Acid-durable intermetallic CaNi2Si2 catalyst with electron-rich Ni sites for aqueous phase hydrogenation of unsaturated organic anhydrides/acids

doi:10.1016/S1872-2067(23)64473-0

Abstract

Abstract:

The study of the aqueous-phase selective hydrogenation of maleic anhydride to succinic acid is important for expanding the coal chemical industry chain and promoting biomass conversion. The key lies in the development of highly efficient and stable non-noble metal catalysts. Herein, we report a novel intermetallic CaNi₂Si₂ catalyst with high activity and stability for the aqueous-phase selective hydrogenation of maleic anhydride. The results from the experiments and theoretical calculations demonstrated that the high catalytic performance was due to the synergy of the electron-rich Ni active sites, enhanced adsorption of C=C bonds, and favorable activation of H₂. The yield of succinic acid can be 100% over the CaNi₂Si₂ catalyst at the contact time of 5.4 g_cat/(mmol_reactant·min^-1) under 3 MPa and 120 °C in the continuous flow reactor. Furthermore, the special coordination environment and electronic structure of Ni in CaNi₂Si₂ inhibit the formation of carboxylates, thus enhancing the acid resistance in the reaction environment. The fine design and regulation of the structure of intermetallic silicides will be important references for the controllable optimization of maleic anhydride hydrogenation catalysts and provide new insights into the development of efficient and stable selective hydrogenation catalysts in harsh reaction environments.

Key words: CaNi₂Si₂, Intermetallic compound, Electron-rich Ni active site, Selective hydrogenation, Succinic acid

Shiyao Liu, Yutong Gong, Xiao Yang, Nannan Zhang, Huibin Liu, Changhai Liang, Xiao Chen. Acid-durable intermetallic CaNi₂Si₂ catalyst with electron-rich Ni sites for aqueous phase hydrogenation of unsaturated organic anhydrides/acids[J]. Chinese Journal of Catalysis, 2023, 50: 260-272.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64473-0

https://www.cjcatal.com/EN/Y2023/V50/I7/260

Figures/Tables 9

Fig. 1. (a) Schematic showing synthetic steps for CaNi2Si2 NPs. (b) Crystal structure and powder XRD pattern of CaNi2Si2 sample with Rietveld analysis. (c) WF (?) calculated from the measurement of secondary electron cut-off using UPS at a bias voltage of 6 V. H2-TPR (d) and H2-TPD (e) profiles of CaNi2Si2, Ni2Si, and Ni/SBA-15 samples.

Fig. 2. TEM (a), HRTEM (b), and HAADF-STEM (c) images with the corresponding EDS mappings of CaNi2Si2 sample.

Fig. 3. (a) XPS spectra of Ni 2p, Ca 2p, Si 2p, and O 1s of CaNi2Si2 after Ar+ sputtering. (b) Bader charges of CaNi2Si2 and 3D electron density isosurface map in the region from -0.5 eV to EF at 0.0025 A-3. (c) Calculated electronic DOS of CaNi2Si2 (112)-Ni and Ni metal (111)-Ni. The dotted lines are the d-band centers of CaNi2Si2 (112)-Ni (-1.35 eV) and Ni metal (111)-Ni (-1.06 eV), respectively.

Fig. 4. (a) Reaction pathway for the hydrogenation of MAn in the aqueous phase. (b) Comparison of the catalytic performance of different catalysts (CaNi2Si2, Ni2Si, CaSi2, Ni/SBA-15, and SBA-15). Effect of reaction temperature (c) and H2 pressure (d) on the hydrogenation of MAn in the aqueous phase over CaNi2Si2 (2.0 wt% of MAn aqueous and 0.2 g catalyst). (e) Product distribution for the hydrogenation of MAn in the aqueous phase over CaNi2Si2 catalyst at 3 MPa and 120 °C.

Fig. 5. Kinetic equilibrium constant (a-d) and Arrhenius plot (e) for aqueous phase hydrogenation of MAn (The Ea was estimated in the range of 60-120 °C for controlling the conversion of MAc below 30%).

Fig. 6. Stability tests of the CaNi2Si2 (a) and Ni/SBA-15 (b) for the aqueous-phase hydrogenation of MAn (The inset images display the photos of products at different reaction times and the fresh and spent catalysts).

Table 1 Hydrogenation of other unsaturated organic acids/anhydrides over CaNi2Si2.

Entry	Substrate	Product	pH	Reaction condition		Contact time (g_cat/(mmol·min^-1))	Conv. (%)	Sel. (%)
Entry	Substrate	Product	pH	T (°C)	P (MPa)	Contact time (g_cat/(mmol·min^-1))	Conv. (%)	Sel. (%)
1^a			2.52	100	1	14.4	100	100
2^a			2.64	120	3	2.1	100	99
3^a			2.33	120	3	4.5	100	99
4^a			1.81	120	3	8.4	92	100
5^a			2.04	240	3	4.5	98	95
6^b			1.95	120	3	5.0 h	100	97

Fig. 7. TPD (a) and TPSR (b) profiles of acrylic acid over the CaNi2Si2 catalyst. (c) DRIFT spectra of acrylic acid desorbed on CaNi2Si2 under Ar flow at 30, 50, and 100 °C. (d) DRIFT spectra of acrylic acid over the CaNi2Si2 catalyst in 10 vol% H2/Ar.

Fig. 8. DFT-calculated models of the carboxyl C=O bonds of acrylic acid on CaNi2Si2 (112)-top (a-d) and metallic Ni (111)-top (e-f).

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Acid-durable intermetallic CaNi₂Si₂ catalyst with electron-rich Ni sites for aqueous phase hydrogenation of unsaturated organic anhydrides/acids

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