论文简介如下：
本研究通过改进的机械化学方法，利用过渡金属氯化物和氢化锂合成了TiNbZrVHf氢化物（以下简称：HEH）。同时，选择具有独特层状结构和活性催化位点的Ti3C2作为支撑基底。通过一步球磨法将纳米级HEH负载到Ti3C2上，并将其用作高效催化剂来改性Mg(BH4)2的放氢动力学和可逆性。研究表明HEH表现出显著增强的催化性能，极大地提高了脱氢动力学和可逆性。高熵氢化物中的“鸡尾酒效应”有助于Mg(BH4)2+HEH@Ti3C2可逆性提升，这与之前关于高熵材料在储氢中具有高催化活性的报道一致。此外，Ti3C2的纳米层状结构为HEH纳米粒提供了稳定的支撑，同时有效地促进了再放氢过程中的氢原子转移。HEH@Ti3C2催化剂提供的双重催化作用在Mg(BH4)2的可逆性提升中发挥了关键作用，并为氢能应用中简便合成HEH提供了一条新途径。
Herein, TiNbZrVHf-hydride (HEH) was synthesized through the modified mechanochemical method using transition metal chlorides and lithium hydride. Ti3C2 was selected as the support substrate, known for its unique layered structure and active catalytic sites. The nano-sized HEH was loaded onto Ti3C2 via a one-step ball milling method, and then used as an efficient catalyst to modify Mg(BH4)2. HEH has shown greatly enhanced catalytic performance, significantly improving the dehydrogenation kinetics and reversibility. A “cocktail effect” in high-entropy hydrides contributed to the excellent reversible ability of Mg(BH4)2+HEH@Ti3C2, which was consistent with previous reports to explain the high catalytic activity of high-entropy materials in hydrogen storage. Moreover, the nanolayered structure of Ti3C2 provided stable support for HEH while effectively facilitating hydrogen atom transfer during re/dehydrogenation. The dual-functional catalysis provided by HEH@Ti3C2 catalyst played an essential role in the reversibility of Mg(BH4)2 and a new route was provide to facile synthesize HEH for energy applications.
下载链接：DOIhttps://doi.org/10.1039/D5CC01503K
