Effect of BaNH,CaNH,Mg3N2 on the activity of Co in NH3 decomposition catalysis  

作　　者：Pei Yu Han Wu Jianping Guo Peikun Wang Fei Chang Wenbo Gao Weijin Zhang Lin Liu Ping Chen 

机构地区：[1]Dalian Institute of Chemical Physics,Dalian National Laboratory for Clean Energy,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao 266101,Shandong,China [3]Collaborative Innovation Center of Chemistry for Energy Materials,Dalian 116023,Liaoning,China [4]University of Chinese Academy of Sciences,Beijing 100049,China

出　　处：《Journal of Energy Chemistry》2020年第7期16-21,I0002,共7页能源化学（英文版）

基　　金：financial supports from the Project of the National Natural Science Foundation of China(Grant Nos.21633011and 21872137);“Transformational Technologies for Clean Energy and Demonstration”;Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21000000);Youth Innovation Promotion Association CAS(No.2018213);the Shanghai Synchrotron Radiation Facility(SSRF)for providing the beam time。

摘　　要：Development of active and non-noble metal-based catalyst for H2 production via NH3 decomposition is crucial for the implementation of NH3 as a H2 carrier.Co-based catalysts have received increasing attention because of its high intrinsic activity and moderate cost.In this work,we examined the effect of BaNH,CaNH and Mg3 N2 on the catalytic activity of Co in the NH3 decomposition reaction.The H2 formation rate ranks the order as Co-BaNH>Co-CaNH>Co-Mg3 N2≈Co/CNTs within a reaction temperature range of 300-550℃.It is worth pointing out that the H2 formation rate of Co-BaNH at 500℃reaches20 mmolH2 gcat-1 min-1,which is comparable to those of the active Ru/Al2 O3(ca.17 mmolH2 gcat-1 min1)and Ru/AC(21 mmolH2 gcat-1 min-1)catalysts under the similar reaction conditions.In-depth research shows that Co-BaNH exhibits an obviously higher intrinsic activity and much lower Ea(46.2 kJ mol-1)than other Co-based catalysts,suggesting that BaNH may play a different role from CaNH,Mg3 N2 and CNTs during the catalytic process.Combined results of XRD,Ar-TPD and XAS show that a[Co-N-Ba]-like intermediate species is likely formed at the interface of Co metal and BaNH,which may lead to a more energy-efficient reaction pathway than that of neat Co metal for NH3 decomposition.

关 键 词：Alkaline earth metal imide COBALT NH3 decomposition Heterogeneous catalysis 

分 类 号：O643.36[理学—物理化学] TQ116.2[理学—化学]