A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Highly Robust but Surface-Active : An N-Heterocyclic Carbene-Stabilized Au25 Nanocluster (2019)

Shen, H., Deng, G., Kaappa, S., Tan, T., Han, Y.-Z., Malola, S., Lin, S.-C., Teo, B. K., Häkkinen, H., & Zheng, N. (2019). Highly Robust but Surface-Active : An N-Heterocyclic Carbene-Stabilized Au25 Nanocluster. Angewandte Chemie, 58(49), 17731-17735. https://doi.org/10.1002/anie.201908983

JYU-tekijät tai -toimittajat

Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Shen, Hui; Deng, Guocheng; Kaappa, Sami; Tan, Tongde; Han, Ying-Zi; Malola, Sami; Lin, Shui-Chao; Teo, Boon K.; Häkkinen, Hannu; Zheng, Nanfeng

Lehti tai sarja: Angewandte Chemie

ISSN: 1433-7851

eISSN: 1521-3773

Julkaisuvuosi: 2019

Volyymi: 58

Lehden numero: 49

Artikkelin sivunumerot: 17731-17735

Kustantaja: Wiley-VCH Verlag

Julkaisumaa: Saksa

Julkaisun kieli: englanti

DOI: https://doi.org/10.1002/anie.201908983

Julkaisun avoin saatavuus: Ei avoin

Julkaisukanavan avoin saatavuus: 

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/67174

Tiivistelmä

Surface organic ligands play a critical role in stabilizing atomically precise metal nanoclusters in solutions. However, it is still challenging to prepare highly robust ligated metal nanoclusters that are surface-active for liquid-phase catalysis without any pre-treatment. Now, an N-heterocyclic carbene-stabilized Au25 nanocluster with high thermal and air stabilities is presented as a homogenous catalyst for cycloisomerization of alkynyl amines to indoles. The nanocluster, characterized as [Au25(iPr2-bimy)10Br7]2+ (iPr2-bimy=1,3-diisopropylbenzimidazolin-2-ylidene) (1), was synthesized by direct reduction of AuSMe2Cl and iPr2-bimyAuBr with NaBH4 in one pot. X-ray crystallization analysis revealed that the cluster comprises two centered Au13 icosahedra sharing a vertex. Cluster 1 is highly stable and can survive in solution at 80 °C for 12 h, which is superior to Au25 nanoclusters passivated with phosphines or thiols. DFT computations reveal the origins of both electronic and thermal stability of 1 and point to the probable catalytic sites. This work provides new insights into the bonding capability of N-heterocyclic carbene to Au in a cluster, and offers an opportunity to probe the catalytic mechanism at the atomic level.

YSO-asiasanat: nanohiukkaset; kulta; katalyytit; katalyysi

Vapaat asiasanat: Au25; carbene ligands; gold catalysis; gold nanoclusters; homogeneous catalysis

Liittyvät organisaatiot

OKM-raportointi: Kyllä

Raportointivuosi: 2019

JUFO-taso: 3