Direct Evidence for Ethanol Dissociation on Rutile<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi>TiO</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:mo stretchy="false">(</mml:mo><mml:mn>110</mml:mn><mml:mo stretchy="false">)</mml:mo></mml:math>

Hansen, James D.; Huo, Peipei; Martinez, Umberto; Lira, Estephanía; Wei, Yinying; Streber, Regine; Lægsgaard, Erik; Hammer, Bjørk; Wendt, Stefan; Besenbacher, Flemming

doi:10.1103/physrevlett.107.136102

Cited by 61 publications

(110 citation statements)

References 33 publications

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“…However, after annealing Ru 0.07 TiO 2 at 700 • C, the catalytic activity decreased dramatically (entry 10), and the Lewis acid catalyzed products (o, m, p-benzyltoluenes and dibenzyl ether) were not produced by A-Ru 0.07 TiO 2 in the same reaction conditions. Based on the previous mechanistic studies using the single crystal of TiO 2 (typically rutile (110) surface) in vacuum conditions, the reactivity of alcohol on TiO 2 is strongly dependent on the surface defects of TiO 2 , such as oxygen vacant sites [35][36][37]. Besides the reduction of surface area and the aggregation of Ru into RuO 2 during annealing process, the decrease of the surface defects after annealing at 700 • C might result in the low reactivity of A-Ru 0.07 TiO 2 .…”

Section: Catalytic Testsmentioning

confidence: 99%

Dehydrogenative Oxidation of Alcohols Catalyzed by Highly Dispersed Ruthenium Incorporated Titanium Oxide

et al. 2016

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Ruthenium incorporated titanium oxides (Ru x TiO 2 ) were prepared by a one-step hydrothermal method using Ti(SO 4 ) 2 and RuCl 3 as the precursor of Ti and Ru, respectively. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), Energy-dispersive X-ray spectroscopy (EDS) mapping, and BET were applied for the analyses of catalysts. Ruthenium atoms are well dispersed in the anatase phase of TiO 2 and the crystallite size of Ru x TiO 2 (≈17 nm) is smaller than that of pure TiO 2 (≈45 nm). In particular, we found that our homemade pure TiO 2 exhibits a strong Lewis acid property. Therefore, the cooperation of ruthenium atoms playing a role in the hydride elimination and the Lewis acid site of TiO 2 can efficiently transfer primary alcohols into corresponding aldehydes in an oxidant-free condition.

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Section: Catalytic Testsmentioning

confidence: 99%

Dehydrogenative Oxidation of Alcohols Catalyzed by Highly Dispersed Ruthenium Incorporated Titanium Oxide

et al. 2016

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“…The spontaneous splitting of ethanol through O−H bond cleavage at the BBOv's has been directly imaged [14]. However, the adsorption of ethanol on the Ti 5c is debatable.…”

Section: Introductionmentioning

confidence: 99%

“…However, the adsorption of ethanol on the Ti 5c is debatable. Dissociative [12,15,16] and coexistence of both molecu-lar and dissociative [11,13,14] adsorption of ethanol on Ti 5c sites have been proposed. Most recently, TPD and DFT calculations in our laboratory have shown the most stable adsorption state of ethanol on Ti 5c sites is the molecular adsorption.…”

Section: Introductionmentioning

confidence: 99%

“…Therefore, a lot of surface science techniques have been used to study the fundamental aspects of this important system. For example, the thermal chemistry of ethanol on TiO 2 (110) has been examined by temperature programmed desorption (TPD) [11−13], scanning tunneling microscopy (STM) [14], X-ray photoelectron spectroscopy (XPS) [12,15], * Authors to whom correspondence should be addressed. E-mail: chuanyaozhou@dicp.ac.cn, xmyang@dicp.ac.cn and density functional theory (DFT) calculations [14,16].…”

Section: Introductionmentioning

confidence: 99%

“…For example, the thermal chemistry of ethanol on TiO 2 (110) has been examined by temperature programmed desorption (TPD) [11−13], scanning tunneling microscopy (STM) [14], X-ray photoelectron spectroscopy (XPS) [12,15], * Authors to whom correspondence should be addressed. E-mail: chuanyaozhou@dicp.ac.cn, xmyang@dicp.ac.cn and density functional theory (DFT) calculations [14,16]. The photoreaction of ethanol on TiO 2 (110) has also been investigated by TPD and XPS techniques [15,16].…”

Section: Introductionmentioning

confidence: 99%

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Kinetics and Dynamics of Photocatalyzed Dissociation of Ethanol on TiO2(110)

Zhou

Mao

et al. 2013

Chinese Journal of Chemical Physics

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The kinetics and dynamics of photocatalyzed dissociation of ethanol on TiO 2 (110) surface have been studied using the time-dependent and time-resolved femtosecond two-photon photoemission spectroscopy respectively, in order to unravel the photochemical properties of ethanol on this prototypical metal oxide surface. By monitoring the time evolution of the photoinduced excited state which is associated with the photocatalyzed dissociation of ethanol on Ti 5c sites of TiO 2 (110), the fractal-like kinetics of this surface photocatalytic reaction has been obtained. The measured photocatalytic dissociation rate on reduced TiO 2 (110) is faster than that on the oxidized surface. This is attributed to the larger defect density on the reduced surface which lowers the reaction barrier of the photocatalytic reaction at least methodologically. Possible reasons associated with the defect electrons for the acceleration have been discussed. By performing the interferometric two-pulse correlation on ethanol/TiO 2 (110) interface, the ultrafast electron dynamics of the excited state has been measured. The analyzed lifetime (24 fs) of the excited state is similar to that on methanol/TiO 2 (110). The appearance of the excited state provides a channel to mediate the electron transfer between the TiO 2 substrate and its environment. Therefore studying its ultrafast electron dynamics may lead to the understanding of the microscopic mechanism of photocatalysis and photoelectrochemical energy conversion on TiO 2 .

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Heterogeneous Photocatalytic Hydrogenative Reactions Using Liquid Hydrogen Donors: Mechanisms, Catalysts Design, and Applications

Zhang

2023

Chemistry A European J

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Heterogeneous photocatalysis is a promising approach for a wide range of hydrogenative reactions owing to the mild reaction conditions and the possibility of employing liquid hydrogen donors. Currently, the major interest is focused on the development of high performance photocatalyst materials and the expansion of reaction scope. An overview from a perspective of hydrogen donor and thus the related mechanistic understanding of the light‐induced hydrogenative reactions is rare. Here, we have categorized the photocatalytic hydrogenative reactions by the type of employed liquid hydrogen donors (hydrocarbons and water), discussed the basic criteria of hydrogen abstraction from these donors, and elaborated the design strategy of the photocatalyst materials.

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Direct Evidence for Ethanol Dissociation on RutileTiO2(110)

Cited by 61 publications

References 33 publications

Dehydrogenative Oxidation of Alcohols Catalyzed by Highly Dispersed Ruthenium Incorporated Titanium Oxide

Dehydrogenative Oxidation of Alcohols Catalyzed by Highly Dispersed Ruthenium Incorporated Titanium Oxide

Kinetics and Dynamics of Photocatalyzed Dissociation of Ethanol on TiO2(110)

Heterogeneous Photocatalytic Hydrogenative Reactions Using Liquid Hydrogen Donors: Mechanisms, Catalysts Design, and Applications

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