Promoting Catalytic Oxygen Activation by Localized Surface Plasmon Resonance: Effect of Visible Light Pre‐treatment and Bimetallic Interactions

Wong, Roong Jien; Tsounis, Constantine; Scott, Jason; Low, Gary; Amal, Rose

doi:10.1002/cctc.201701238

Cited by 10 publications

(6 citation statements)

References 34 publications

(77 reference statements)

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“…Consequently, the oxidation state of K may be an underlying reason behind the shifting selectivity due to changes in intermediate stability [52]. The proposed K to Ni electronic pathway agrees with the work function-driven electron transfer mechanism observed in our earlier works on bimetallic alloys [53,54], resulting in the decreased H 2 TPR peak for the reduction of Ni 2+ into Ni 0 .…”

Section: Role Of Potassium Substitution In Changing Reaction Selectivitysupporting

confidence: 87%

Tuning the Selectivity of LaNiO3 Perovskites for CO2 Hydrogenation through Potassium Substitution

et al. 2020

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Herein, we demonstrate a method used to tune the selectivity of LaNiO3 (LNO) perovskite catalysts through the substitution of La with K cations. LNO perovskites were synthesised using a simple sol-gel method, which exhibited 100% selectivity towards the methanation of CO2 at all temperatures investigated. La cations were partially replaced by K cations to varying degrees via control of precursor metal concentration during synthesis. It was demonstrated that the reaction selectivity between CO2 methanation and the reverse water gas shift (rWGS) could be tuned depending on the initial amount of K substituted. Tuning the selectivity (i.e., ratio of CH4 and CO products) between these reactions has been shown to be beneficial for downstream hydrocarbon reforming, while valorizing waste CO2. Spectroscopic and temperature-controlled desorption characterizations show that K incorporation on the catalyst surface decrease the stability of C-based intermediates, promoting the desorption of CO formed via the rWGS prior to methanation.

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Section: Role Of Potassium Substitution In Changing Reaction Selectivitysupporting

confidence: 87%

Tuning the Selectivity of LaNiO3 Perovskites for CO2 Hydrogenation through Potassium Substitution

et al. 2020

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“…Such a plasmonic effect is expected to enhance the photoactivity upon visible light illumination. 42,43 With the plasmonic Au-TiO 2 catalyst in hand, we started investigating the envisioned photocatalytic oxidation of organosilanes. Dimethylphenylsilane (1a) was used as a model substrate in the envisioned photocatalytic oxidation of silane (Figure 2).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…UV–vis diffuse reflectance spectroscopy of Au-TiO 2 showed a distinct absorption band occurring at approximately 560 nm compared to bare TiO 2 , which is associated with the localized surface plasmon resonance (LSPR) of Au nanoparticles (Figure S7). Such a plasmonic effect is expected to enhance the photoactivity upon visible light illumination. , …”

Section: Resultsmentioning

confidence: 99%

Highly Active and Selective Photocatalytic Oxidation of Organosilanes to Silanols

Chen

Duan

et al. 2022

ACS Sustainable Chem. Eng.

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Silanols are ubiquitous building blocks for organic synthesis and material fabrication. To date, a number of stoichiometric and catalytic methods have been developed for the direct oxidation of Si−H to Si−OH bonds. A common challenge in the oxidation of silanes is to combine both catalytic activity and selectivity. Herein, we report a highly active and selective photocatalytic approach for the oxidation of organosilanes to silanols. Using plasmonic Au-TiO 2 as a photocatalyst for dimethylphenylsilane oxidation enables complete conversion (>99% yield) and high selectivity (98.3%) with catalytic activity up to 121.8 g g −1 . The observed activity substantially exceeds those of most reported homogeneous and heterogeneous catalysts. Silanol synthesis could be achieved under mild conditions in either aqueous or solvent-free conditions and allows the oxidation of a broad scope of sterically hindered hydrosilanes in excellent yield and selectivity. The general concept of photocatalytic synthesis of valuable silanols is further demonstrated by five photocatalysts.

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“…As both Ni and Ag are known to be highly prone to uncontrolled oxidation when exposed to air without any protection measures, , the catalysts were passivated in a controlled oxidation step prior to XPS analysis. The change in oxidation states or local electron densities was then compared on the basis of other findings on the effect of light pretreatment on AuPt/TiO 2 . , The previous findings demonstrated that a higher electron density surface was more favorable to oxygen activation, leading to catalyst surface oxidation. Consequently, a catalyst with a more oxidized surface after passivation implies a higher electron density than in its original state.…”

Section: Resultsmentioning

confidence: 99%

Silver-Based Plasmonic Catalysts for Carbon Dioxide Reduction

García-García

Lovell

Wong

et al. 2020

ACS Sustainable Chem. Eng.

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Light-enhanced valorization of CO 2 provides a potentially useful pathway to offsetting carbon emissions to the atmosphere. Ni, a thermally active metal for the methanation of CO 2 , was coupled with Ag, a metal that exhibits a surface plasmon resonance effect in the visible light region, with the intention of exploiting the catalytic CO 2 conversion by Ni and light enhancement from Ag. The catalytic metals were loaded onto an insulating silica support and exposed to 405 nm laser light during the reaction. The impact of the Ni−Ag bimetallic interaction intimacy on the influence of the light illumination on CO 2 conversion and CH 4 selectivity was examined. Sequentially impregnating Ni and Ag (regardless of the order) provided a stronger bimetallic interaction relative to the coimpregnation procedure. The coimpregnated sample, with the weakest metallic interaction, exhibited the highest CH 4 productivity in the dark, while irradiating the catalyst at 405 nm had minimal impact on its performance. The poor photoeffect was attributed to the lack of interaction between Ni and Ag in conjunction with the low catalytic activity of Ag. The sequentially impregnated samples, which facilitated a stronger bimetallic interaction, exhibited an increase in CO 2 conversion when illuminated, with the greatest improvement produced when Ni was loaded first. The increase in CO 2 conversion under laser irradiation was attributed to the contribution of the Ag photoresponse. Comparing the three bimetallic catalysts clearly revealed that Ni−Ag/SiO 2 with the strongest bimetallic interaction delivered the highest photoenhancement in terms of both CO 2 conversion and CH 4 selectivity.

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Promoting Catalytic Oxygen Activation by Localized Surface Plasmon Resonance: Effect of Visible Light Pre‐treatment and Bimetallic Interactions

Cited by 10 publications

References 34 publications

Tuning the Selectivity of LaNiO3 Perovskites for CO2 Hydrogenation through Potassium Substitution

Tuning the Selectivity of LaNiO3 Perovskites for CO2 Hydrogenation through Potassium Substitution

Highly Active and Selective Photocatalytic Oxidation of Organosilanes to Silanols

Silver-Based Plasmonic Catalysts for Carbon Dioxide Reduction

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