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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Defect-rich Ni-Ti layered double hydroxide as a highly efficient support for Au nanoparticles in base-free and solvent-free selective oxidation of benzyl alcohol
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Defect-rich Ni-Ti layered double hydroxide as a highly efficient support for Au nanoparticles in base-free and solvent-free selective oxidation of benzyl alcohol

机译：富含缺陷的Ni-Ti层状双氢氧化物作为Au纳米颗粒的高效支持，无溶剂无溶剂选择性氧化苄醇

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摘要

Tuning the surface properties of supported metal catalysts is of vital importance for governing their catalytic performances in nanocatalysis. Here, we report highly dispersed nanometric gold nanoparticles (NPs) supported on Ni-Ti layered double hydroxides (NiTi-LDHs), which were employed in solvent-free and base-free selective oxidation of benzyl alcohol. A series of characterization techniques demonstrated that defect-rich NiTi-LDHs could efficiently stabilize Au NPs and decrease surface electron density of Au NPs. The as-formed Au/NiTi-LDH catalyst with a Ni/Ti molar ratio of 3 : 1 and an Au loading of 0.71 wt% yielded the highest turnover frequency value of similar to 4981 h(-1) at 120 degrees C among tested Au/NiTi-LDH catalysts with different Ni/Ti molar ratios, along with a high benzaldehyde selectivity of 98%. High catalytic efficiency of the catalyst was mainly correlated with surface cooperation between unique defects (i.e. defective Ti3+ species and oxygen vacancies) and abundant hydroxyl groups on the brucite-like layers of the NiTi-LDH support, which could lead to the preferential adsorption and activation of an alcohol hydroxyl moiety in benzyl alcohol and oxygen molecule, as well as the formation of more electron-deficient Ni3+ and Au-0 species on the catalyst surface. Furthermore, the present Au/NiTi-LDH catalyst tolerated the oxidation of a wide variety of substrate structures into the corresponding aldehydes, acids or ketones. Our primary results illustrate that defect-rich NiTi-LDHs are promising supports which can efficiently modify surface structure and electronic properties of supported metal catalysts and consequently improve their catalytic performances.
机译：调节负载金属催化剂的表面性质对于控制纳米分析中的催化性能至关重要。在此，我们报告了高度分散的纳米金纳米颗粒（NPS），其支持在Ni-Ti层叠双氢氧化物（NITI-LDH）上，其在无溶剂和基本的苄醇选择性氧化中使用。一系列表征技术表明，富含缺陷的NITI-LDH可以有效地稳定Au NP和降低Au nps的表面电子密度。具有Ni / Ti摩尔比为3：1的AS-Ti / Nit-LDH催化剂，载荷为0.71wt％的Au负荷，得到最高的周转频率值与测试中的120摄氏度在120摄氏度下相似具有不同Ni / Ti摩尔比的Au / Niti-LDH催化剂，以及高苯甲醛选择性为98％。催化剂的高催化效率主要与硝酸盐的层状层上独特的缺陷（即缺陷Ti3 +物种和氧空位）和丰富的羟基之间的表面合作相关，这可能导致优先的吸附和活化苄醇和氧分子中的醇羟基部分，以及在催化剂表面上形成更多电子缺陷的Ni3 +和Au-0种。此外，本发明的Au / Nit-LDH催化剂可容忍各种底物结构的氧化成相应的醛，酸或酮。我们的主要结果说明了富含缺陷的NITI-LDH，这是有效的支持，可以有效地修改支持的金属催化剂的表面结构和电子性质，从而改善其催化性能。

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    Liu Mengran; Fan Guoli; Yu Jiaying; Yang Lan; Li Feng;

  • 作者单位

    Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci &

    Engn State Key Lab Chem Resources Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci &

    Engn State Key Lab Chem Resources Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci &

    Engn State Key Lab Chem Resources Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci &

    Engn State Key Lab Chem Resources Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci &

    Engn State Key Lab Chem Resources Engn Beijing 100029 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;无机化学;
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