燃料化学学报（中英文）2025，Vol.53Issue(6)：954-963,10.DOI:10.3724/2097-213X.2025.JFCT.0001
基于GO穿插的Ni/Cu@MIL-101(Cr)催化氨硼烷水解释氢研究
Research on hydrogen generation from hydrolysis of ammonia borane catalyzed by Ni/Cu@MIL-101(Cr)incorporated by GO
摘要
Abstract
For improving the performance of hydrogen production from ammonia borane(AB)by hydrolyzing,Ni and Cu were selected as catalyst metals which were supposed to load on the matrix developed by incorporating MIL-101(Cr)with certain amount of graphene oxide(GO).Solvothermal method was employed to synthesize the MIL-101(Cr)and its composites,isotherms of nitrogen adsorption at 77.15 K were then measured and used to determine the textural parameters,which were further employed to evaluate the effect of the amount of GO incorporated on the performance of loading the metal particles.Microscopic morphological observations of the prepared samples were also conducted in terms of measuring the X-ray diffraction(XRD)and scanning electron microscope(SEM).The tests of hydrogen production from hydrolysis of AB were finally performed within the temperature range 288-328 K to evaluate the catalyzing performances of the composites.It shows that,within the range of the incorporated amount 0-0.45％,GO would gradually fill within the interspace among the crystals,and the structure of the crystal became irregular with the increment in the amount of GO incorporated,but the sample prepared by incorporating MIL-101(Cr)with GO about 0.45％had the largest specific surface area about 3452 m2/g with an average pore width about 0.839 nm,which is 2-3 times the diameter of metal ions and beneficial to the loading of the metal particles.It also shows that the characteristic peak positions of the main peak of the XRD of the composite samples overlap with that of the MIL-101(Cr),in comparing with the decrement in the accompanying stray peak,the diffraction peak of the main peak of the composite has been enhanced.It suggests that the crystal structure of the composite can be remained while incorporating MIL-101(Cr)with suitable amount of GO,and the incorporation did not bring about the formation of Cr2O3,but the order and crystallinity of the crystal plane of the sample had been enhanced;the metal particles were mostly in sizes of 4-5 nm and in the form of metal oxides and alloys that had been evenly distributed around with the surface and the interspace of the composite.Results reveal that,within the temperature range 288-328 K,while hydrolyzing AB catalyzed by the composite having already been loaded Ni and Cu particles,the composite formed by loading equal molar amounts of these two metal had the best catalytic efficiency with a TOF value and the activation energy respectively about 27 min-1 and 35.7 kJ/mol,and the hydrolyzing reaction of AB at different concentrations can also be considered to be in zero-order kinetics.Results also show that there is about 48％increment in the duration for hydrogen releasing after 10 cycles of the composite,but the decrement in the amount of hydrogen released is less than 0.06％,suggesting a good recycling performance of the as-prepared catalyst.It can be concluded that,while developing the catalyst for hydrolyzing AB by using MIL-101(Cr)as the matrix,it is reasonable to select Ni and Cu as catalyst metals and incorporate with certain amount of GO for enhancing its performance.关键词
氨硼烷/催化剂/MOFs/水解Key words
ammonia borane/catalyst/MOFs/hydrolysis分类
化学引用本文复制引用
安科迪,仵梦博,郑青榕..基于GO穿插的Ni/Cu@MIL-101(Cr)催化氨硼烷水解释氢研究[J].燃料化学学报（中英文）,2025,53(6):954-963,10.基金项目
The project was supported by the National Natural Science Foundation of China(51979121),Natural Science Foundation of Fujian Province(2024J01713)and Xiamen Municipal Bureau of Sciences & Technology(3502Z20226011). 国家自然科学基金(51979121),福建省自然科学基金(2024J01713)和厦门市科技计划(3502Z20226011)资助 （51979121）
