物理化学学报 >> 2017, Vol. 33 >> Issue (5): 993-1000.doi: 10.3866/PKU.WHXB201702087

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快速合成廉价CuMo纳米粒子高效催化氨硼烷水解产氢

杨昆1,姚淇露1,卢章辉1,*(),康志兵2,陈祥树1,*()   

  1. 1 江西师范大学化学化工学院,无机膜材料工程技术研究中心,南昌330022
    2 南昌航空大学航天制造工程学院,南昌330036
  • 收稿日期:2016-12-15 发布日期:2017-04-20
  • 通讯作者: 卢章辉,陈祥树 E-mail:luzh@jxnu.edu.cn;cxs66cn@jxnu.edu.cn
  • 基金资助:
    国家自然科学基金(21463012);江西省青年科学家培养对象(20133BCB23011);江西省赣鄱英才555工程资助

Facile Synthesis of CuMo Nanoparticles as Highly Active and Cost-Effective Catalysts for the Hydrolysis of Ammonia Borane

Kun YANG1,Qi-Lu YAO1,Zhang-Hui LU1,*(),Zhi-Bing KANG2,Xiang-Shu CHEN1,*()   

  1. 1 Jiangxi Inorganic Membrane Materials Engineering Research Centre, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, P. R. China
    2 School of Aeronautical Manufacture Engineering, Nanchang Hangkong University, Nanchang 330036, P. R. China
  • Received:2016-12-15 Published:2017-04-20
  • Contact: Zhang-Hui LU,Xiang-Shu CHEN E-mail:luzh@jxnu.edu.cn;cxs66cn@jxnu.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21463012);Young Scientist Foundation of Jiangxi Province, China(20133BCB23011);and"Gan-po talent 555"Project of Jiangxi Province, China

摘要:

在无表面活性剂和载体的情况下,使用硼氢化钠作为还原剂,简单快速地合成了CuMo非贵金属纳米粒子.采用X射线粉末衍射(XRD)、透射电子显微镜(TEM)、高分辨透射电子显微镜(HRTEM)、选区电子衍射(SAED)、电感耦合等离子体原子发射光谱(ICP-AES)、光电子能谱(XPS)和比表面积分析(BET)等方法详细地表征了所合成的CuMo纳米粒子,并在室温下将其用于催化氨硼烷水解产氢.所合成的Cu0.9Mo0.1纳米粒子对于氨硼烷水解制氢表现出优异的催化性能,在室温下其转化频率(TOF)达到14.9 min-1,在已报道的Cu催化剂中处于相对较高的值.这种简单的合成方法不仅仅局限于合成CuMo纳米粒子,还可以扩展到合成CuW (3.6 min-1)、CuCr (2 min-1)、NiMo (55.6 min-1)和CoMo (21.7 min-1)纳米粒子,它提供了一种普适的方法合成Cu-M (M = Mo, W, Cr)和TM-Mo (TM = Cu, Ni, Co)纳米粒子作为一系列新型催化剂用于氨硼烷水解.双金属纳米粒子增强的催化活性归因于应力和配体效应诱导的Cu-M纳米粒子的协同促进效果.

关键词: 铜, 氨硼烷, 水解, 氢能源, 纳米粒子

Abstract:

Noble-metal-free CuMo nanoparticles (NPs) without surfactant or support have been facilely prepared using NaBH4 as a reducing agent. The as-prepared CuMo nanocatalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area measurements, and used as catalysts for the hydrolysis of ammonia borane (AB, NH3BH3) at room temperature. The as-synthesized Cu0.9Mo0.1 NPs exhibited a high activity towards the hydrolysis of AB with a turnover frequency (TOF) of 14.9 min-1, a higher value than that reported for Cu catalysts. Our synthesis is not limited to CuMo NPs alone, but can easily be extended to CuW (3.6 min-1), CuCr (2 min-1), NiMo (55.6 min-1), and CoMo (21.7 min-1) NPs, providing a general approach to Cu-M (M = Mo, W, Cr) and TM-Mo (TM = Cu, Ni, Co) NPs as a series of novel catalysts for the hydrolysis of AB. The enhanced activity of bimetallic NPs may be attributed to the synergistic effects of the Cu-M NPs induced by the strain and ligand effects.

Key words: Copper, Ammonia borane, Hydrolysis, Hydrogen energy, Nanoparticle

MSC2000: 

  • O643