Zhou Hui, Chen Zixuan, Kountoupi Evgenia, Tsoukalou Athanasia, Abdala Paula M, Florian Pierre, Fedorov Alexey, Müller Christoph R
Department of Mechanical and Process Engineering, ETH Zürich, CH 8092, Zürich, Switzerland.
Department of Energy and Power Engineering, Tsinghua University, Beijing, 100084, China.
Nat Commun. 2021 Sep 17;12(1):5510. doi: 10.1038/s41467-021-25784-0.
Early transitional metal carbides are promising catalysts for hydrogenation of CO. Here, a two-dimensional (2D) multilayered 2D-MoC material is prepared from MoCT of the MXene family. Surface termination groups T (O, OH, and F) are reductively de-functionalized in MoCT (500 °C, pure H) avoiding the formation of a 3D carbide structure. CO hydrogenation studies show that the activity and product selectivity (CO, CH, C-C alkanes, methanol, and dimethyl ether) of MoCT and 2D-MoC are controlled by the surface coverage of T groups that are tunable by the H pretreatment conditions. 2D-MoC contains no T groups and outperforms MoCT, β-MoC, or the industrial Cu-ZnO-AlO catalyst in CO hydrogenation (evaluated by CO weight time yield at 430 °C and 1 bar). We show that the lack of surface termination groups drives the selectivity and activity of Mo-terminated carbidic surfaces in CO hydrogenation.
早期过渡金属碳化物是用于CO加氢的有前景的催化剂。在此，一种二维（2D）多层2D-MoC材料由MXene家族的MoCT制备而成。表面端基T（O、OH和F）在MoCT中（500°C，纯H）被还原去官能化，避免形成三维碳化物结构。CO加氢研究表明，MoCT和2D-MoC的活性和产物选择性（CO、CH、C-C烷烃、甲醇和二甲醚）由T基团的表面覆盖率控制，而T基团的表面覆盖率可通过H预处理条件进行调节。2D-MoC不含T基团，并且在CO加氢中（通过430°C和1 bar下的CO重量时空产率评估）优于MoCT、β-MoC或工业Cu-ZnO-AlO催化剂。我们表明，表面端基的缺失驱动了Mo端接的碳化物表面在CO加氢中的选择性和活性。
