Статья

Concerted catalysis of single atom and nanocluster enhances bio-ethanol activation and dehydrogenation

Zhao SunHunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering, Central South University, Changsha, 410083, ChinaWeizhi ShiHunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering, Central South University, Changsha, 410083, ChinaLouise R. SmithHunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering, Central South University, Changsha, 410083, ChinaNicholas F. DummerMax Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff, CF24 4HQ, United KingdomHaifeng QiMax Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff, CF24 4HQ, United KingdomZhiqiang SunMax Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff, CF24 4HQ, United KingdomGraham J. HutchingsHunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering, Central South University, Changsha, 410083, China

2025en

ABI

Аннотация

Abstract Single atom and nanocluster catalysts are extensively investigated in heterogeneous catalysis due to their high catalytic activity and atomic utilization, while their coexisting properties and potentially synergistic effect are yet to be clarified. Herein, we construct three systems of atomic-scale catalysts ( x Ni/Mo 2 TiAlC 2 , x = 0.5, 1, and 1.5) for bio-ethanol reforming, which correspond to single atoms, single atoms mixed with nanoclusters, and nanoclusters. The respective hydrogen utilization efficiency of mixed-form catalyst increases by 43.7% and 29.3% compared to single atom and nanocluster catalysts. Results demonstrate that the adjacent Ni single atom facilitates electron transfer from Mo 2 TiAlC 2 to Ni-Mo interface and raises the d-band center, thus enhancing bio-ethanol adsorption and activation; while the existence of Ni nanoclusters contributes to lowering the energy barriers of CH 3 CHO* dehydrogenation. The catalytically active sites are Ni-Mo alloyed single atoms with adjacent Ni nanoclusters. This work provides new implications for highly activated catalytic site construction and advanced catalyst design.

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Идентификаторы

DOI: 10.1038/s41467-025-59127-0

Цитирования и источники

Цитирований: 2Использованных источников: 0

Показатели — AkademScholar