Enhancing the chemoselective hydrogenation of nitroarenes: Designing a novel surface-strained carbon-based Pt nanocatalyst

doi:10.1016/S1872-2067(23)64424-9

Abstract

Abstract:

Supported Pt nanoparticles (NPs) are highly active catalysts for heterogeneous catalytic hydrogenation reactions; however, controlling their selectivity remains the biggest challenge toward their applicability. Herein, we propose the formation of a highly selective and stable, surface-strained Pt-based nanocatalyst via a facile and scalable thermal reduction treatment. Spherical-aberration-corrected transmission electron microscopy (SACTEM) and various spectral analytic techniques reveal a strong metal-support interaction between the Pt NPs and carbon nanotubes (CNTs) support during the annealing process. Thereafter, a fraction of carbon atoms is etched from the carbon-coated Pt NPs, inducing a compressive strain on the surface of the Pt NPs. Notably, the chemoselectivity of the surface-strained Pt/CNTs-800H catalyst (where 800 represents the heat-treatment temperature; H represents a hydrogen atmosphere) is almost completely different compared to that of its pristine counterpart. This catalyst is used for the hydrogenation reactions of a styrene and nitrobenzene mixture as well as 4-nitrostyrene. Interestingly, similar findings were observed with 5 wt% Pt/C and Pt/rGO catalysts, confirming that this treatment could be generalized. Hence, it has great potential in the design and synthesis of carbon-based catalytic materials.

Key words: Pt-based nanocatalyst, Thermal reduction treatment, Strong metal-support interaction, Compressive strain, Selective hydrogenation

Fengwei Zhang, Hefang Guo, Mengmeng Liu, Yang Zhao, Feng Hong, Jingjing Li, Zhengping Dong, Botao Qiao. Enhancing the chemoselective hydrogenation of nitroarenes: Designing a novel surface-strained carbon-based Pt nanocatalyst[J]. Chinese Journal of Catalysis, 2023, 48: 195-204.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64424-9

https://www.cjcatal.com/EN/Y2023/V48/I5/195

Figures/Tables 7

Scheme 1. Schematic diagram of the preparation of a compressive-strained Pt/CNTs-800H catalyst.

Fig. 1. TEM and HRTEM images of Pt/OCNTs (a,b) and Pt/CNTs-800H (c,d). (e) HAADF-STEM and the corresponding elemental mapping images. (f) SACTEM image of the Pt/CNTs-800H catalyst.

Fig. 2. XRD patterns (a) and XANES spectra (b) at the Pt K-edge of the Pt foil, Pt/C, and Pt/CNTs-800H. (c) Fourier-transform (FT) k3-weighted χ (k)-function of the EXAFS spectra for the Pt K-edge. Raman spectra (d) and N2 adsorption-desorption isotherms (e) of Pt-based catalysts prepared at different heat treatment temperatures. (f) In-situ DRIFT spectra of CO adsorption on Pt/OCNTs and Pt/CNTs-800H obtained at room temperature.

Fig. 3. HRTEM images (a-d) and high-resolution XPS analysis (e-h) in the Pt 4f region of the as-prepared Pt/CNTs-TH (from left to right: T = 200, 400, 600, and 800 °C, respectively).

Fig. 4. Reaction kinetics for the hydrogenation of the nitrobenzene and styrene mixture in the presence of Pt/CNTs-TH (T = 200 °C (a), 400 °C (b), 600 °C (c), and 800 °C (d)). Reaction conditions: 0.25 mmol styrene, 0.25 mmol nitrobenzene, 10 mg Pt-based catalyst, 40 °C, 0.1-0.3 MPa H2, and 5 mL EtOH.

Table 1 Selective hydrogenation of 4-nitrostyrene with different catalysts. a

Entry	Catalyst	P (MPa)	t (h)	Conv.^b (%)	Sel.^b (%)
1	Pt/OCNTs	0.1	1	>99	12.1
2	Pt/CNTs-200H	0.1	1	>99	27.3
3	Pt/CNTs-400H	0.1	1.5	>99	55.7
4	Pt/CNTs-600H	0.1	4	>99	60.8
5	Pt/CNTs-800H	0.3	8	91.4	89.2
6^c	Pt/CNTs-800H	0.1	7	94.8	81.1
7^d	Pt/CNTs-800Ar	0.3	24	76.5	69.5
8	5 wt% Pt/C	0.1	0.5	>99	—
9	5 wt% Pt/C-800H	0.1	1	>99	61.7
10	Pt/rGO	0.1	1	>99	1.5
11	Pt/rGO-800H	0.3	12	97.3	68.2

Table 2 Selective hydrogenation of a variety of nitroarenes with Pt/CNTs-800H. a

Entry	Time (h)	Conv. (%)^a	Sel. (%)^b
1	8	97.1	>99
2	6	98.2	>99
3 ^c	4	>99	>99
4 ^c	4	>99	>99
5	3	>99	>99
6	6	96.3	>99
7	8	92.5	>99
8	12	91.0	>99
9	12	>99	>99
10 ^c	8	91.4	89.2

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