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Activation of Molecular Oxygen for Alcohol Oxidation over Vanadium Carbon Catalysts Synthesized via the Heterogeneous Ligand Strategy
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-11-29 , DOI: 10.1021/acscatal.2c04601 Li Zhao 1, 2 , Piaoping Yang 3 , Song Shi 1, 3 , Guozhi Zhu 1 , Xiao Feng 1 , Weiqing Zheng 3 , Dionisios G. Vlachos 3 , Jie Xu 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-11-29 , DOI: 10.1021/acscatal.2c04601 Li Zhao 1, 2 , Piaoping Yang 3 , Song Shi 1, 3 , Guozhi Zhu 1 , Xiao Feng 1 , Weiqing Zheng 3 , Dionisios G. Vlachos 3 , Jie Xu 1
Affiliation
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Activation of molecular oxygen to realize selective oxidation is challenging. We employ a heterogeneous ligand method to prepare a vanadium carbon catalyst (V–C catalyst) of high efficiency in alcohol oxidation via oxygen activation. Principal component analysis revealed that the chemisorbed oxygen and pentavalent vanadium oxide are crucial in catalyst performance. Isotopic labeling, electron paramagnetic resonance, and control experiments confirmed that the V–C catalyst activates molecular oxygen to singlet oxygen or its analogue and carries out the reaction. A kinetic study and in situ React-IR spectra illustrated that the main reaction route is the O2 activation to 1O2 or its analogue and oxidizes the substrate through C–H bond activation. We demonstrate the efficiency of the V–C catalyst in selectively oxidizing the hydroxyl group in other substrates, including benzyl alcohols, methyl lactate, and ethyl lactate biomass-based alcohols. This will guide the development of highly active nonprecious metal catalysts for activating O2 for aerobic oxidation.
中文翻译：
通过多相配体策略合成的钒碳催化剂上分子氧的活化用于醇氧化
激活分子氧以实现选择性氧化具有挑战性。我们采用多相配体法制备了氧活化高效氧化醇的钒碳催化剂（V-C 催化剂）。主成分分析表明，化学吸附氧和五价氧化钒对催化剂性能至关重要。同位素标记、电子顺磁共振和对照实验证实，V-C催化剂将分子氧活化为单线态氧或其类似物并进行反应。动力学研究和原位 React-IR 光谱表明主要反应途径是 O 2活化为1 O 2或其类似物并通过 C-H 键激活氧化底物。我们证明了 V-C 催化剂在选择性氧化其他底物（包括苯甲醇、乳酸甲酯和乳酸乙酯生物质醇）中的羟基方面的效率。这将指导开发用于激活 O 2进行有氧氧化的高活性非贵金属催化剂。
更新日期：2022-11-29
中文翻译：
通过多相配体策略合成的钒碳催化剂上分子氧的活化用于醇氧化
激活分子氧以实现选择性氧化具有挑战性。我们采用多相配体法制备了氧活化高效氧化醇的钒碳催化剂（V-C 催化剂）。主成分分析表明，化学吸附氧和五价氧化钒对催化剂性能至关重要。同位素标记、电子顺磁共振和对照实验证实，V-C催化剂将分子氧活化为单线态氧或其类似物并进行反应。动力学研究和原位 React-IR 光谱表明主要反应途径是 O 2活化为1 O 2或其类似物并通过 C-H 键激活氧化底物。我们证明了 V-C 催化剂在选择性氧化其他底物（包括苯甲醇、乳酸甲酯和乳酸乙酯生物质醇）中的羟基方面的效率。这将指导开发用于激活 O 2进行有氧氧化的高活性非贵金属催化剂。
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