Liu, Kaidi; Shen, Huachen; Xin, Jing; Zhao, Yonghui; Qiao, Shan; Zhang, Peipei; Mi, Xiaotong; Gong, Kun; An, Yunlei; Lin, Tiejun; Zhong, Liangshu

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

2025, ,

Liu, Kaidi; Shen, Huachen; Xin, Jing; Zhao, Yonghui; Qiao, Shan; Zhang, Peipei; Mi, Xiaotong; Gong, Kun; An, Yunlei; Lin, Tiejun; Zhong, Liangshu

Fischer-Tropsch synthesis to olefins (FTO) with remarkable efficiency using cobalt metal catalyst is highly appealing yet encountering a trade-off between activity and olefin selectivity. Herein, we engineered a confined Ru1Consingle-atom alloy catalyst featuring a graphitic carbon shell layer, which exhibits at least a 2-fold activity increase compared with all previously reported Co-based catalysts, along with ultralow CO2 selectivity (1.3 %), remarkable olefin selectivity (53.5 %) and long-term stability. Incorporating Ru single atoms into Co nano-particles can stabilize highly active hexagonal close-packed Co phase by forming Ru1Conalloy, which exhibits much stronger CO adsorption and dissociation capabilities. Moreover, probe experiments and DFT calculations confirmed that it also creates an electron-rich Co active center, altering the CO activation pathway from Hassisted to direct CO dissociation. The surface graphitic carbon promoted olefins desorption and impeded its secondary adsorption, thus boosting olefins production. This work provides an effective confinement and Ru-Co alloy strategy for the rational design of Co metal catalysts for the Fischer-Tropsch reaction, successfully steering product distribution from benchmark paraffins to high value-added olefins with exceptional efficiency.