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The pairing of ions of opposite charge is a fundamental principle in chemistry, and is widely applied in synthesis and catalysis. In contrast, cation–cation association remains an elusive concept, lacking in supporting experimental evidence. While studying the structure and properties of 4‐oxopiperidinium salts [OC5H8NH2]X for a series of anions X− of decreasing basicity, we observed a gradual self‐association...
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