Aluminum-based nitrogen carriers for chemical looping ammonia generation represent a novel technique with promising potentialfor the efficient production of ammonia and the clean utilization of carbon-based energy sources like coal. However, at the temperaturesrequisite for nitridation reactions, the aluminum-based nitrogen carriers inevitably transform into α-Al2O3, which possesses lower activityand adversely affects the efficiency of ammonia synthesis. To address this issue, a series of Cr-doped CA-x% (x = 0, 2.5, 5.0, 7.5,10.0) nitrogen carrier samples were prepared using the co-precipitation method for the study of their characteristics in chemical loopingammonia synthesis reactions. XRD and XPS analyses confirm that Cr atoms are uniformly doped into the Al2O3 lattice, enhancing its oxygen activity. When the five nitrogen carrier samples were tested in nitridation-ammoniation reactions, the CA-5% sample demonstratedsuperior ammonia synthesis performance, with an ammonia yield approximately 3 times higher than that of the undoped counterpart. Theinclusion of Cr also facilitates both nitridation and ammoniation reactions. Utilizing Material Studio software to construct a model for the nitridation reaction of the nitrogen carrier, analysis of the computational results reveal that Cr doping significantly reduces the formation of COduring the nitridation process and the energy barrier for the dissociative adsorption of N2. After Cr incorporation, the stability of lattice oxygen in Al2O3 decreases, rendering oxygen atoms more prone to dissociate from the surface of the nitrogen carrier and to react with N2 toform aluminum nitride. Finally, repeated nitridation-ammoniation reaction experiments conducted with CA- 5% nitrogen carrier affirmthe cyclic stability of Cr-doped aluminum-based nitrogen carriers