<p>Nanocarbides exhibit interesting mechanical properties and strong oxidation and corrosion resistance. The use of high-entropy effects has enhanced the performance of nanomaterials and enabled new functionalities. Despite the successful development of high-entropy nanoalloys and nanoceramics, controlled synthesis of high-entropy nanocarbides (HENCs) remains challenging due to high growth temperatures, agglomeration of nanoproducts and multi-component immiscibility. Here we achieve synthesis of HENCs containing 5–22 metal elements through a nanoconfined impulse synthetic strategy enabled by Joule heating-induced in situ reactions in carbon nanotube films. These HENCs exhibit multi-element effects and enhanced electrocatalytic activities due to nanoscale size and modification of catalytic sites. In particular, (Pt<sub>0.15</sub>WTaFe<sub>0.15</sub>Ni)C<sub><i>x</i></sub> is highly stable for the hydrogen evolution reaction at 5 A cm<sup>−2</sup> and demonstrates low overall-water-splitting cell voltages under industrial conditions. Moreover, (Pt<sub>0.5</sub>WTaHfCe)C<sub><i>x</i></sub> shows high mass activities for alcohol oxidation. Density functional theory calculations elucidate the mechanism by which specific sites are modified to achieve optimal adsorption capabilities in HENC catalysts. These results demonstrate the promise of our approach for the synthesis of high performance HENC electrocatalysts.</p><p></p>

错误:搜索内容不能为空,请输入英文关键词
错误:关键词超出字数限制,请精简
高级检索

Nanoconfined impulse synthesis of high-entropy nanocarbides for active and stable electrocatalysis

  • Chenyu Li,
  • Zhichao Zhang,
  • Kunlei Zhu,
  • Mingda Liu,
  • Jiayuan Chen,
  • Liang Zhou,
  • Qinghua Zhang,
  • Yonghuang Wu,
  • Jing Guo,
  • Run Shi,
  • Zeqin Xin,
  • Yinghui Sun,
  • Peng Liu,
  • Hui Wu,
  • Lin Gu,
  • Dingsheng Wang,
  • Rongming Wang,
  • Yadong Li,
  • Shoushan Fan,
  • Jia Li,
  • Kai Liu

摘要

Nanocarbides exhibit interesting mechanical properties and strong oxidation and corrosion resistance. The use of high-entropy effects has enhanced the performance of nanomaterials and enabled new functionalities. Despite the successful development of high-entropy nanoalloys and nanoceramics, controlled synthesis of high-entropy nanocarbides (HENCs) remains challenging due to high growth temperatures, agglomeration of nanoproducts and multi-component immiscibility. Here we achieve synthesis of HENCs containing 5–22 metal elements through a nanoconfined impulse synthetic strategy enabled by Joule heating-induced in situ reactions in carbon nanotube films. These HENCs exhibit multi-element effects and enhanced electrocatalytic activities due to nanoscale size and modification of catalytic sites. In particular, (Pt0.15WTaFe0.15Ni)Cx is highly stable for the hydrogen evolution reaction at 5 A cm−2 and demonstrates low overall-water-splitting cell voltages under industrial conditions. Moreover, (Pt0.5WTaHfCe)Cx shows high mass activities for alcohol oxidation. Density functional theory calculations elucidate the mechanism by which specific sites are modified to achieve optimal adsorption capabilities in HENC catalysts. These results demonstrate the promise of our approach for the synthesis of high performance HENC electrocatalysts.