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Near 100% ethene selectivity achieved by tailoring dual active sites to isolate dehydrogenation and oxidation.

ABSTRACT: Prohibiting deep oxidation remains a challenging task in oxidative dehydrogenation of light alkane since the targeted alkene is more reactive than parent substrate. Here we tailor dual active sites to isolate dehydrogenation and oxidation instead of homogeneously active sites responsible for these two steps leading to consecutive oxidation of alkene. The introduction of HY zeolite with acid sites, three-dimensional pore structure and supercages gives rise to Ni²⁺ Lewis acid sites (LAS) and NiO nanoclusters confined in framework wherein catalytic dehydrogenation of ethane occurs on Ni²⁺ LAS resulting in the formation of ethene and hydrogen while NiO nanoclusters with decreased oxygen reactivity are responsible for selective oxidation of hydrogen rather than over-oxidizing ethene. Such tailored strategy achieves near 100% ethene selectivity and constitutes a promising basis for highly selective oxidation catalysis beyond oxidative dehydrogenation of light alkane.

SUBMITTER: Wang C

PROVIDER: S-EPMC8440631 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Near 100% ethene selectivity achieved by tailoring dual active sites to isolate dehydrogenation and oxidation.

Wang Chaojie C Yang Bing B Gu Qingqing Q Han Yujia Y Tian Ming M Su Yang Y Pan Xiaoli X Kang Yu Y Huang Chuande C Liu Hua H Liu Xiaoyan X Li Lin L Wang Xiaodong X

Nature communications 20210914 1

Prohibiting deep oxidation remains a challenging task in oxidative dehydrogenation of light alkane since the targeted alkene is more reactive than parent substrate. Here we tailor dual active sites to isolate dehydrogenation and oxidation instead of homogeneously active sites responsible for these two steps leading to consecutive oxidation of alkene. The introduction of HY zeolite with acid sites, three-dimensional pore structure and supercages gives rise to Ni<sup>2+</sup> Lewis acid sites (LAS ...[more]

PMID: 34521830

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Project description:Solid/liquid heterogeneous photocatalysis was often considered to occur on the active sites of a solid catalyst surface. Herein, we report that the selectivity of photocatalytic dehydrogenative oxidations of aliphatic primary alcohols in acetonitrile solution into corresponding aldehydes exhibits an anomalous relationship with adsorption behavior of the alcohols. By using Pt-loaded TiO2 photocatalyst in an inert atmosphere under UV light illumination, primary short-chain alcohols (SCAs) with strong adsorption were dehydrogenated into aldehydes in very poor selectivity, whereas weak-adsorbable long-chain alcohols (LCAs) were transformed into corresponding aldehydes with much higher selectivity. More than 20 examples of primary LCAs (C4-C10) were successfully transformed into their corresponding aldehydes with satisfactory selectivity and yield. Both solid-state magic-angle-spinning 13C NMR and attenuated total reflectance-Fourier transform infrared spectroscopy studies provided concrete differences in adsorption behaviors on the Pt-TiO2 photocatalyst surface between SCA ethanol and LCA n-octanol. To further uncover the mechanism for different selectivities of SCAs and LCAs in photodehydrogenation, in situ electron paramagnetic resonance (EPR) experiments (at 8 K temperature) were employed to observe the oxidation features of photogenerated hole in the valance band of Pt-TiO2 (hvb +). The EPR experimental studies exhibited that unlike ethanol, either n-octanol or solvent acetonitrile alone all could not scavenge photogenerated hvb + on Pt-P25 photocatalyst and only n-octanol dissolved in acetonitrile solvent could smoothly react with photoinduced hole. This indicated that selective oxidations of LCAs were achieved by solvent-delivered oxidation rather than directly destructive oxidation of photogenerated hvb +. Our results may open an alternative way in selective dehydrogenative oxidation of various substrates sensitive to both dioxygen and high-temperature treatments.

Dataset Information

Near 100% ethene selectivity achieved by tailoring dual active sites to isolate dehydrogenation and oxidation.

Publications

Near 100% ethene selectivity achieved by tailoring dual active sites to isolate dehydrogenation and oxidation.

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