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Support stabilized PtCu single-atom alloys for propane dehydrogenation.

ABSTRACT: PtCu single-atom alloys (SAAs) open an extensive prospect for heterogeneous catalysis. However, as the host of SAAs, Cu suffers from severe sintering at elevated temperature, resulting in poor stability of catalysts. This paper describes the suppression of the agglomeration of Cu nanoparticles under high temperature conditions using copper phyllosilicate (CuSiO₃) as the support of PtCu SAAs. Based on quasi in situ XPS, in situ CO-DRIFTS, in situ Raman spectroscopy and in situ XRD, we demonstrated that the interfacial Cu⁺-O-Si formed upon reduction at 680 °C serves as the adhesive between Cu nanoparticles and the silicon dioxide matrix, strengthening the metal-support interaction. Consequently, the resistance to sintering of PtCu SAAs was improved, leading to high catalytic stability during propane dehydrogenation without sacrificing conversion and selectivity. The optimized PtCu SAA catalyst achieved more than 42% propane conversion and 93% propylene selectivity at 580 °C for at least 30 hours. It paves a way for the design and development of highly active supported single-atom alloy catalysts with excellent thermal stability.

SUBMITTER: Liu X

PROVIDER: S-EPMC9400610 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature

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Support stabilized PtCu single-atom alloys for propane dehydrogenation.

Liu Xiaohe X Wang Xianhui X Zhen Shiyu S Sun Guodong G Pei Chunlei C Zhao Zhi-Jian ZJ Gong Jinlong J

Chemical science 20220722 33

PtCu single-atom alloys (SAAs) open an extensive prospect for heterogeneous catalysis. However, as the host of SAAs, Cu suffers from severe sintering at elevated temperature, resulting in poor stability of catalysts. This paper describes the suppression of the agglomeration of Cu nanoparticles under high temperature conditions using copper phyllosilicate (CuSiO3) as the support of PtCu SAAs. Based on quasi in situ XPS, in situ CO-DRIFTS, in situ Raman spectroscopy ...[more]

PMID: 36091913

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Project description:Single atom alloys (SAAs) have gained remarkable attention due to their tunable properties leading to enhanced catalytic performance, such as high activity and selectivity. The stability of SAAs is dictated by surface segregation, which can be affected by the presence of surface adsorbates. Research efforts have primarily focused on the effect of commonly found catalytic reaction intermediates, such as CO and H, on the stability of SAAs. However, there is a knowledge gap in understanding the effect of ligands from colloidal nanoparticle (NP) synthesis on surface segregation. Herein, we combine density functional theory (DFT) and machine learning to investigate the effect of thiol and amine ligands on the stability of colloidal SAAs. DFT calculations revealed rich segregation energy (Eseg) data of SAAs with d8 (Pt, Pd, Ni) and d9 (Ag, Au, Cu) metals exposing (111) and (100) surfaces, in the presence and absence of ligands. Using these data, we developed an accurate four-feature neural network using a multilayer perceptron regression (NN MLP) model. The model captures the underlying physics behind surface segregation in the presence of adsorbed ligands by incorporating features representing the thermodynamic stability of metals through the bulk cohesive energy, structural effects using the coordination number of the dopant and the ligands, the binding strength of the adsorbate to the metals, strain effects using the Wigner-Seitz radius, and electronic effects through electron affinities. We found that the presence of ligands makes the thermodynamics of segregation milder compared to the bare (nonligated) SAA surfaces. Importantly, the adsorption configuration (e.g., top vs bridge) and the binding strength of the ligand to the SAA surface (e.g., amines vs thiols) play an important role in altering the Eseg trends compared to the bare surface. We also developed an accurate NN MLP model that predicts Eseg in the presence of ligands to find thermodynamically stable SAAs, leading to the rapid and efficient screening of colloidal SAAs. Our model captures several experimental observations and elucidates complex physics governing segregation at nanoscale interfaces.

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Support stabilized PtCu single-atom alloys for propane dehydrogenation.

Publications

Support stabilized PtCu single-atom alloys for propane dehydrogenation.

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