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Separation of liquid mixtures, frequently by distillation, is ubiquitous in the chemical and process industries (CPI). Distillation accounts for ~95% of the energy used in liquid separations, ~25–40% of overall energy used in CPI, and ~3% of global energy consumption.1-2 The low efficiency of distillation is largely due to two issues. First, there are large irreversible losses due to heat transfer.3 Second, a significant fraction of energy used in liquid separations is used to separate azeotropic mixtures in azeotrope-forming systems (e.g., ethanol/water). While a number of conventional distillation technologies4-5 (e.g., pressure-swing, extractive distillation, and azeotropic distillation6) and new separation approaches5 (e.g., dividing-wall columns, membranes, molecular sieves, and bio-absorbance) have been developed for azeotropic systems, these approaches largely rely on thermal separation via phase equilibrium or involve large capital and/or operational costs.