One-pot synthesis of core-shell Cu@SiO2 nanospheres and their catalysis for hydrolytic dehydrogenation of ammonia borane and hydrazine borane

被引:198
作者
Yao, Qilu [1 ]
Lu, Zhang-Hui [1 ]
Zhang, Zhujun [1 ]
Chen, Xiangshu [1 ]
Lan, Yaqian [2 ]
机构
[1] Jiangxi Normal Univ, Coll Chem & Chem Engn, Jiangxi Inorgan Membrane Mat Engn Res Ctr, Nanchang 330022, Peoples R China
[2] Nanjing Normal Univ, Coll Chem & Mat Sci, Jiangsu Key Lab Biofunct Mat, Nanjing 210023, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
METAL-ORGANIC-FRAMEWORK; HIGH-EXTENT DEHYDROGENATION; HYDROGEN GENERATION SYSTEM; SYNERGISTIC CATALYSIS; NI NANOPARTICLES; SILICA; CU; N2H4BH3; NICKEL; NH3BH3;
D O I
10.1038/srep07597
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Ultrafine copper nanoparticles (Cu NPs) within porous silica nanospheres (Cu@SiO2) were prepared via a simple one-pot synthetic route in a reverse micelle system and characterized by SEM, TEM, EDX, XRD, N-2 adsorption-desorption, CO-TPD, XPS, and ICP methods. The characterized results show that ultrafine Cu NPs with diameter of around 2 nm are effectively embedded in the center of well-proportioned spherical SiO2 NPs of about 25 nm in diameter. Compared to commercial SiO2 supported Cu NPs, SiO2 nanospheres supported Cu NPs, and free Cu NPs, the synthesized core-shell nanospheres Cu@SiO2 exhibit a superior catalytic activity for the hydrolytic dehydrogenation of ammonia borane (AB, NH3BH3) and hydrazine borane (HB, N2H4BH3) under ambient atmosphere at room temperature. The turnover frequencies (TOF) for the hydrolysis of AB and HB in the presence of Cu@SiO2 nanospheres were measured to be 3.24 and 7.58 mol H-2 (mol Cu min) 21, respectively, relatively high values for Cu nanocatalysts in the same reaction. In addition, the recycle tests show that the Cu@SiO2 nanospheres are still highly active in the hydrolysis of AB and HB, preserving 90 and 85% of their initial catalytic activity even after ten recycles, respectively.
引用
收藏
页数:8
相关论文
共 60 条
[21]   First row transition metal ion-assisted ammonia-borane hydrolysis for hydrogen generation [J].
Kalidindi, Suresh Babu ;
Indirani, M. ;
Jagirdar, Balaji R. .
INORGANIC CHEMISTRY, 2008, 47 (16) :7424-7429
[22]   Catalytic methanolysis of hydrazine borane: a new and efficient hydrogen generation system under mild conditions [J].
Karahan, Senem ;
Zahmakiran, Mehmet ;
Ozkar, Saim .
DALTON TRANSACTIONS, 2012, 41 (16) :4912-4918
[23]   Catalytic hydrolysis of hydrazine borane for chemical hydrogen storage: Highly efficient and fast hydrogen generation system at room temperature [J].
Karahan, Senem ;
Zahmakiran, Mehmet ;
Ozkar, Saim .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2011, 36 (08) :4958-4966
[24]   Copper(0) Nanoparticles Supported on Silica-Coated Cobalt Ferrite Magnetic Particles: Cost Effective Catalyst in the Hydrolysis of Ammonia-Borane with an Exceptional Reusability Performance [J].
Kaya, Murat ;
Zahmakiran, Mehmet ;
Ozkar, Saim ;
Volkan, Murvet .
ACS APPLIED MATERIALS & INTERFACES, 2012, 4 (08) :3866-3873
[25]   Synthesis of supported Ni@(RhNi-alloy) nanocomposites as an efficient catalyst towards hydrogen generation from N2H4BH3 [J].
Li, Changming ;
Dou, Yibo ;
Liu, Jie ;
Chen, Yudi ;
He, Shan ;
Wei, Min ;
Evans, David G. ;
Duan, Xue .
CHEMICAL COMMUNICATIONS, 2013, 49 (85) :9992-9994
[26]   Binary Cu-Co catalysts derived from hydrotalcites with excellent activity and recyclability towards NH3BH3 dehydrogenation [J].
Li, Changming ;
Zhou, Junyao ;
Gao, Wa ;
Zhao, Jingwen ;
Liu, Jie ;
Zhao, Yufei ;
Wei, Min ;
Evans, David G. ;
Duan, Xue .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (17) :5370-5376
[27]  
Li P, 2012, CAM ST AD M, V134, P1
[28]   Metal-Organic-Framework-Based Catalyst for Highly Efficient H2 Generation from Aqueous NH3BH3 Solution [J].
Li, Yaoqi ;
Xie, Lei ;
Li, Yan ;
Zheng, Jie ;
Li, Xingguo .
CHEMISTRY-A EUROPEAN JOURNAL, 2009, 15 (36) :8951-8954
[29]   Ammonia Borane Confined by a Metal-Organic Framework for Chemical Hydrogen Storage: Enhancing Kinetics and Eliminating Ammonia [J].
Li, Zhongyue ;
Zhu, Guangshan ;
Lu, Gaoqing ;
Qiu, Shilun ;
Yao, Xiangdong .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (05) :1490-+
[30]   Core-shell structured nanospheres with mesoporous silica shell and Ni core as a stable catalyst for hydrolytic dehydrogenation of ammonia borane [J].
Liu, Hua ;
Cao, Changyan ;
Li, Ping ;
Yu, Yu ;
Song, Weiguo .
JOURNAL OF ENERGY CHEMISTRY, 2014, 23 (01) :50-56