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Facile synthesis of a nano titanium catalyst and its performance in selective oxidation of aromatic and pyridinic alcohols under visible light
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-06-15 , DOI: 10.1039/d2re00180b Peng Zheng 1, 2 , Jianguo Liu 3 , Xinghua Zhang 3 , Lungang Chen 3 , Longlong Ma 3 , Qi Zhang 3
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-06-15 , DOI: 10.1039/d2re00180b Peng Zheng 1, 2 , Jianguo Liu 3 , Xinghua Zhang 3 , Lungang Chen 3 , Longlong Ma 3 , Qi Zhang 3
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The oxidation of alcohols to the corresponding carbonyl compounds is of great significance in chemical synthesis and fine chemical production. Traditional oxidants such as MnO2, chromium oxide, high-valent iodine, etc. will produce corresponding stoichiometric derivative waste when oxidizing alcohols. Polluting the environment does not conform to the concepts of green chemistry and atom economy. Herein, we successfully synthesized a small particle size 150-TiO2 by a simple solvothermal process in a hydrothermal reactor using tetrabutyl titanate, water, and ethanol as raw materials. Under visible blue light irradiation, the 150-TiO2 catalyst synthesized in this study exhibited the best catalytic activity and desirable product selectivity among commercial P25, anatase catalysts. Moreover, this catalyst has universality for the catalytic oxidation of different aromatic alcohol substrates, including the interesting pyridyl alcohols which are high-value chemicals for the preparation of pyridine aldehydes and ketones. The in situ facile synthesis heterogeneous catalyst 150-TiO2 not only has excellent stability and recyclability, but also broadly expands the application of green, atom-efficient, and sustainable photocatalytic oxidation of alcohols in pharmaceutical intermediates. Through characterization and result analysis, we confirmed that TiO2 adsorption of benzyl alcohol to form surface complexes is the key to achieving visible light response, and the high specific surface area of TiO2 is the key to achieving high catalytic activity.
中文翻译：
纳米钛催化剂的简便合成及其在可见光下选择性氧化芳族和吡啶醇的性能
将醇类氧化成相应的羰基化合物在化学合成和精细化工生产中具有重要意义。传统氧化剂如MnO 2、氧化铬、高价碘等在氧化醇类时会产生相应的化学计量衍生物废物。污染环境不符合绿色化学和原子经济的概念。在此，我们以钛酸四丁酯、水和乙醇为原料，通过简单的溶剂热法在水热反应器中成功合成了小粒径的 150-TiO 2 。在可见蓝光照射下，150-TiO 2本研究合成的催化剂在商业 P25、锐钛矿催化剂中表现出最好的催化活性和理想的产物选择性。此外，该催化剂对于催化氧化不同的芳香醇底物具有普遍性，包括有趣的吡啶醇，它们是制备吡啶醛和酮的高价值化学品。原位简易合成多相催化剂150-TiO 2不仅具有优异的稳定性和可回收性，还广泛拓展了绿色、原子效率、可持续的醇类光催化氧化在医药中间体中的应用。通过表征和结果分析，我们证实了TiO 2苯甲醇吸附形成表面配合物是实现可见光响应的关键，而TiO 2的高比表面积是实现高催化活性的关键。
更新日期：2022-06-15
中文翻译：
纳米钛催化剂的简便合成及其在可见光下选择性氧化芳族和吡啶醇的性能
将醇类氧化成相应的羰基化合物在化学合成和精细化工生产中具有重要意义。传统氧化剂如MnO 2、氧化铬、高价碘等在氧化醇类时会产生相应的化学计量衍生物废物。污染环境不符合绿色化学和原子经济的概念。在此，我们以钛酸四丁酯、水和乙醇为原料，通过简单的溶剂热法在水热反应器中成功合成了小粒径的 150-TiO 2 。在可见蓝光照射下，150-TiO 2本研究合成的催化剂在商业 P25、锐钛矿催化剂中表现出最好的催化活性和理想的产物选择性。此外，该催化剂对于催化氧化不同的芳香醇底物具有普遍性，包括有趣的吡啶醇，它们是制备吡啶醛和酮的高价值化学品。原位简易合成多相催化剂150-TiO 2不仅具有优异的稳定性和可回收性，还广泛拓展了绿色、原子效率、可持续的醇类光催化氧化在医药中间体中的应用。通过表征和结果分析，我们证实了TiO 2苯甲醇吸附形成表面配合物是实现可见光响应的关键，而TiO 2的高比表面积是实现高催化活性的关键。
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