School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW, Atlanta, GA, 30332, USA.
National Renewable Energy Laboratory, Golden, CO, 80401, USA.
Angew Chem Int Ed Engl. 2017 Oct 23;56(44):13876-13881. doi: 10.1002/anie.201704704. Epub 2017 Sep 26.
The conversion of methane into alcohols under moderate reaction conditions is a promising technology for converting stranded methane reserves into liquids that can be transported in pipelines and upgraded to value-added chemicals. We demonstrate that a catalyst consisting of small nickel oxide clusters supported on ceria-zirconia (NiO/CZ) can convert methane to methanol and ethanol in a single, steady-state process at 723 K using O as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO as the product of catalytic combustion. The unusual activity of this catalyst is attributed to the synergy between the small Lewis acidic NiO clusters and the redox-active CZ support, which also stabilizes the small NiO clusters.
在温和的反应条件下将甲烷转化为醇是一项很有前途的技术，可将搁浅的甲烷储量转化为可在管道中运输并升级为高附加值化学品的液体。我们证明，由负载在氧化铈-氧化锆（CeO2-ZrO2，CZ）上的小氧化镍簇组成的催化剂可以在 723 K 下使用 O2 作为丰富的氧化剂，在单一、稳态过程中催化甲烷转化为甲醇和乙醇。需要蒸汽才能获得醇，而不是催化燃烧的产物 CO。该催化剂的异常活性归因于小的路易斯酸性 NiO 簇与氧化还原活性 CZ 载体之间的协同作用，该协同作用也稳定了小的 NiO 簇。
