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General synthesis of single-atom catalysts with high metal loading using graphene quantum dots.

Chuan XiaYunrui QiuYang XiaPeng ZhuGraham KingXiao ZhangZhen-Yu WuJung Yoon Timothy KimDavid A CullenDongxing ZhengPeng LiMohsen ShakouriEmilio HerediaPei-Xin CuiHusam N AlshareefYongfeng HuHaotian Wang
Published in: Nature chemistry (2021)
Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.
Keyphrases
  • transition metal
  • molecular dynamics
  • quantum dots
  • electron transfer
  • room temperature
  • systematic review
  • gold nanoparticles
  • ionic liquid
  • sensitive detection
  • high resolution
  • mass spectrometry