Key Laboratory of Materials Physics, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, P.R. China.
Institute of Physical Science and Information Technology, Anhui University, Hefei 230601, P.R. China.
Nano Lett. 2022 Sep 14;22(17):7144-7150. doi: 10.1021/acs.nanolett.2c02290. Epub 2022 Jul 22.
To propose the concept of single-atom-kernelled nanocluster, we synthesized a Pd-based trimetal nanocluster with a single-Ag atom-kernel for the first time by introducing some steric hindrance factors and employing a joint alloying strategy that combines the coreduction with an antigalvanic reduction (AGR). Although the AGR-derived Pd-based trimetal nanoclusters with single-silver atom kernels have low contents of gold, they show higher activity and selectivity than those of the bimetal precursor nanocluster in the electrocatalytical reduction of CO to CO. Furthermore, it is revealed that the kernel single atoms from both AuPd(TBBT) and AuAgPd(TBBT) are not the active sites for catalysis, but greatly influence the catalytical performance by effecting the electronic configuration. Thus, it is demonstrated that the single-atom-kernelled nanocluster can not only improve the precious metal utilization (even to 100%) but also better the properties and provide insight into the structure-property correlation for metal nanoclusters.
为了提出单原子核纳米团簇的概念,我们首次通过引入一些空间位阻因素并采用结合核心还原与反析氢还原(AGR)的联合合金化策略,合成了一种基于钯的三金属纳米团簇,其中含有单个银原子核。尽管源自 AGR 的具有单银原子核的基于钯的三金属纳米团簇中金的含量较低,但它们在电催化 CO 还原为 CO 反应中比双金属前体纳米团簇具有更高的活性和选择性。此外,研究表明,来自 AuPd(TBBT)和 AuAgPd(TBBT)的核单原子不是催化反应的活性位点,但通过影响电子构型极大地影响了催化性能。因此,证明了单原子核纳米团簇不仅可以提高贵金属利用率(甚至达到 100%),还可以改善性能,并深入了解金属纳米团簇的结构-性能关系。