Wen Zhaoyu, Fu Qiong, Wu Jie, Fan Guangyin
College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
Nanomaterials (Basel). 2020 Aug 17;10(8):1612. doi: 10.3390/nano10081612.
Simple and efficient synthesis of a nano-catalyst with an excellent catalytic property for hydrogen generation from hydrolysis of dimethyl amine-borane (DMAB) is a missing piece. Herein, effective and recycled palladium (Pd) nanoparticles (NPs) supported on soft nitriding porous carbon (NPC) are fabricated and applied for DMAB hydrolysis. It is discovered that the soft nitriding via a low-temperature urea-pretreatment induces abundant nitrogen-containing species on the NPC support, thus promoting the affinity of the Pd precursor and hindering the agglomeration of formed Pd NPs onto the NPC surface during the preparation process. Surface-clean Pd NPs with a diameter of sub-2.0 nm deposited on the NPC support (Pd/NPC) exhibit an outstanding catalytic performance with a turnover frequency (TOF) of 2758 h toward DMAB hydrolysis, better than many previous reported Pd-based catalysts. It should be emphasized that the Pd/NPC also possesses a good stability without an obvious decrease in catalytic activity for DMAB hydrolysis in five successive recycling runs. This study provides a facile but efficient way for preparing high-performance Pd catalysts for catalytic hydrogen productions.
简单高效地合成一种对二甲胺硼烷（DMAB）水解制氢具有优异催化性能的纳米催化剂是一个缺失的环节。在此，制备了负载在软氮化多孔碳（NPC）上的有效且可循环的钯（Pd）纳米颗粒（NPs），并将其应用于DMAB水解。研究发现，通过低温尿素预处理进行的软氮化在NPC载体上诱导产生了大量含氮物种，从而提高了Pd前驱体的亲和力，并在制备过程中阻碍了形成的Pd NPs在NPC表面的团聚。沉积在NPC载体上（Pd/NPC）的直径小于2.0 nm的表面清洁的Pd NPs对DMAB水解表现出出色的催化性能，周转频率（TOF）为2758 h⁻¹，优于许多先前报道的Pd基催化剂。需要强调的是，Pd/NPC在连续五次循环运行中对DMAB水解的催化活性也没有明显下降，具有良好的稳定性。本研究为制备用于催化制氢的高性能Pd催化剂提供了一种简便而有效的方法。
