Design of earth-abundant Ni3ZnC0.7@Ni@C catalyst for selective butadiene hydrogenation

doi:10.1016/S1872-2067(23)64641-8

Abstract

Abstract:

The pursuit of developing catalysts from earth-abundant materials to supplant those based on precious metals is of paramount importance in selective hydrogenations. While nickel-based systems have shown promise in the selective hydrogenation of butadiene, their practical applications are hampered by severe deactivation issues due to coke deposition and excessive hydrogenation. Here, a novel catalyst, Ni₃ZnC_0.7@Ni@C, is ingeniously engineered through the controlled oxidation of Ni₃ZnC_0.7@C. This catalyst is characterized by small Ni⁰ ensembles elegantly embellishing the Ni₃ZnC_0.7 nanoparticles, all encased within porous carbon shells. The evolutions of this catalyst, in terms of composition and structure during the oxidation process, is meticulously observed and characterized using a spectrum of advanced techniques. The Ni₃ZnC_0.7@Ni@C catalyst exhibits outstanding activity and stability in the hydrogenation of butadiene, surpassing other Ni-based systems, including its precursor Ni₃ZnC_0.7@C and other previously documented catalysts such as Ni₃InC_0.5 and the Ni₃In alloy. A pivotal finding of this research is the self-limiting behavior of coke deposition in the initial reaction stages. This intriguing phenomenon not only curbs further deactivation but also significantly enhances butene production, maintaining operational stability for an impressive duration of 80 hours. This discovery underscores the advantageous role of in situ generated 'soft' cokes in augmenting the selectivity and stability of the catalyst, which is particularly enlightening for other catalytic processes that are similarly afflicted by coking issues, thereby opening avenues for further in-depth investigations in this field.

Key words: Butadiene hydrogenation, Interstitial compound, Ni₃ZnC_0.7@Ni@C, Stability, Structural evolution

Zhibing Chen, Xintai Chen, Yali Lv, Xiaoling Mou, Jiahui Fan, Jingwei Li, Li Yan, Ronghe Lin, Yunjie Ding. Design of earth-abundant Ni₃ZnC_0.7@Ni@C catalyst for selective butadiene hydrogenation[J]. Chinese Journal of Catalysis, 2024, 60: 304-315.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64641-8

https://www.cjcatal.com/EN/Y2024/V60/I5/304

Figures/Tables 13

Fig. 1. Characterizations of Ni3ZnC0.7@C and Ni3InC0.5@C. (a) PXRD and STEM with elemental color mapping images: Ni3ZnC0.7@C (b?d) and Ni3InC0.5@C (e?g).

Fig. 2. PXRD patterns of fresh Ni3ZnC0.7@C and the oxidized samples (AT) (a) and after H2 reduction at 673 K (c). (b) The zoomed patterns in (a) at 2θ = 42°-44°. Vertical lines denote the reference standards. The reduced catalysts were denoted as Ni3ZnC0.7@C-H and AT-H.

Fig. 3. Raman spectra of Ni3ZnC0.7@C and the oxidized samples (AT) with or without H2 reduction.

Fig. 5. The Ar sputtering profiles of Ni 2p (a) and Zn 2p (b) XPS spectra of the H2 reduced A623.

Fig. 4. TEM (a,b) and HRTEM (c) images of A623-H.

Fig. 6. Evolutions of Ni3ZnC0.7@C subject to different oxidation and reduction treatments.

Fig. 7. Catalytic performance of different catalysts in BD hydrogenation. Conditions: Wcat = 50 mg, R673, Ftotal = 75 cm3 min-1, GHSV = 90000 cm3 gcat-1 h-1. (a,b) H2:BD = 50; (c,d) H2:BD = 10; (e,f) catalyst: A623.

Fig. 8. The stability performance of A623 in BD hydrogenation under different temperatures and H2:BD ratios. Conditions: Wcat = 50 mg, R673, Ftotal = 75 cm3 min-1, GHSV = 90000 cm3 gcat-1 h-1. (a) H2:BD = 5, T = 363 K; (b) H2:BD = 10, T = 323 K; (c) H2:BD = 7.5, T = 343 K.

Fig. 9. The radar plot connecting the performance descriptors of A623 in BD hydrogenation under different reaction conditions.

Fig. 10. The PXRD patterns of the reduced A623 and after stability tests at different reaction temperatures.

Fig. 11. The Raman spectra of the reduced A623 and after stability tests at different reaction temperatures.

Fig. 12. The TGA profiles (a) and the accompanied CO2 signals (b) for the reduced A623 and after stability tests at different reaction temperatures. The dashed line in (b) highlight the CO2 formation owing to coke deposits.

Fig. 13. A correlation of the deactivation rate of A623 with coke deposits from TGA.

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Design of earth-abundant Ni₃ZnC_0.7@Ni@C catalyst for selective butadiene hydrogenation

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