Photomethanation of Gaseous CO<sub>2</sub> over Ru/Silicon Nanowire Catalysts with Visible and Near‐Infrared Photons

O’Brien, Paul G.; Sandhel, Amit; Wood, Thomas E.; Jelle, Abdinoor A.; Hoch, Laura; Perović, D. D.; Mims, Charles A.; Ozin, Geoffrey A.

doi:10.1002/advs.201400001

Cited by 152 publications

(110 citation statements)

References 44 publications

(74 reference statements)

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“…Since that time the photoreduction of CO 2 by H 2 O or H 2 have been studied in the aqueous and gas phase using almost every conceivable nanostructured composition imaginable3246474849. While CO 2 conversion rates and efficiencies of reported photocatalysts are still orders of magnitude below those required to inspire technological development5051, progress towards achieving this objective has been steady and promising.…”

Section: Discussionmentioning

confidence: 99%

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Sun

Qian

et al. 2016

Nat Commun

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Silicon constitutes 28% of the earth's mass. Its high abundance, lack of toxicity and low cost coupled with its electrical and optical properties, make silicon unique among the semiconductors for converting sunlight into electricity. In the quest for semiconductors that can make chemicals and fuels from sunlight and carbon dioxide, unfortunately the best performers are invariably made from rare and expensive elements. Here we report the observation that hydride-terminated silicon nanocrystals with average diameter 3.5 nm, denoted ncSi:H, can function as a single component heterogeneous reducing agent for converting gaseous carbon dioxide selectively to carbon monoxide, at a rate of hundreds of μmol h−1 g−1. The large surface area, broadband visible to near infrared light harvesting and reducing power of SiH surface sites of ncSi:H, together play key roles in this conversion. Making use of the reducing power of nanostructured hydrides towards gaseous carbon dioxide is a conceptually distinct and commercially interesting strategy for making fuels directly from sunlight.

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Section: Discussionmentioning

confidence: 99%

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Sun

Qian

et al. 2016

Nat Commun

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“…catalysts [11,12]. A further step in this sense would be the use of H 2 O instead of H 2 as the reducing agent, in essence mimicking the activation route of natural photosynthesis.…”

Section: Introductionmentioning

confidence: 99%

Copper-doped titania photocatalysts for simultaneous reduction of CO2 and production of H2 from aqueous sulfide

Gonell

Puga

Julián‐López

et al. 2016

Applied Catalysis B: Environmental

104

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Copper-doped titanium dioxide materials with anatase phase (Cu-TiO 2 , atomic Cu contents ranging from 0 to 3% relative to the sum of Cu and Ti), and particle sizes of 12-15 nm, were synthesised by a solvo-thermal method using ethanol as the solvent and small amounts of water to promote the hydrolysis-condensation processes. Diffuse reflectance UV-vis spectroscopy show that the edges of absorption of the titania materials are somewhat shifted to higher wavelengths due to the presence of Cu. X-Ray Photoelectron Spectroscopy (XPS) indicate that Cu(II) is predominant. Photocatalytic CO 2 reduction experiments were performed in aqueous Cu-TiO 2 suspensions under UV-rich light and in the presence of different solutes. Sulfide was found to promote the efficient production of H 2 from water and formic acid from CO 2 . The effect of the Cu content on the photoactivity of Cu-TiO 2 was also studied, showing that copper plays a role on the photocatalytic reduction of CO 2 . IntroductionCarbon dioxide is an inexpensive and widely available feedstock. Its use for the production of chemicals is doubly beneficial, since in addition to its availability, it would represent a decrease in the carbon footprint for the manufacturing of the particular chemical. Other researchers have reported lower but noticeable methanol yields using similarly prepared photocatalysts and Hg lamp irradiation (10-23 µmol g cat −1 h −1 ) [19,20]. In gas-phase reactions, the formation of methanol was also reported, but in considerably lower yields (2 nmol g cat −1 h −1 ), being methane the major product formed by Cu/TiO 2 photocatalysis [21]. In contrast, similar materials were found to promote the formation of several hydrocarbons including methane, ethane and ethylene in conjunction with larger amounts of H 2 [22], whereas CO and methane were major products found in a more recent study [23]. A significant degree of discrepancy regarding the identity of the reaction products (in addition to their selectivities and yields) is apparent by considering the aforementioned literature data, although this could be in part due to the different synthetic procedures used for the preparation of the photocatalysts and to the varied irradiation conditions used.Despite the notable progress in this field of research, there is no clear trend which may allow to conclude on the actual mechanistic route and to gain knowledge on the role of copper on the reaction. Thorough kinetic and in situ spectroscopic studies would provide valuable information on the reaction at the surface of the photocatalyst and may guide future design of more active copper-titania materials. An important issue to focus on is the possible back-reactions of the reduction products on the photocatalyst. For example, it was observed that methanol and formaldehyde, initially formed by a photocatalytic process using Cu(0) powder and TiO 2 , were 3 rapidly consumed by in situ formed Cu/TiO 2 [24]. The simultaneous occurrence of CO 2 reduction and decomposition of the products should result in stat...

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“…In line with the use of ruthenium catalysts for light-promoted methanation of CO2, Ozin and coworkers have recently reported the preparation of novel Ru/Si nanomaterials whereby ruthenium was deposited in the form of small nanoparticles by sputtering on silicon nanowires [49]. These materials outperformed counterparts based on silicon wafer supports (990 and 140 µmol gcat −1 h −1 , respectively, see Table 3), presumably as a consequence of a superior light absorbance.…”

Section: Light-promoted Methanation Of Co2mentioning

confidence: 95%

“…With these evidences in hand, the process was claimed to be genuinely promoted, at least in part, by photocatalysis [49].…”

Section: Light-promoted Methanation Of Co2mentioning

confidence: 99%

Light-Promoted Hydrogenation of Carbon Dioxide—An Overview

Puga

2016

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Photomethanation of Gaseous CO₂ over Ru/Silicon Nanowire Catalysts with Visible and Near‐Infrared Photons

Cited by 152 publications

References 44 publications

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Copper-doped titania photocatalysts for simultaneous reduction of CO2 and production of H2 from aqueous sulfide

Light-Promoted Hydrogenation of Carbon Dioxide—An Overview

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Photomethanation of Gaseous CO2 over Ru/Silicon Nanowire Catalysts with Visible and Near‐Infrared Photons

Cited by 152 publications

References 44 publications

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Heterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals

Copper-doped titania photocatalysts for simultaneous reduction of CO2 and production of H2 from aqueous sulfide

Light-Promoted Hydrogenation of Carbon Dioxide—An Overview

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Photomethanation of Gaseous CO₂ over Ru/Silicon Nanowire Catalysts with Visible and Near‐Infrared Photons