Inhibition of H2 and O2 Recombination: The Key to a Most Efficient Single‐Atom Co‐Catalyst for Photocatalytic H2 Evolution from Plain Water

Hwang, Imgon; Mazare, Anca; Will, Johannes; Yokosawa, Tadahiro; Spiecker, Erdmann; Schmuki, Patrik

doi:10.1002/adfm.202207849

Cited by 33 publications

(17 citation statements)

References 93 publications

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“…In photocatalytic H 2 production, TiO 2 needs to be decorated with a suitable co-catalyst such as Pt. 11,12 As such, TiO 2 has sufficient surface oxo groups for SA-trapping. 13−16 However, it is still challenging to stabilize many noble metals as SAs on TiO 2 surfaces because of the relatively weak bonding between oxo groups and most noble metal SAs.…”

Section: ■ Introductionmentioning

confidence: 99%

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Hwang

Osuagwu

et al. 2022

ACS Catal.

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Trapping sites in single atom (SA) catalysts are critical to the stabilization and reactivity of isolated atoms. Herein, we show that anchoring of Pt SAs on TiO 2 nanosheets is strongly aided by lattice incorporated fluorine species. Tailoring the speciation of fluorine on TiO 2 nanosheets is a key factor for uniform and stable dispersion of the Pt SAs and high efficiency in Pt SA co-catalyzed photocatalytic H 2 production. Fluorinestabilized uniformly dispersed Pt SAs on the (001) surface of TiO 2 can provide a remarkable photocatalytic activity (a H 2 production rate of 45.3 mmol h −1 mg −1 Pt for 65 mW/cm 2 365 nm light). This high (maximized) efficiency can be achieved with a remarkably low loading amount of Pt SAs on TiO 2 nanosheets (0.03 wt %), which is far superior to Pt nanoparticles on a TiO 2 nanosheet with the same or a higher loading amount. F-stabilized Pt SAs on TiO 2 nanosheets also exhibit an excellent stability in long-term photocatalytic reactions.

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Section: ■ Introductionmentioning

confidence: 99%

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Hwang

Osuagwu

et al. 2022

ACS Catal.

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“…TiO 2 , as one of the most mature semiconductor materials, has the advantages of stability, cheapness, and environmentally friendly and is also a potential support for anchoring SAs. [68] Introducing defects in TiO 2 can improve the stability and activity of SACs. [33,[69][70][71] TiO 2 with oxygen-vacancy-rich defects exhibited superior photocatalytic hydrogen production and CO 2 reduction performance than original TiO 2 at the same Pt SAs loading.…”

Section: Metal Oxides/sulfidesmentioning

confidence: 99%

Recent Progress of Single‐Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Pan

Zhang

et al. 2023

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Photocatalysis driven by solar energy is a feasible strategy to alleviate energy crises and environmental problems. In recent years, significant progress has been made in developing advanced photocatalysts for efficient solar‐to‐chemical energy conversion. Single‐atom catalysts have the advantages of highly dispersed active sites, maximum atomic utilization, unique coordination environment, and electronic structure, which have become a research hotspot in heterogeneous photocatalysis. This paper introduces the potential supports, preparation, and characterization methods of single‐atom photocatalysts in detail. Subsequently, the fascinating effects of single‐atom photocatalysts on three critical steps of photocatalysis (the absorption of incident light to produce electron‐hole pairs, carrier separation and migration, and interface reactions) are analyzed. At the same time, the applications of single‐atom photocatalysts in energy conversion and environmental protection (CO2 reduction, water splitting, N2 fixation, organic macromolecule reforming, air pollutant removal, and water pollutant degradation) are systematically summarized. Finally, the opportunities and challenges of single‐atom catalysts in heterogeneous photocatalysis are discussed. It is hoped that this work can provide insights into the design, synthesis, and application of single‐atom photocatalysts and promote the development of high‐performance photocatalytic systems.

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“…Interestingly, it has been reported that noble metal co-catalysts can catalyze the backward reaction between H 2 and O 2 . However, when noble metals are present in the form of single atoms, they hinder this recombination process, thus potentially improving the overall efficiency of water splitting …”

Section: Introductionmentioning

confidence: 99%

“…However, when noble metals are present in the form of single atoms, they hinder this recombination process, thus potentially improving the overall efficiency of water splitting. 14 Various methods have been proposed to synthesize SACs, including bath deposition, vapor deposition, atomic layer deposition (ALD), 15−17 co-precipitation, 18,19 and wet-chemical synthesis such as impregnation and photo deposition. 20−22 A promising and straightforward strategy for anchoring single atoms (SAs) onto suitable support materials involves nanoand atomic-scale defect engineering.…”

Section: Introductionmentioning

confidence: 99%

Ultrasound-Driven Defect Engineering in TiO_2–x Nanotubes─Toward Highly Efficient Platinum Single Atom-Enhanced Photocatalytic Water Splitting

Shahrezaei

Hejazi

Šedajová

et al. 2023

ACS Appl. Mater. Interfaces

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Single-atom catalysts (SACs) have demonstrated superior catalytic activity and selectivity compared to nanoparticle catalysts due to their high reactivity and atom efficiency. However, stabilizing SACs within hosting substrates and their controllable loading preventing single atom clustering remain the key challenges in this field. Moreover, the direct comparison of (co-) catalytic effect of single atoms vs nanoparticles is still highly challenging. Here, we present a novel ultrasound-driven strategy for stabilizing Pt single-atomic sites over highly ordered TiO 2 nanotubes. This controllable low-temperature defect engineering enables entrapment of platinum single atoms and controlling their content through the reaction time of consequent chemical impregnation. The novel methodology enables achieving nearly 50 times higher normalized hydrogen evolution compared to pristine titania nanotubes. Moreover, the developed procedure allows the decoration of titania also with ultrasmall nanoparticles through a longer impregnation time of the substrate in a very dilute hexachloroplatinic acid solution. The comparison shows a 10 times higher normalized hydrogen production of platinum single atoms compared to nanoparticles. The mechanistic study shows that the novel approach creates homogeneously distributed defects, such as oxygen vacancies and Ti 3+ species, which effectively trap and stabilize Pt 2+ and Pt 4+ single atoms. The optimized platinum singleatom photocatalyst shows excellent performance of photocatalytic water splitting and hydrogen evolution under one sun solarsimulated light, with TOF values being one order of magnitude higher compared to those of traditional thermal reduction-based methods. The single-atom engineering based on the creation of ultrasound-triggered chemical traps provides a pathway for controllable assembling stable and highly active single-atomic site catalysts on metal oxide support layers.

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Inhibition of H₂ and O₂ Recombination: The Key to a Most Efficient Single‐Atom Co‐Catalyst for Photocatalytic H₂ Evolution from Plain Water

Cited by 33 publications

References 93 publications

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Recent Progress of Single‐Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Ultrasound-Driven Defect Engineering in TiO_2–x Nanotubes─Toward Highly Efficient Platinum Single Atom-Enhanced Photocatalytic Water Splitting

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Inhibition of H2 and O2 Recombination: The Key to a Most Efficient Single‐Atom Co‐Catalyst for Photocatalytic H2 Evolution from Plain Water

Cited by 33 publications

References 93 publications

Fluorine Aided Stabilization of Pt Single Atoms on TiO2 Nanosheets and Strongly Enhanced Photocatalytic H2 Evolution

Fluorine Aided Stabilization of Pt Single Atoms on TiO2 Nanosheets and Strongly Enhanced Photocatalytic H2 Evolution

Recent Progress of Single‐Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Ultrasound-Driven Defect Engineering in TiO2–x Nanotubes─Toward Highly Efficient Platinum Single Atom-Enhanced Photocatalytic Water Splitting

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Product

Resources

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Inhibition of H₂ and O₂ Recombination: The Key to a Most Efficient Single‐Atom Co‐Catalyst for Photocatalytic H₂ Evolution from Plain Water

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Fluorine Aided Stabilization of Pt Single Atoms on TiO₂ Nanosheets and Strongly Enhanced Photocatalytic H₂ Evolution

Ultrasound-Driven Defect Engineering in TiO_2–x Nanotubes─Toward Highly Efficient Platinum Single Atom-Enhanced Photocatalytic Water Splitting