Synthesis of an Sp‐Carbon‐Rich Carbonaceous Material Exhibiting Distinctive Anode Performance

Abstract Among carbon allotropes, carbyne, composed solely of sp ‐hybridized carbon atoms, has garnered significant interest due to its potential unique physical and chemical properties. Nevertheless, the synthesis of carbyne or its analogs remains a persistent challenge, hindering further exploration in this area. Herein, a straightforward synthesis method is proposed to prepare TMS‐capped sp‐ carbon hybridized carbonaceous material (TMS‐C). Trimethylsilylacetylene (TMSA) with two types of bond‐cleaving spots was used as the precursor to obtain TMS‐C via a one‐pot coupling reaction. TMS not only inhibits side reactions but can also be cleaved to generate reaction intermediates participating in subsequent coupling reactions via a copper catalyst. The as‐synthesized TMS‐C contains conjugated linear acetylene bonds composed of over 92 continuous sp‐ hybridized carbon atoms. Due to the large amount of sp‐ hybridized carbon atoms, the lithium (Li)‐ion half‐cell prepared based on TMS‐C delivered an impressive reversible capacity of approximately 3219 mA h g −1 at a current density of 50 mA g −1 , and at a high current density of 5000 mA g −1 , it can be stably cycled 8865 times. Our results reveal immense promise for developing methodologies capable of cutting multiple types of bonds within a single reaction system for the synthesis of carbyne‐based materials.