This article highlights the revolution in main group chemistry that was ignited through the advent of frustrated Lewis pairs, a term coined in 2006 to describe the combination of sterically demanding Lewis acids and Lewis bases. This pairing was extremely effective in heterolytic hydrogen cleavage, with further applications in the activation of various other small molecules. These advancements are described herein, highlighting the application of both main group and transition metal‐centered frustrated Lewis pairs in the capture and recycling of small molecules focusing on
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