Jiamin Ma, Yang Gao, Wanning Zhang, Lu Han, Shunai Che, Yuxi Fang
ABSTRACT Direct synthesis of urea through photocatalytic N 2 and CO 2 reduction (PNCR) offers a sustainable approach to mitigate CO 2 emissions and reduce energy consumption from urea production for industry and agriculture. However, achieving high yield of urea is limited by the high energy barrier for co‐reduction of N 2 and CO 2 with subsequent C–N coupling. Herein, we propose that the spin polarization of chiral mesostructured Mo doped Bi 2 WO 6 (CMMB) can facilitate the formation of triplet 3 NOH by regulating the parallel electron spin alignment and promote the separation and transfer of photogenerated carriers, leading to enhanced C–N formation. The incorporation of Mo sites into Bi 2 WO 6 promotes the adsorption and activation of N 2 . A state‐of‐the‐art urea yield was achieved without additives via PNCR on CMMB, surpassing the best‐reported inorganic catalyst by a significant margin. This study provides an effective strategy for designing catalyst structures for the green synthesis of organonitrogen compounds.