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Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation

机译：稳定的纳米多孔NiCu稀释合金催化剂non-oxidative乙醇脱氢

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Producing acetaldehyde, an important industrial chemical, by direct catalytic non-oxidative dehydrogenation of ethanol presents many advantages over current production methods, including generating hydrogen. However, a stable, active, and selective catalyst is currently unavailable. This work demonstrates that the high activity and selectivity of nanoporous (np) NiCu for this reaction can be stabilized by keeping the catalyst in a metastable ("kinetically trapped") state. Using a combination ofin situambient-pressure andex situX-ray photoelectron spectroscopy, environmental transmission electron microscopy, and density functional theory calculations enabled correlating changes in surface composition with the changes in activity and stability upon treatment of np NiCu with H(2)and O-2. Reduction of Ni-doped nanoporous Cu by H(2)exposure enhanced the initial activity but led to complete catalyst deactivation within similar to 40 hours. In contrast, O(2)pretreatment of the same catalyst increased both activity and long-term stability, with only 15% activity loss over 40 hours. The stability of np NiCu as a catalyst inversely correlates with the amount of metallic Ni at the surface, which is enriched by the H(2)pretreatment, while the O(2)pretreatment leads to a kinetically trapped Ni(2+)subsurface state. This work emphasizes that detailed understanding of pretreatment-induced nanoscale structural and compositional changes is necessary to optimize catalyst performance.
机译：重要的工业生产乙醛化学,通过直接催化non-oxidative许多乙醇脱氢的礼物优势目前的生产方法,包括生成氢气。目前活跃,有选择性的催化剂不可用。纳米多孔(np) NiCu的活性和选择性这个反应可以通过保持稳定亚稳态的催化剂(“活动困”)的状态。situambient-pressure andex situX-ray光电子能谱、环境透射电子显微镜法和密度功能理论计算启用关联表面成分的变化活性和稳定性的变化治疗np NiCu H(2)和0 2。Ni-doped的纳米多孔铜的H(2)曝光但导致完整的初始活性增加类似于40小时内催化剂失活。相比之下,O(2)相同的预处理两个活动增加和长期催化剂稳定,只有15%的活动损失超过40个小时。反向与金属的数量倪在表面,这是丰富的H(2)预处理,而O(2)预处理导致活动困倪(2 +)地下状态。理解pretreatment-induced纳米结构和成分的变化是必要的优化催化剂的性能。

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