Li Zhinian, He Lei, Wang Shenliang, Yi Wuzhong, Zou Shihui, Xiao Liping, Fan Jie
Department of Chemistry, Zhejiang University , HangZhou 310027, China.
ACS Comb Sci. 2017 Jan 9;19(1):15-24. doi: 10.1021/acscombsci.6b00108. Epub 2016 Dec 1.
The development of efficient catalyst for oxidative coupling of methane (OCM) reaction represents a grand challenge in direct conversion of methane into other useful products. Here, we reported that a newly developed combinatorial approach can be used for ultrafast optimization of LaO-based multicomponent metal oxide catalysts in OCM reaction. This new approach integrated inkjet printing assisted synthesis (IJP-A) with multidimensional group testing strategy (m-GT) tactfully takes the place of conventionally high-throughput synthesis-and-screen experiment. Just within a week, 2048 formulated LiMgMnO-LaO catalysts in a 64·8·8·8·8 = 262 144 compositional space were fabricated by IJP-A in a four-round synthesis-and-screen process, and an optimized formulation has been successfully identified through only 4·8 = 32 times of tests via m-GT screening strategy. The screening process identifies the most promising ternary composition region is LiMgMn-LaO with an external C yield of 10.87% at 700 °C. The yield of C is two times as high as the pure nano-LaO. The good performance of the optimized catalyst formulation has been validated by the manual preparation, which further prove the effectiveness of the new combinatorial methodology in fast discovery of heterogeneous catalyst.
开发用于甲烷氧化偶联(OCM)反应的高效催化剂是将甲烷直接转化为其他有用产物面临的重大挑战。在此,我们报道了一种新开发的组合方法可用于在OCM反应中对基于LaO的多组分金属氧化物催化剂进行超快优化。这种新方法巧妙地将喷墨打印辅助合成(IJP-A)与多维分组测试策略(m-GT)相结合,取代了传统的高通量合成及筛选实验。仅在一周内,通过IJP-A在四轮合成及筛选过程中,在64·8·8·8·8 = 262144的组成空间内制备了2048种配方的LiMgMnO-LaO催化剂,并且通过m-GT筛选策略仅经过4·8 = 32次测试就成功确定了一种优化配方。筛选过程确定最有前景的三元组成区域是LiMgMn-LaO,在700℃下外部C产率为10.87%。C的产率是纯纳米LaO的两倍。通过手动制备验证了优化催化剂配方的良好性能,这进一步证明了新组合方法在快速发现多相催化剂方面的有效性。