Highly efficient subnanometer Ru-based catalyst for ammonia synthesis via an associative mechanism

作     者：Yanliang Zhou Qianjin Sai Zhenni Tan Congying Wang Xiuyun Wang Bingyu Lin Jun Ni Jianxin Lin Lilong Jiang Yanliang Zhou;Qianjin Sai;Zhenni Tan;Congying Wang;Xiuyun Wang;Bingyu Lin;Jun Ni;Jianxin Lin;Lilong Jiang

作者机构：National Engineering Research Center of Chemical Fertilizer CatalystFuzhou UniversityFuzhou 350002China 

出 版 物：《Chinese Journal of Chemical Engineering》 (中国化学工程学报（英文版）)

年 卷 期：2022年第35卷第3期

页      面：177-184页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：the Key Research&Development Program of National Natural Science Foundation of China(22038002) the National Natural Science Foundation of China(21972019,22108037) 

主　　题：Ammonia synthesis Sustainability Subnanometer Ru clusters Associative route Catalysis 

摘      要：The industrial manufacture of ammonia(NH_(3))using Fe-based catalyst works under rigorous *** the goal of carbon-neutrality,it is highly desired to develop advanced catalyst for NH_(3)synthesis at mild conditions to reduce energy consumption and CO_(2)***,the main challenge of NH_(3)synthesis at mild conditions lies in the dissociation of steady N≡N triple *** this work,we report the design of subnanometer Ru clusters(0.8 nm)anchored on the hollow N-doped carbon spheres catalyst(Ru-SNCs),which effectively promotes the NH_(3)synthesis at mild conditions via an associative *** NH_(3)synthesis rate over Ru-SNCs(0.49%(mass)Ru)reaches up to 11.7 mmol NH_(3)·(g cat)^(-1)·h^(-1) at 400℃ and 3 MPa,which is superior to that of 8.3 mmol NH_(3)·(g cat)^(-1)·h^(-1) over Ru nanoparticle catalyst(1.20%(mass)Ru).Various characterizations show that the N_(2)H_(4)species are the main intermediates for NH_(3)synthesis on Ru-SNCs *** demonstrates that Ru-SNCs catalyst can follow an associative route for N_(2)activation,which circumvents the direct dissociation of N_(2)and results in highly efficient NH_(3)synthesis at mild conditions.