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Atomically synergistic Zn-Cr catalyst for iso-stoichiometric co-conversion of ethane and CO2 to ethylene and CO, Nature Communications15,911(2024)
Ji Yang, Lu Wang, Jiawei Wan, Farid El Gabaly, Andre L. Fernandes Cauduro, Bernice E. Mills, Jeng-Lung Chen, Liang-Ching Hsu, Daewon Lee, Xiao Zhao , Haimei Zheng, Miquel Salmeron, Caiqi Wang, Zhun Dong, Hongfei Lin, Gabor A. Somorjai, Fabian Rosner, Hanna Breunig, David Prendergast, De-en Jiang*, Seema Singh*,and Ji Su*
Developing atomically synergistic bifunctional catalysts relies on the creation of colocalized active atoms to facilitate distinct elementary steps in catalytic cycles. Herein, we show that the atomically-synergistic binuclear-site catalyst (ABC) consisting of [Formula: see text]-O-Cr6+ on zeolite SSZ-13 displays unique catalytic properties for iso-stoichiometric co-conversion of ethane and CO2. Ethylene selectivity and utilization of converted CO2 can reach 100 % and 99.0% under 500 °C at ethane conversion of 9.6%, respectively. In-situ/ex-situ spectroscopic studies and DFT calculations reveal atomic synergies between acidic Zn and redox Cr sites. [Formula: see text] ([Formula: see text]) sites facilitate β-C-H bond cleavage in ethane and the formation of Zn-Hδ- hydride, thereby the enhanced basicity promotes CO2 adsorption/activation and prevents ethane C-C bond scission. The redox Cr site accelerates CO2 dissociation by replenishing lattice oxygen and facilitates H2O formation/desorption. This study presents the advantages of the ABC concept, paving the way for the rational design of novel advanced catalysts.