Journal
FRONTIERS IN CHEMISTRY
Volume 9, Issue -, Pages -Publisher
FRONTIERS MEDIA SA
DOI: 10.3389/fchem.2021.756993
Keywords
Bimetallic nanoclusters; pH ratiometric sensing; Structural water molecules; nanoscale interface; Dual-emission
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Funding
- NSFC [22172051, 21872053, 21573074]
- Science and Technology Commission of Shanghai Municipality [19520711400]
- Open Project Program of Academician and Expert Workstation, Shanghai Curui Low-Carbon Energy Technology Co., Ltd.
- JORISS program
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This study reveals that the origin of photoluminescence in noble metal NCs lies in the structurally confined water molecules in nanocavities formed by surface-protective ligand packing. The Ag cation mediated Au-Ag bimetal NCs exhibit a pH-dependent dual-emission characteristic with a large Stokes shift of up to 200 nm, making them potential ratiometric nanosensors for pH detection. These findings provide a new understanding of the abnormal photoluminescence emission phenomena in metal NCs.
On the origin of photoluminescence of noble metal NCs, there are always hot debates: metal-centered quantum-size confinement effect VS ligand-centered surface state mechanism. Herein, we provided solid evidence that structural water molecules (SWs) confined in the nanocavity formed by surface-protective-ligand packing on the metal NCs are the real luminescent emitters of Au-Ag bimetal NCs. The Ag cation mediated Au-Ag bimetal NCs exhibit the unique pH-dependent dual-emission characteristic with larger Stokes shift up to 200 nm, which could be used as potential ratiometric nanosensors for pH detection. Our results provide a completely new insight on the understanding of the origin of photoluminescence of metal NCs, which elucidates the abnormal PL emission phenomena, including solvent effect, pH-dependent behavior, surface ligand effect, multiple emitter centers, and large-Stoke's shift.
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