Ru-Cluster-Modified Ni Surface Defects toward Selective Bond Breaking between C–O and C–C

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• 作者：Hao Chen ; Shan He ; Xingzhong Cao ; Shitong Zhang ; Ming Xu ; Min Pu ; Dangsheng Su ; Min Wei ; David G. Evans ; Xue Duan
• 刊名：Chemistry of Materials
• 出版年：2016
• 出版时间：July 12, 2016
• 年：2016
• 卷：28
• 期：13
• 页码：4751-4761
• 全文大小：709K
• 年卷期：0
• ISSN：1520-5002

文摘

For catalytic processes involving multiple reaction pathways such as the ethanol steam reforming (ESR), tailoring the active site structure of catalysts to achieve the desired catalytic selectivity is of vital importance and remains a challenge. Here, we report a heterogeneous Ru–Ni catalyst by anchoring Ru clusters onto the defect sites of Ni nanoparticles. The resulting strained Ru–Ni interface shows a high activity toward the C–C bond cleavage that is essentially required for hydrogen production via ESR. The C–O bond rupture in the side reaction (methanation) is significantly inhibited. This results in an extremely high H₂ yield of 4.2 mol_H2/mol_EtOH at 350 °C, superior to the previously reported ESR catalysts working at medium-low temperature (300–500 °C). An experimental-computational combination study verifies that the conversion of Ni surface defects to the Ru–Ni interface plays a decisive role in the remarkably improved H₂ yield. This work demonstrates an effective strategy to largely enhance the bond-breaking selectivity via tuning the active site structure at the catalyst surface/interface.