Key Laboratory of Biomedical Polymers-Ministry of Education, College of Chemistry and Molecular Sciences , Wuhan University , Wuhan 430072 , Hubei , China.
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials , Fudan University , Shanghai 200433 , PR China.
ACS Appl Mater Interfaces. 2019 Nov 27;11(47):44573-44581. doi: 10.1021/acsami.9b13864. Epub 2019 Nov 13.
We report the fast and efficient conversion of metal-organic frameworks (MOFs) to phase pure transition-metal carbide (TMC) nanoparticles with uniform size using laser as the energy source, consuming only 6 W power. Nanoparticles of HfC, ZrC, TiC, VC, α-MoC, CrC, and FeC with homogeneous sizes (varied between 6 and 20 nm) were successfully produced, among which HfC and ZrC nanoparticles were obtained, for the first time, with sizes less than 10 nm and in the pure phase. This method was operated directly in air, in stark contrast to traditional furnace heating and laser spray methods, where a protective atmosphere is required. The use of MOFs allowed us to precisely tune the composition of TMC nanoparticles by dialing in the right type and desirable amounts of organic linkers. FeC nanoparticles doped with various percentages of nitrogen atoms were synthesized for the Fischer-Tropsch reaction without any pretreatment or activation. Extremely high iron time of yield (FTY) values were observed, 415 and 550 μmol g s (with addition of K), in a 40 h test without any decay in performance. A high olefin to paraffin ratio was achieved for C to C products, where the ratio for C was higher than 10.
我们报告了一种快速高效的方法,可将金属有机骨架(MOFs)转换为具有均匀尺寸的纯相过渡金属碳化物(TMC)纳米粒子,仅使用激光作为能源,消耗的功率仅为 6 W。成功制备了尺寸均匀(在 6 至 20nm 之间变化)的 HfC、ZrC、TiC、VC、α-MoC、CrC 和 FeC 纳米粒子,其中 HfC 和 ZrC 纳米粒子首次获得了小于 10nm 的尺寸和纯相。该方法可直接在空气中进行,与传统的炉加热和激光喷涂方法形成鲜明对比,后者需要保护性气氛。使用 MOFs,我们可以通过调整合适的有机配体的类型和数量,精确地调整 TMC 纳米粒子的组成。无需任何预处理或激活,就可以合成掺杂不同百分比氮原子的 FeC 纳米粒子,用于费托合成反应。在没有任何性能衰减的情况下,在 40 小时的测试中,观察到极高的铁时空收率(FTY)值,分别为 415 和 550μmol g s(添加 K)。对于 C 到 C 的产物,实现了高烯烃到石蜡的比例,其中 C 的比例高于 10。