LAUSR

The ultimate objective of chemical conversion is to achieve 100 % selectivity from catalysis, and this is also a prodigious challenge for the conversion of light paraffins into olefins, because it involves controlled activation of highly stable aliphatic C−H bonds. Herein, we show that metal‐free boron nitride (BN) nanosheets not only enable the oxidative dehydrogenation of ethane to ethylene exclusively at near 10 % conversion, but they also deliver a remarkable 60 % selectivity at an ethane conversion of 78 % and remain stable over 400 h at 575 °C. Our operando infrared spectroscopy and 18O isotope tracer study explicitly demonstrates that B−O(H) active sites are formed at the edges of BN through the aid of ethane, and the dehydrogenation circle is completed over these B−O sites by the assistance of O2.