Fine tuning the dynamic PdCx formation for enhanced acetylene semi-hydrogenation: The role of gas environment and ZnO addition

doi:10.1016/S1872-2067(24)60033-1

Abstract

Abstract:

Palladium carbide (PdC_x) has been extensively reported as active phase in acetylene semi-hydrogenation that can be dynamically formed during reaction. However, fine tuning of dynamic PdC_x formation towards enhanced acetylene semi-hydrogenation is of great challenge and the dynamic insights remain elusive. In this paper, the state-of-the-art in situ characterizations have been adopted to elucidate the dynamic PdC_x formation for acetylene semi-hydrogenation. The role of hydrogen atmosphere and ZnO addition in tuning the carburization process were clearly identified by in situ spectroscopies. The hydrogen in the gas environment assisted the carbon infiltration via PdH_x hydrides, while the addition of ZnO suppress the carburization by the surface Zn alloy. As a result, the carbon content in PdC_x can be precisely modulated by altering the hydrogen atmosphere and ZnO additives, and exhibits a linear correlation with the activity of acetylene semi-hydrogenation. The carbon insertion enriched the electron state of Pd sites in PdC_x that favors the activation of hydrogen for acetylene semi-hydrogenation. This work thus provides a new route for the design of Pd catalyst for high-performance acetylene semi-hydrogenation by fine tuning the reaction environment and the degree of carburization during dynamic PdC_x formation.

Key words: Acetylene semi-hydrogenation, Palladium carbide, Carburization process, In situ spectroscopy, Dynamic insight

Huan Chen, Zhounan Yu, Bing Yang, Yafeng Zhang, Chunxia Che, Xiaoyan Liu, Feng Zhang, Wei Han, He Wen, Aiqin Wang, Tao Zhang. Fine tuning the dynamic PdC_x formation for enhanced acetylene semi-hydrogenation: The role of gas environment and ZnO addition[J]. Chinese Journal of Catalysis, 2024, 60: 190-200.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60033-1

https://www.cjcatal.com/EN/Y2024/V60/I5/190

Figures/Tables 4

Fig. 1. In situ identification of dynamic PdCx formation. (a) In situ XRD patterns of PdO/Al2O3 sample during the in situ reduction-carburization process. (b?d) BF-STEM images of the typical structure transition of Pd species during in situ reduction-carburization process. The normalized in situ XANES spectra and EXAFS spectra in R-space at Pd K-edge for PdO/Al2O3 sample (e,f), and the evolution of Pd?Pd bond length during the in situ reduction-carburization process (g).

Fig. 2. The role of hydrogen atmosphere and ZnO additives for dynamic PdCx formation. (a) In situ XRD patterns of PdO/Al2O3 and PdO/ZnO/Al2O3 sample under reaction atmosphere with hydrogen or without hydrogen at 120 °C. BF-STEM images of PdZnAl-120 (b) and PdZnAl-N-120 (c) samples were obtained after carburization under reaction atmosphere at 120 °C. The dashed line indicates carbon deposition on particle surface. (d) Carbon content of palladium carbides formed on different samples after carburization at 120 °C. (e) In situ CO-DRIFTS on PdO/Al2O3 sample after treatment under reaction environment with hydrogen (red line) or without hydrogen (black line). (f) In situ CO-DRIFTS on PdO/ZnO/Al2O3 sample after treatment under reaction environment with hydrogen (red line) or without hydrogen (black line). (g) Schematic diagram of hydrogen assisted carbon insertion mechanism.

Fig. 3. Identification of surface Zn and its inhibition effect on carburization. In situ CO-DRIFTS on PdO/Al2O3 sample (a) and PdO/ZnO/Al2O3 sample (b) after in situ reduction-carburization pretreatment under reaction atmosphere with hydrogen at 120 °C. (c) Quasi in situ XPS spectra of Zn LMM of PdO/ZnO/Al2O3 sample under a hydrogen atmosphere. (d) Schematic diagram of in situ reduction-carburization process under different atmospheres and different supports.

Fig. 4. Catalytic performance and the fine tuning of carbon content for acetylene semi-hydrogenation. (a) Acetylene conversion on different catalysts. GHSV are denoted by parentheses in a unit of mL g?1 h?1. T = 80 °C. P = 0.1 MPa. (b) Comparison of acetylene selective hydrogenation mass activity of samples with different degrees of carburization. (c) The linear relationship between mass activity of acetylene semi-hydrogenation and carbon content of catalysts (Activity correction according to ICP results in Table S3). (d) H2-D2 exchange reaction at temperature of 25 °C for PdAl-120 sample carburized at 120 °C (red line) and PdAl-80 sample carburized at 80 °C (marine green line).

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