The effects of TiO2 crystal-plane-dependent Ir-TiOx interactions on the selective hydrogenation of crotonaldehyde over Ir/TiO2 catalysts

doi:10.1016/S1872-2067(21)63810-X

Abstract

Abstract:

Three supported Ir/TiO₂ catalysts, containing anatase TiO₂ nanocrystals with predominantly exposed {101}, {100}, and {001} planes, were subjected to various pre-treatments (H₂ reduction at different temperatures and O₂ re-oxidation) and then tested in the vapor phase selective hydrogenation of crotonaldehyde. The pre-treatments significantly altered the Ir-TiO_x interactions, including the morphologies and electronic properties of the Ir species and their surface acidity. These interactions were also closely related to the crystal planes of TiO₂, which further supported the observed reaction behaviors of the various Ir/TiO₂ catalysts. The best performance was obtained using the Ir/TiO₂-{101} catalyst pre-reduced at 300 °C, owing to its higher Ir⁰ surface concentration and moderate surface acidity compared to the other catalysts. Moreover, these findings indicated the synergistic role of the Ir-TiO_x interface in the reaction, as the interfacial sites were responsible for the adsorption/activation of H₂ and the C=O bond in the crotonaldehyde molecule. However, pre-reduction at 400 °C resulted in partial encapsulation of the Ir particles by TiO_x via strong metal-support interactions, which is unfavorable for the catalytic reaction owing to the loss of Ir-TiO_x interfacial sites.

Key words: Hydrogenation, α,β-unsaturated aldehyde, Ir/TiO₂, Metal-support interactions, Surface acidity

Aiping Jia, Yunshang Zhang, Tongyang Song, Yiming Hu, Wanbin Zheng, Mengfei Luo, Jiqing Lu, Weixin Huang. The effects of TiO₂ crystal-plane-dependent Ir-TiO_x interactions on the selective hydrogenation of crotonaldehyde over Ir/TiO₂ catalysts[J]. Chinese Journal of Catalysis, 2021, 42(10): 1742-1754.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63810-X

https://www.cjcatal.com/EN/Y2021/V42/I10/1742

Figures/Tables 12

Scheme 1. CRAL hydrogenation reaction pathways.

Fig. 1. HRTEM images and Ir particle size distributions for the Ir/TiO2-{101}, Ir/TiO2-{100}, and Ir/TiO2-{001} catalysts after the reduction pre-treatment at 200 °C (a1-a3), 300 °C (b1-b3), 400 °C (c1-c3), and reduction at 400 °C followed by re-oxidation at 300 °C (d1-d3).

Table 1 Physical properties of the various Ir-based catalysts.

Catalysts	d_VA^a /nm	Ir⁰/Ir^δ⁺ molar ratio ^b	Ir/Ti molar ratio		Surface Cl/Ti molar ratio ^e
Catalysts	d_VA^a /nm	Ir⁰/Ir^δ⁺ molar ratio ^b	Bulk ^c	Surface ^d	Calcined	Pre-treated
Ir/TiO₂-{101}-H200	1.0	1.5	0.012	0.038	0.037	0.012
Ir/TiO₂-{101}-H300	1.3	5.9	0.012	0.042	0.037	0.008
Ir/TiO₂-{101}-H400	1.4	3.0	0.012	0.036	0.037	0.002
Ir/TiO₂-{101}-H400+O300	1.5	0.4	0.012	0.039	0.037	0.001
Ir/TiO₂-{100}-H200	0.9	0.5	0.013	0.048	0.042	0.015
Ir/TiO₂-{100}-H300	1.3	2.5	0.013	0.055	0.042	0.007
Ir/TiO₂-{100}-H400	1.6	2.0	0.013	0.051	0.042	0.003
Ir/TiO₂-{100}-H400+O300	2.3	0.4	0.013	0.038	0.042	0.002
Ir/TiO₂-{001}-H200	1.3	0.7	0.012	0.044	0.042	0.016
Ir/TiO₂-{001}-H300	1.4	2.9	0.012	0.056	0.038	0.008
Ir/TiO₂-{001}-H400	1.5	2.3	0.012	0.050	0.038	0.003
Ir/TiO₂-{001}- H400+O300	2.0	0.7	0.012	0.037	0.038	0.002

Fig. 2. XPS spectra of the Ir 4f core level of the pre-treated Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts.

Fig. 3. In situ DRIFTS of CO adsorption on the pre-treated Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts at 30 °C.

Fig. 4. EPR spectra of Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts after conducting the various pre-treatments at 130 K. (Note: similar sample weights (~30 ± 1 mg) were used).

Fig. 5. NH3-TPD profiles of the pre-treated Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts.

Fig. 6. A comparison between the CRAL conversion, selectivity to CROL, CRAL reaction rates, and TOFs (turnover frequencies for CROL formation based on Ir dispersion) over the pre-treated Ir/TiO2-{101} (a,d), Ir/TiO2-{100} (b,f), and Ir/TiO2-{001} (c,e) catalysts after 30 min on stream. Reaction conditions: catalyst weight = 4.0 ± 0.1 mg; T = 80 °C; total flow rate = 26 mL min-1; CRAL concentration = 1 mol%.

Fig. 7. FTIR spectra of CRAL desorption at elevated temperatures from the pre-treated Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts between 1200 and 1800 cm-1.

Fig. 8. CRAL hydrogenation over the various pre-reduced Ir/TiO2-{101} (a), Ir/TiO2-{100} (b), and Ir/TiO2-{001} (c) catalysts at 30 °C between 1200 and 1800 cm-1.

Fig. 9. Evolution of the Ir particle size (a), Ir0/Irδ+ molar ratio (b), surface acidity (c), CRAL reaction rate (d), and TOF (e) of CROL formation for Ir/TiO2; (f) Selectivity to CROL over the pre-treated Ir/TiO2 catalysts.

Scheme 2. Proposed reaction mechanism for crotonaldehyde hydrogenation over the Ir/TiO2 catalysts.

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The effects of TiO₂ crystal-plane-dependent Ir-TiO_x interactions on the selective hydrogenation of crotonaldehyde over Ir/TiO₂ catalysts

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