Photocatalytic Hydrogenation of Carbon Dioxide with High Selectivity to Methanol at Atmospheric Pressure

Wang, Lu; Ghoussoub, Mireille; Wang, Hong; Shao, Yue; Sun, Wei; Tountas, Athanasios A.; Wood, Thomas E.; Li, Hai; Loh, Joel Y. Y.; Dong, Yuchan; Xia, Meikun; Li, Young; Wang, Shenghua; Jia, Jia; Qiu, Chenyue; Qian, Chenxi; Kherani, Nazir P.; He, Le; Zhang, Xiaohong; Ozin, Geoffrey A.

doi:10.1016/j.joule.2018.03.007

Cited by 178 publications

(127 citation statements)

References 67 publications

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“…These results have implications for the design of In 2 O 3 based materials optoelectronic applications: Although the ubiquitous hydrogen species and adsorbed OH/oxygen groups do not affect the surface conductivity, their presence may have a strong influence on the optical transparency. In addition, while an n ‐type surface can be unwanted for a particular electronic application, it clearly proves to be beneficial in photocatalysis, enabling the reverse water‐gas‐shift and methanol production reactions . This appears to be particularly relevant for oxygen defect rich In 2 O 3 with nanometer scale particles with high surface to volume ratios .…”

Section: Resultsmentioning

confidence: 99%

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

Jovic

Moser

Papadogianni

et al. 2019

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Transparent conducting oxides (TCO) have integral and emerging roles in photovoltaic, thermoelectric energy conversion, and more recently, photocatalytic systems. The functional properties of TCOs, and thus their role in these applications, are often mediated by the bulk electronic band structure but are also strongly influenced by the electronic structure of the native surface 2D electron gas (2DEG), particularly under operating conditions. This study investigates the 2DEG, and its response to changes in chemistry, at the (111) surface of the model TCO In2O3, through angle resolved and core level X‐ray photoemission spectroscopy. It is found that the itinerant charge carriers of the 2DEG reside in two quantum well subbands penetrating up to 65 Å below the surface. The charge carrier concentration of this 2DEG, and thus the high surface n‐type conductivity, emerges from donor‐type oxygen vacancies of surface character and proves to be remarkably robust against surface absorbents and contamination. The optical transparency, however, may rely on the presence of ubiquitous surface adsorbed oxygen groups and hydrogen defect states that passivate localized oxygen vacancy states in the bandgap of In2O3.

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Section: Resultsmentioning

confidence: 99%

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

Jovic

Moser

Papadogianni

et al. 2019

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“…Es folgt ein verbotener direkter e-Übergang von einem O-2p-Orbital auf M-3d (M = Zn, Ga), gefolgt von der Übertragung photogenerierter Elektronen und Lçcher in den LDHs auf die Cu II -Zentren bzw.d as H-Atom. [149] In einem bei Atmosphärendruck und 250 8 8Cb etriebenen Durchflussreaktorsystem wurde mit und ohne UV/Vis-Bestrahlung eine Methanolproduktion von 97.3 bzw. Zum Verbessern der Photoaktivitätd er CO 2 -Reduktion wurden WO 3 und CuZnGa-LDH in eine reverse Polymerelektrolyt-Photobrennstoffzelle integriert.…”

Section: Lichtgetriebene Methanolerzeugungunclassified

Section: Mmol G Katunclassified

“…[148] Eine weitere Untersuchung zeigte,d ass defekthaltiges In 2 O 3 ,I n 2 O 3Àx (OH) y ,e ffizient die Hydrierung von CO 2 zu Methanol photokatalysieren kann (Abbildung 13 a,b). [149] In…”

Section: Angewandte Chemieunclassified

“…Copyright2 017, Nature Publishing Group.Abbildung 13. a) Geschwindigkeit und b) Selektivitätder Methanolerzeugung über einer In 2 O 3Àx (OH) y -Nanokristall-Überstruktur fürdie CO 2 -Hydrierung mit und ohne Sonnenbestrahlung. c) Reaktionsenergieprofil aus DFT-Rechnungen fürdie Methanolerzeugung durch CO 2 -Hydrierung über In 2 O 3Àx (OH) y .G enehmigte Wiedergabe [149]. Copyright 2018, Elsevier.…”

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Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie

et al. 2019

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Die katalytische C1‐Chemie auf der Grundlage der Aktivierung/Umwandlung von Synthesegas (CO+H2), Methan, Kohlendioxid und Methanol verfügt über enormes Potential für die Entwicklung nachhaltiger Kohlenwasserstoffbrennstoffe als Ersatz für Öl, Kohle und Erdgas. Herkömmliche thermisch‐katalytische Verfahren zur C1‐Umsetzung benötigen hohe Temperaturen und Drücke und sind daher mit einem großen CO2‐Fußabdruck verbunden. Dagegen bietet die solargetriebene C1‐Katalyse einen umweltfreundlichen und nachhaltigen Weg für die Herstellung von Brennstoffen und anderen chemischen Grundstoffen, wenn auch die Umwandlungseffizienzen noch zu niedrig für industrielle Wirtschaftlichkeit sind. In unserem Aufsatz beleuchten wir aktuelle Fortschritte und Meilensteine der C1‐Solarchemie, einschließlich der solaren Fischer‐Tropsch‐Synthese, Wassergas‐Shift‐Reaktion, CO2‐Hydrierung, Methan‐ und Methanolumwandlung. Ein besonderer Schwerpunkt liegt auf der rationalen Entwicklung von Katalysatoren, Struktur‐Reaktivitäts‐Beziehungen und Reaktionsmechanismen. Strategien für die Hochskalierung solargetriebener C1‐Verfahren werden ebenfalls diskutiert.

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Frustrated Lewis Pairs Accelerating CO₂ Reduction on Oxyhydroxide Photocatalysts with Surface Lattice Hydroxyls as a Solid‐State Proton Donor

Wang

Lü

Wang

et al. 2018

Adv Funct Materials

128

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Light-driven CO 2 reduction into high value-added product is a potential route to convert and store solar energy. Here, using the hydroxyls on an oxyhydroxide photocatalyst, CoGeO 2 (OH) 2 , as solid-state proton source to reduce the CO 2 into CH 4 is proposed. It is found that under irradiation, the lattice hydroxyls on surface of CoGeO 2 (OH) 2 are oxidized by photogenerated holes, resulting in the generation of oxygen vacancies (O Vs ) and protons. The photoinduced O Vs (Lewis acid) and its proximal surface hydroxyls (Lewis base) are more likely to form the frustrated Lewis acid-base pairs, which can capture, activate, and reduce CO 2 with the assistance of protons into CH 4 . The surface lattice hydroxyls are able to regenerate when the catalyst is exposed to the water molecule-containing atmosphere, thus achieving a sustainable CO 2 conversion. The proposed CO 2 reduction by self-breathing surface hydroxyls may open a new avenue to use photocatalysis for energy conversion.

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Photocatalytic Hydrogenation of Carbon Dioxide with High Selectivity to Methanol at Atmospheric Pressure

Abstract: Rod-like In 2 O 3Àx (OH) y nanocrystal superstructure enhanced solar methanol synthesis with a remarkable production rate (0.06 mmol g cat À1 h À1 ) and selectivity (50%) at atmospheric pressure.

Cited by 178 publications

References 67 publications

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie

Frustrated Lewis Pairs Accelerating CO₂ Reduction on Oxyhydroxide Photocatalysts with Surface Lattice Hydroxyls as a Solid‐State Proton Donor

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Photocatalytic Hydrogenation of Carbon Dioxide with High Selectivity to Methanol at Atmospheric Pressure

Abstract: Rod-like In 2 O 3Àx (OH) y nanocrystal superstructure enhanced solar methanol synthesis with a remarkable production rate (0.06 mmol g cat À1 h À1 ) and selectivity (50%) at atmospheric pressure.

Cited by 178 publications

References 67 publications

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C1‐Solarchemie

Frustrated Lewis Pairs Accelerating CO2 Reduction on Oxyhydroxide Photocatalysts with Surface Lattice Hydroxyls as a Solid‐State Proton Donor

Contact Info

Product

Resources

About

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie

Frustrated Lewis Pairs Accelerating CO₂ Reduction on Oxyhydroxide Photocatalysts with Surface Lattice Hydroxyls as a Solid‐State Proton Donor