标题: Anionic Defects Enhanced Ammonia Synthesis Over Ru Catalyst Supported on Barium Niobate Reduced with CaH2

作者: Zhao, YS (Zhao, Yushi); Huang, J (Huang, Jia); Yuan, MW (Yuan, Mingwei); Li, XZ (Li, Xiaozhong); Wang, Y (Wang, Yan); Li, MW (Li, Mengwei); Li, JJ (Li, Jinjun); You, ZX (You, Zhixiong)

来源出版物: CATALYSIS LETTERS DOI: 10.1007/s10562-023-04399-8 提前访问日期: JUL 2023

摘要: Anionic defects of H- ((HO)-O-center dot) and oxygen vacancies with trapped electrons (V-O(center dot)) have been built in the lattice of a hydrothermally derived perovskite (Ba5Nb4O15, BNO) by CaH2 reduction in Ar flow at 600 degrees C for 12 h. The formed anionic defects in the CaH2- reduced BNO (CaBNO) have been found to improve drastically the ammonia synthesis activity of Ru/CaBNO by donating electrons from both H-O(center dot) and/or V-O(center dot) to Ru atoms. The stoichiometry of H-O(center dot) and V-O(center dot) has been determined by TPR and TPO method, respectively. The H-O(center dot) defects have been proved to react with N-2 under ammonia synthesis conditions via TPD, XPS measurements and isotope (D-2) reaction, which provides secondary pathways for ammonia synthesis. Kinetic studies revealed that oxygen vacancies accept spilledover H atoms from Ru particles to alleviate the H-2 poisoning effect. Cs-promoter has been demonstrated to accelerate the formation of anionic defects in CaBNO under ammonia synthesis reactions.

作者关键词: Ammonia synthesis; Ruthenium catalyst; Anionic defect; Barium niobate; Cs-promotion

地址: [Zhao, Yushi; Huang, Jia; Yuan, Mingwei; Li, Xiaozhong; Wang, Yan; Li, Mengwei; Li, Jinjun; You, Zhixiong] Wuhan Univ, Sch Resources & Environm Sci, Wuhan 430079, Peoples R China.

[Zhao, Yushi; Huang, Jia; Yuan, Mingwei; Li, Xiaozhong; Wang, Yan; Li, Mengwei; You, Zhixiong] Int Cooperat Base Sustainable Utilizat Resources &, Wuhan 430072, Peoples R China.

通讯作者地址: You, ZX (通讯作者)，Wuhan Univ, Sch Resources & Environm Sci, Wuhan 430079, Peoples R China.

You, ZX (通讯作者)，Int Cooperat Base Sustainable Utilizat Resources &, Wuhan 430072, Peoples R China.

电子邮件地址: zyou@whu.edu.cn

影响因子：2.8