Reaction mechanism and kinetics for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst
Reaction mechanism and kinetics for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst
复制标题
Pt/CNT 催化剂上氨硼烷水解脱氢的反应机理和动力学
DOI：
10.1002/aic.15389
复制
发表时间：
2017-01-01
期刊：
影响因子：
3.7
通讯作者：
Chen, De
中科院分区：
文献类型：
--
作者：
Chen, Wenyao;Li, Dali;Chen, De
A reaction mechanism is proposed for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst. A combination of thermodynamic analysis and FTIR measurement reveals that B-containing byproducts are mainly in the form of an NH4B(OH)4-B(OH)3 mixture rather than NH4BO2 reported previously. The revised main reaction is NH3BH3+4H2O→NH4++B(OH)4−+3H2↑, involving the B–H, B–N, and O–H bond cleavages. Isotopic experiments using D2O instead of H2O as reactant or introducing D2 into the reaction atmosphere suggest the O–H bond cleavage being in the rate-determining step, and an unfavorable occurrence of the chemisorbed H2O dissociation (i.e., the direct O–H bond cleavage), respectively. Different reaction pathways with indirect O–H bond cleavages are analyzed, and then NH3BH2*+H2O*→NH3BH2(OH)*+H* is suggested as the rate-determining step. Subsequently, a Langmuir–Hinshelwood kinetic model is developed, which fits well with the experimental data. © 2016 American Institute of Chemical Engineers AIChE J, 63: 60–65, 2017
