Tuning Reaction Pathway of CO<sub>2</sub> Photoreduction via PtRu Bimetallic Microstructure Regulation

Hu, Songchang; Dong, Chunyang; Deng, Zesheng; Xing, Mingyang; Zhang, Jinlong

doi:10.1021/acs.jpcc.1c02769

Cited by 11 publications

(7 citation statements)

References 40 publications

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“…By far, TiO 2 -based materials continuously attract tremendous research attention − because of its natural abundance, low price, non-toxicity, and superior photostability. Many modification techniques, such as ion doping, − cocatalyst loading, − morphology control, − and phase transition, − were developed to enhance the photocatalytic efficiency. On the other hand, since the OER is known as the bottleneck in water splitting, mechanistic studies revealing the favorable OER pathway and/or kinetic trends are highly encouraged, holding the potential to locate and tackle fundamental problems hindering the overall performance.…”

Section: Introductionmentioning

confidence: 99%

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Chen

Gong

et al. 2022

ACS Catal.

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While the structure–function relationship is frequently referred in heterogeneous catalysis, the concept falls short of applications in photocatalysis owing to its complicated processes. Here, we take the photocatalytic oxygen evolution reaction (OER) as a case study and demonstrate the significance of subtle surface structures in altering the photooxidation functions of anatase and rutile TiO2 under aqueous environments. On the basis of our recent progresses in developing a solution simulation method and clarifying the photocatalytic OER process at rutile TiO2 (Nat. Catal. 2018, 1, 291–299), we successfully identified a complete OER mechanism at the water/anatase-TiO2(101) interface with an explicit involvement of photoholes/radicals and lattice oxygens. Kinetic analysis further revealed the leading reaction pathway varying with the concentration of surface-reaching photoholes (C h+), as well as the most efficient way to boost the OER via enriching the C h+ rather than lowering the reaction barriers (of water dissociation or O/O coupling). Anatase TiO2(101) generally shows poorer OER activity relative to the rutile TiO2(110) but much higher surface coverage of Ot – radicals under experimental conditions, rationalizing its good activity for photodegradation of organics. Such varied catalytic functions were found to be simply decided by the distance between two vicinal under-coordinated Ti cations on the surface that promotes or prohibits the key step of O/O coupling. These results not only provide essential understandings on the structure–function principles governing the photooxidation behaviors but also offer strategies to achieve efficient catalysis via matching proper surface structures with targeted reaction characteristics.

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Section: Introductionmentioning

confidence: 99%

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Chen

Gong

et al. 2022

ACS Catal.

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“…Therefore, the higher photocatalytic H 2 evolution activity of smaller PtRu NPs can be linked to improved charge separation and an increased number of active sites. [ 19,42,43 ] The monotonic relationship between the cocatalyst size and activity in this work implies the importance of the deposition in ensuring the small size of the cocatalyst (Figure 5E). These results highlight the utility of our colloidal approach for a controllable design and loading of ultrafine bimetallic NPs as HER cocatalysts for photocatalytic water splitting.…”

Section: Resultsmentioning

confidence: 73%

“…For instance, apart from improving charge separation and transfer efficiency, introducing Ru on Pt NPs promotes CO 2 photoreduction in PtRu/TiO 2 photocatalyst system to selectively generate CH 4 . [19] Indeed, a remarkable boost in photocatalytic H 2 production of PtRu-loaded Nb-doped TiO 2 is achieved even in the presence of oxidized Ru phases. [20] On the basis of these concepts, we present the application of PtRu solid-solution NPs as high-performance HER cocatalysts for SrTiO 3 :Al photocatalysts.…”

Section: Introductionmentioning

confidence: 99%

Bimetallic Synergy in Ultrafine Cocatalyst Alloy Nanoparticles for Efficient Photocatalytic Water Splitting

Pelicano

Saruyama

Takahata

et al. 2022

Adv Funct Materials

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Herein, PtRu solid‐solution alloy nanoparticles enable high‐performance H2 evolution reaction cocatalysts through the transfer of knowledge from electrocatalysis to photocatalysis. Ultrafine PtRu alloy nanoparticles (1.0 ± 0.2 nm in diameter) are synthesized by using a chemical polyol method and used for electro/photo‐catalyses. Integration of PtRu nanoparticles with carbon and Al‐doped SrTiO3 powders via liquid‐phase adsorption and successive two‐step air and H2 annealing ensures uniform deposition of PtRu alloy nanoparticles (<2 nm) with a solid‐solution structure. The PtRu alloy nanoparticles exhibit higher electrocatalytic activity for the hydrogen evolution reaction than monometallic Pt counterparts. Modifying Al‐doped SrTiO3 with PtRu alloy nanoparticles results in efficient photocatalytic overall water‐splitting activity with an apparent quantum yield of 65% at 365 nm and a solar‐to‐hydrogen energy conversion efficiency of 0.45%, which are the highest values among SrTiO3‐based photocatalytic water splitting systems with Rh‐free cocatalysts. Transient diffuse reflectance spectroscopy reveals that the PtRu nanoparticles have a superior electron‐capturing ability than the Pt counterparts, probably due to the decreased work function of Pt by alloying with Ru. This work establishes a framework to elucidate catalytic trends and provides rational design guidance toward the development of bimetallic solid‐solution nanoparticles as cost‐effective and highly active cocatalysts for overall water splitting.

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“…Until now, multiple energy production technical routes based on CO 2 conversion have been developed, including thermocatalysis, photocatalysis, electrocatalysis, photo-electrocatalysis, and biocatalysis. − Among them, solar light-driven CO 2 conversion used inexhaustible and cost-free solar energy as the only energy input. It can be performed under mild conditions, which is highly deserving for investigation.…”

Section: Introductionmentioning

confidence: 99%

Advances for CO₂ Photocatalytic Reduction in Porous Ti-Based Photocatalysts

Liu

et al. 2022

ACS EST Eng.

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The photoreduction of CO2 into high value-added fuels is a prospective approach for dealing with energy depletion and global warming from the root. Ti-based photocatalysts with porous structures have aroused wide concern due to the potential advantages like high specific surface area, cost-effective, earth-abundant, nontoxicity, and so on. This review presented the current achievements on porous TiO2, Ti-based zeolites, and Ti-based metal–organic frameworks for CO2 photoreduction. Multiple modification methods (such as heterojunction construction, cocatalyst modification, element doping, and surface adjustment) for optimizing the performance of these Ti-based materials are discussed. Finally, challenges and perspectives of porous Ti-based photocatalysts for CO2 photoreduction are proposed. This review is expected to provide directions for researchers to design and exploit more efficient materials for photoenergy conversion.

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Tuning Reaction Pathway of CO₂ Photoreduction via PtRu Bimetallic Microstructure Regulation

Cited by 11 publications

References 40 publications

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Bimetallic Synergy in Ultrafine Cocatalyst Alloy Nanoparticles for Efficient Photocatalytic Water Splitting

Advances for CO₂ Photocatalytic Reduction in Porous Ti-Based Photocatalysts

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Tuning Reaction Pathway of CO2 Photoreduction via PtRu Bimetallic Microstructure Regulation

Cited by 11 publications

References 40 publications

Subtle Structure Matters: The Vicinity of Surface Ti5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO2 under Aqueous Environments

Subtle Structure Matters: The Vicinity of Surface Ti5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO2 under Aqueous Environments

Bimetallic Synergy in Ultrafine Cocatalyst Alloy Nanoparticles for Efficient Photocatalytic Water Splitting

Advances for CO2 Photocatalytic Reduction in Porous Ti-Based Photocatalysts

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Tuning Reaction Pathway of CO₂ Photoreduction via PtRu Bimetallic Microstructure Regulation

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Subtle Structure Matters: The Vicinity of Surface Ti_5c Cations Alters the Photooxidation Behaviors of Anatase and Rutile TiO₂ under Aqueous Environments

Advances for CO₂ Photocatalytic Reduction in Porous Ti-Based Photocatalysts