Top-down fabrication of active interface between TiO2 and Pt nanoclusters. Part 2: Catalytic performance and reaction mechanism in CO oxidation

doi:10.1016/S1872-2067(23)64598-X

Abstract

Abstract:

In this work, following Part 1 that has found a redispersion process from Pt nanoparticles (NPs, about 3.4 nm) to nanoclusters (NCs, about 1 nm) on TiO₂ and elucidated its mechanism, we carefully investigated the catalytic performance of the obtained Pt NC catalyst in CO oxidation as well as the corresponding reaction mechanism. The Pt NC catalyst excels than its parent catalyst in terms of both intrinsic and apparent activity. Detailed studies by combining kinetic measurements, isotopic labeling reaction experiments, and low-temperature operando FT-IR unambiguously demonstrated that the Pt NCs deposited on TiO₂ can form unique interfacial sites that enable to active O₂ at very low temperature, thus the CO adsorbed on TiO₂ can diffuses to, and reacts with, the activated oxygen, rendering a high activity at low temperatures. This work is contributory in understanding the origin of the high activity of the supported metal cluster catalysts.

Key words: Heterogeneous catalysis, Nanocluster, Redispersion, Metal-oxide interface, CO oxidation

Xiaorui Du, Yike Huang, Xiaoli Pan, Xunzhu Jiang, Yang Su, Jingyi Yang, Yalin Guo, Bing Han, Chengyan Wen, Chenguang Wang, Botao Qiao. Top-down fabrication of active interface between TiO₂ and Pt nanoclusters. Part 2: Catalytic performance and reaction mechanism in CO oxidation[J]. Chinese Journal of Catalysis, 2024, 58: 247-254.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64598-X

https://www.cjcatal.com/EN/Y2024/V58/I3/247

Figures/Tables 8

Fig. 1. DRIFT spectra of CO adsorption at the saturation coverage on freshly synthesized Pt/TiO2-400 and Pt/TiO2-550 and the in situ reduced samples.

Fig. 2. Pt 4f XPS of Pt/TiO2-400 and Pt/TiO2-550 samples that reduced at 200 and 500 °C, respectively, under 10 vol% H2/He for 1 h at a flow rate of 30 mL min?1. The green peak represents the Ti 3s energy loss.

Fig. 3. Representative HAADF-STEM images and corresponding Pt size distributions of Pt/TiO2-400-H200 (a,b) and Pt/TiO2-550-H500 (c,d).

Fig. 4. (a) CO conversion as a function of reaction temperature on samples. (b) Repeated light-off curves for CO oxidation on Pt/TiO2-550-H500. (c) CO conversion with time-on-stream over Pt/TiO2-550-H500. Reaction condition: 1 vol% CO, 1 vol% O2, and balance He, gas flow 30 mL min?1; 20 mg catalyst; weight hourly space velocity (WHSV): 90000 mL gcat?1 h?1.

Fig. 5. Reaction rates (rCO, molCO gPt?1 h?1) as a function of CO (a) or O2 (b) concentration over catalysts at 80 °C; reaction orders were determined from the slope of each line.

Fig. 6. Isotopic labeling reaction experiment results over Pt/TiO2-400-H200 (a) and Pt/TiO2-550-H500 (b) samples; In each experiment, the in situ reduced catalyst was heated to 100 °C under He purge, then CO and isotopic 18O2 balanced with He was allowed to pass through for about 10 min followed by He purging until all the signals decreased to baseline level; Afterwards, 16O2 and CO balanced with He was introduced.

Fig. 7. The isotopic oxygen involved pulse reaction experiment results over Pt/TiO2-550-H500 at 100 °C (a,c) and room temperature (b,d), respectively. (a,b) the sample was firstly saturated by CO, followed by He purging until all the signals decreased to baseline level, then pulse of 18O2 introduced, after which mixed reactant gas (CO + 18O2 +He) was allowed to flow past. (c,d) the sample was firstly treated by 18O2 and then purged by He, passed by CO pulse, and mixed reactant gas (CO + 18O2 +He) was flow past afterwards.

Fig. 8. Evolution of operando FT-IR spectra at ?160 °C after introducing O2 to the CO pre-adsorbed Pt/TiO2-550-H500.

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Top-down fabrication of active interface between TiO₂ and Pt nanoclusters. Part 2: Catalytic performance and reaction mechanism in CO oxidation

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