Abstract
At present,industrial synthetic ammonia was still obtained through the Hubble-Bosch process,with large energy consumption.It is a research hotspot to realize green synthetic ammonia by using solar energy.The dif-ficulty of photocatalytic ammonia synthesis was that the photo-excited electrons have not enough energy to active N ≡ N.In this study,Ti was doped into BiOBr by one-step hydrothermal method,which was oxidized into TiO2 when the doping amount reaches the maximum,in situ forming Ti0.31B0.69OB/TiO2 composites.Benefiting from the syn-ergistic effect of Ti doping and S-scheme heterojunction,the synthetic ammonia efficiency of Ti0.31B0.69OB/TiO2-11.96 reached 1.643 mmol·g-1cat at mild conditions and without hole scavenger for up to 7 h,the efficiency of synthetic ammonia is 115 times,10.5 times and 3.3 times of that of BiOBr,Ti0.31B0.69OB and TiO2,respectively.Specifically,DFT calculation confirms that Ti doping accurately refine the electronic structure of BiOBr,facili-tate nitrogen adsorption activation and reduce hydrogena-tion reaction energy barrier,thus accelerating the reaction kinetics of photocatalytic nitrogen reduction(NRR).Meanwhile,constructing S-scheme heterojunction boosts the separation and transfer of photogenerated electron-hole pairs,improving the reduction ability of electrons in the conduction band of TiO2 and the oxidation ability of holes in the valence band of Ti0.31B0.69OB.
基金项目
National Natural Science Foundation of China(22168040)
National Natural Science Foundation of China(22162025)
Project of Science & Technology Office of Shannxi Province(2022JM-062)
NETL
NSTL
万方数据