Mechanistic Study on the Selective Oxidation of Acrolein to Acrylic Acid: Identification of the Rate-Limiting Step via Perdeuterated Acrolein

Knoche Stefan; Heid Maurice; Gora Niklas; Ohlig Dominik; Drochner Alfons; Hess Christian; Etzold Bastian; Vogel Herbert

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Mechanistic Study on the Selective Oxidation of Acrolein to Acrylic Acid: Identification of the Rate-Limiting Step via Perdeuterated Acrolein

机译：丙烯醛对丙烯酸选择性氧化的机械研究：鉴定丙烯醛纯丙烯醛的速率限制步骤

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Gas phase oxidation of acrolein to acrylic acid on hydrothermally prepared Mo/V/W mixed oxides was investigated by isotopic labeling of acrolein. In this context, perdeuterated acrolein was synthesized for the first time and subsequently used for mechanistic studies. A clear kinetic isotopic effect (KIE) is observed referring to the alpha-hydrogen-abstraction as the rate-determining step in the selective acrolein oxidation. Furthermore, no change in the selectivity patterns is observed due to the perdeuteration, which confirms that the alpha-hydrogen-abstraction also acts as the rate-limiting step in the total oxidation of acrolein. Based on these KIE studies combined with additional experiments including D2O-SSITKA and temperature-programmed desorption, a detailed reaction mechanism for acrolein oxidation is proposed.

机译：丙烯醛的同位素标记研究了丙烯酸对水热制备的MO / V / W混合氧化物对丙烯酸的气相氧化。在这种情况下，首次合成备杂的丙烯醛并随后用于机械研究。将透明的动力学同位素效应（KIE）指观察到α-氢抽取作为选择性丙烯醛氧化中的速率确定步骤。此外，由于备注，不观察到选择性模式的变化，这证实了α-氢抽取还可作为丙烯醛总氧化的速率限制步骤。基于这些KIE研究结合了包括D2O-Ssitka和温度编程的解吸的附加实验，提出了一种对丙烯醛氧化的详细反应机理。

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来源
《ChemCatChem》 |2019年第14期|共11页
作者
Knoche Stefan; Heid Maurice; Gora Niklas; Ohlig Dominik; Drochner Alfons; Hess Christian; Etzold Bastian; Vogel Herbert;
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作者单位

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Eduard Zintl Inst Inst Anorgan &

Phys Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

Tech Univ Darmstadt Ernst Berl Inst Tech &

Makromol Chem Alarich Weiss Str 8 D-64287 Darmstadt Germany;

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正文语种 eng
中图分类物理化学（理论化学）、化学物理学;
关键词
Acrylic acid; Deuteration; Isotopic labeling; Kinetic isotopic effect; Mo-V-oxides;

机译：丙烯酸;氘;同位素标记;动力学同位素效果;MO-V氧化物;

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1. Mechanistic Study on the Selective Oxidation of Acrolein to Acrylic Acid: Identification of the Rate-Limiting Step via Perdeuterated Acrolein [J] . Knoche Stefan, Heid Maurice, Gora Niklas, ChemCatChem . 2019,第14期

机译：丙烯醛对丙烯酸选择性氧化的机械研究：鉴定丙烯醛纯丙烯醛的速率限制步骤
2. Novel Mo-V Oxide Catalysts with Nanospheres as Templates for the Selective Oxidation of Acrolein to Acrylic Acid [J] . Wang Weihua, Xu Wenjie, Song Weilin, Catalysis Letters . 2021,第8期

机译：具有纳米球的新型Mo-V氧化物催化剂作为模板，用于选择性氧化丙烯酸至丙烯酸
3. Characterization of V-W and Mo-W Mixed Oxide Catalysts for the Selective Oxidation of Acrolein to Acrylic Acid [J] . C.Schmitt, L.Giebeler, R.Schierholz Zeitschrift fur Physikalische Chemie: International Journal of Research in Physical Chemistry and Chemical Physics . 2007,第11a12期

机译：用于丙烯醛选择性氧化为丙烯酸的V-W和Mo-W混合氧化物催化剂的表征
4. Effects of W on the selective oxidation of acrolein to acrylic acid over orthorhombic and trigonal Mo-V-W-0 [C] . Chuntian Qiu, Satoshi Ishikawa, Toru Murayama 旭川大会石油・石油化学討論会 . 2014

机译：W对正交和三角形MO-V-W-0丙烯酸对丙烯酸对丙烯酸选择性氧化的影响
5. Operando spectroscopic and kinetic study of the selective oxidation of propylene to acrolein over well-defined supported vanadium oxide catalysts [D] . Zhao, Chunli 2007

机译：明确定义的负载型钒氧化物催化剂上丙烯选择性氧化为丙烯醛的操作光谱和动力学研究
6. Nucleotide excision repair deficiency increases levels of acrolein-derived cyclic DNA adduct and sensitizes cells to apoptosis induced by docosahexaenoic acid and acrolein [O] . Jishen Pan, Elizabeth Sinclair, Zhuoli Xuan, -1

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7. Mechanistic Study on the Selective Oxidation of Acrolein to Acrylic Acid concerning the Role of Water [O] . Stefan Knoche, Maurice Heid, Niklas Gora, 2020

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8. Chemical Characterization of the Smokes of Selected US Commercial Cigarettes: Tar, Nicotine, Carbon Monoxide, Oxides of Nitrogen, Hydrogen Cyanide, and Acrolein (32 Brands). [R] . Jenkins, R. A., White, S. K., Griest, W. H., 1983

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Mechanistic Study on the Selective Oxidation of Acrolein to Acrylic Acid: Identification of the Rate-Limiting Step via Perdeuterated Acrolein

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