In Situ Raman Monitoring and Manipulating of Interfacial Hydrogen Spillover by Precise Fabrication of Au/TiO<sub>2</sub>/Pt Sandwich Structures

Wei, Jie; Qin, Si‐Na; Liu, Jing‐Li; Ruan, Xiangyu; Guan, Zhiqiang; Yan, Hao; Wei, Di‐Ye; Zhang, Hua; Cheng, Jun; Xu, Hongxing; Zhang, Tian; Li, Jian‐Feng

doi:10.1002/ange.202000426

Cited by 57 publications

(7 citation statements)

References 51 publications

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“…Quantification of the H 2 -TPR curves (Supplementary Table 1 ) shows that the hydrogen consumed by NiO/Al 2 O 3 /Pt (1.86 mmol H 2 g –1 ) is greater than the sum of the hydrogen consumed by Al 2 O 3 /Pt (0.31 mmol H 2 g –1 ) and NiO/Al 2 O 3 (1.29 mmol H 2 g –1 ). These results demonstrate that the reduction of NiO species is promoted after Pt addition, which can be attributed to the hydrogen spillover effect 38 – 41 . This hydrogen spillover effect is further confirmed from the results of in situ quick XANES experiments under a H 2 atmosphere (0.6 MPa, 80 °C) (Supplementary Figs.…”

Section: Resultsmentioning

confidence: 71%

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

et al. 2022

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The contribution of the reverse spillover effect to hydrogen generation reactions is still controversial. Herein, the promotion functions for reverse spillover in the ammonia borane hydrolysis reaction are proven by constructing a spatially separated NiO/Al2O3/Pt bicomponent catalyst via atomic layer deposition and performing in situ quick X-ray absorption near-edge structure (XANES) characterization. For the NiO/Al2O3/Pt catalyst, NiO and Pt nanoparticles are attached to the outer and inner surfaces of Al2O3 nanotubes, respectively. In situ XANES results reveal that for ammonia borane hydrolysis, the H species generated at NiO sites spill across the support to the Pt sites reversely. The reverse spillover effects account for enhanced H2 generation rates for NiO/Al2O3/Pt. For the CoOx/Al2O3/Pt and NiO/TiO2/Pt catalysts, reverse spillover effects are also confirmed. We believe that an in-depth understanding of the reverse effects will be helpful to clarify the catalytic mechanisms and provide a guide for designing highly efficient catalysts for hydrogen generation reactions.

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Section: Resultsmentioning

confidence: 71%

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

et al. 2022

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“…57−59 It has been demonstrated that the hydrogen spillover between metal and oxide components can be precisely tuned by the intimacy between the neighboring components. 32,36 Here, a series of Co These Co 3 O 4 −ZnO catalysts are used for the CO 2 hydrogenation reaction and the effect of the intimacy between Co 3 O 4 and ZnO components on the catalytic performance is also investigated (Figures 6b and S17). During continuousflow CO 2 hydrogenation on Co 3 O 4 , a 140 min induction period can be observed where CO 2 conversion and CH 4 selectivity keep on increasing, suggesting that the catalyst state is evolving corresponding to the gradual reduction of CoO x to Co 0 (Figure S4b).…”

Section: Local Interfacial Confinementmentioning

confidence: 99%

Disentangling Local Interfacial Confinement and Remote Spillover Effects in Oxide–Oxide Interactions

Cheng

et al. 2023

J. Am. Chem. Soc.

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Supported oxides are widely used in many important catalytic reactions, in which the interaction between the oxide catalyst and oxide support is critical but still remains elusive. Here, we construct a chemically bonded oxide−oxide interface by chemical deposition of Co 3 O 4 onto ZnO powder (Co 3 O 4 /ZnO), in which complete reduction of Co 3 O 4 to Co 0 has been strongly impeded. It was revealed that the local interfacial confinement effect between Co oxide and the ZnO support helps to maintain a metastable CoO x state in CO 2 hydrogenation reaction, producing 93% CO. In contrast, a physically contacted oxide−oxide interface was formed by mechanically mixing Co 3 O 4 and ZnO powders (Co 3 O 4 −ZnO), in which reduction of Co 3 O 4 to Co 0 was significantly promoted, demonstrating a quick increase of CO 2 conversion to 45% and a high selectivity toward CH 4 (92%) in the CO 2 hydrogenation reaction. This interface effect is ascribed to unusual remote spillover of dissociated hydrogen species from ZnO nanoparticles to the neighboring Co oxide nanoparticles. This work clearly illustrates the equally important but opposite local and remote effects at the oxide−oxide interfaces. The distinct oxide− oxide interactions contribute to many diverse interface phenomena in oxide−oxide catalytic systems.

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“…Similarly, the route of hydrogen spillover has also been studied at the spatial resolution of 10 nm by the construction of sandwich nanocomposites (Figures 4C—E). [ 20 ] It demonstrated that hydrogen species could spill over at the interfaces of Pt‐TiO 2 ‐Au with high efficiency, and the maximum distance of hydrogen spillover on TiO 2 was 50 nm approximately. More importantly, we can adjust the selectivity of different reactions according to the different distances of hydrogen spillover.…”

Section: Applications Of Core‐shell Nanostructuresmentioning

confidence: 99%

Plasmonic Core‐Shell Nanostructures Enhanced Spectroscopies

et al. 2021

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Comprehensive Summary Core‐shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies, catalysis, energy, and other fields because of their splendid properties such as multifunctionality, stability, and adjustability. In this article, we summarized the endeavors made by our group in the past decade about the core‐shell nanostructures in the shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) and plasmon‐enhanced spectroscopies. Meanwhile, the potential challenges and perspectives about core‐shell nanostructures in spectroscopies have also been proposed. Thus, we believe this article would provide an avenue for a comprehensive understanding of enhanced spectroscopies with core‐shell nanostructures. What is the most favorite and original chemistry developed in your research group?? Core‐shell nanostructure enhanced Raman spectroscopy for surface analysis. How do you get into this specific field? Could you please share some experiences with our readers?? I started the studies on Raman spectroscopy since I was a Ph.D. candidate. I think most researchers should concentrate on specific fields, especially those that can hardly be solved by others, and make constant research on them. How do you supervise your students?? First, give highly challenging or unique topics to students. Then, make detailed plans for them and supervise them to execute the plans. What is the most important personality for scientific research?? Insistence and diligence. What are your hobbies? What's your favorite book(s)? Playing computer games. My favorite book is State of Divinity (笑傲江湖), by Louis Cha. What is your favorite journal(s)? The journals report systematic and pioneer works on chemistry, materials, or energy, etc.

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In Situ Raman Monitoring and Manipulating of Interfacial Hydrogen Spillover by Precise Fabrication of Au/TiO₂/Pt Sandwich Structures

Cited by 57 publications

References 51 publications

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

Disentangling Local Interfacial Confinement and Remote Spillover Effects in Oxide–Oxide Interactions

Plasmonic Core‐Shell Nanostructures Enhanced Spectroscopies

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In Situ Raman Monitoring and Manipulating of Interfacial Hydrogen Spillover by Precise Fabrication of Au/TiO2/Pt Sandwich Structures

Cited by 57 publications

References 51 publications

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

Enhanced hydrogen generation by reverse spillover effects over bicomponent catalysts

Disentangling Local Interfacial Confinement and Remote Spillover Effects in Oxide–Oxide Interactions

Plasmonic Core‐Shell Nanostructures Enhanced Spectroscopies

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In Situ Raman Monitoring and Manipulating of Interfacial Hydrogen Spillover by Precise Fabrication of Au/TiO₂/Pt Sandwich Structures