Carbon dioxide has received significant attention as a potential environmentally benign medium to replace hazardous organic compounds, but is a relatively poor solvent. The addition of siloxane substituents provides an attractive and inexpensive means to solubilize a wide variety of compounds in CO 2 . By synthesizing and testing a family of gem-diphosphonate ligands that have been rendered CO 2 -philic by incorporation of a number of related, discrete dimethylsiloxane oligomers, we show that small variations in substituents have a significant effect on the CO 2 -philicity of the ligand. To our knowledge, this is the first systematic study of the effect of siloxane substituent size, branching, and
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