，例如将原油或中间炼油工艺流中的馏分加氢裂化为社会有用的石油增值产品。
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