Scientific AchievementProved that changes at the phosphorus centers of diphenylphosphine ligands alter the size of gold clusters synthesized in solution and the fragmentation pathways of otherwise identical clusters.

Significance and ImpactOverturns assumptions about the influence of substitutions in cluster synthesis, a key process for building tailored materials.

Research Details– Synthesized gold clusters capped with diphosphine ligands;

prepared 2 solutions that differed only in the ligands used.– Electrosprayed liquids into mass spectrometer, creating positively

charged ions in a gaseous stream.– Clusters synthesized using the phenyl-based ligand contained

predominantly 11 gold atoms; clusters prepared using the cyclohexane-based ligand contained 9 gold atoms.

– Gold clusters with the phenyl-containing ligand fragmented through the loss of gold atoms as well as activation of the phosphorus-carbon bonds of the ligands. Gold clusters with the cyclohexane ligands exhibited far less activation of the ligand.

Minor Substitution Provides Insight into Designing Materials for Energy Storage and Chemical Manufacturing

Johnson GE, T Priest, and J Laskin. 2013. ChemPlusChem 78:1033-1039. DOI: 10.1002/cplu.201300134

Using a combination of synthesis in solution and high-resolution mass spectrometry, scientists at PNNL demonstrated that the substitution of diphosphine ligands (top: cyclohexane; bottom: phenyl) dramatically influences the size and fragmentation pathways of otherwise identical gold clusters.

Work was performed at EMSL

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