CoB/C催化硼氢化钠水解制氢的性能

引用本文: 蔡凡, 沈晓晨, 戴敏, 高鸣, 王志斌, 赵斌, 丁维平. CoB/C催化硼氢化钠水解制氢的性能[J]. 无机化学学报, 2013, 29(4): 689-696. doi: 10.3969/j.issn.1001-4861.2013.00.143 shu

Citation: CAI Fan, SHEN Xiao-Chen, DAI Min, GAO Ming, WANG Zhi-Bin, ZHAO Bin, DING Wei-Ping. Catalytic Performance of CoB/C for Hydrolysis of NaBH₄ Aqueous Solution[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(4): 689-696. doi: 10.3969/j.issn.1001-4861.2013.00.143 shu

CoB/C催化硼氢化钠水解制氢的性能

蔡凡 ^1, ,
沈晓晨 ^1, ,
戴敏 ^1, ,
高鸣 ^1, ,
王志斌 ^2, ,
赵斌 ^1, ,
丁维平 ^1,

基金项目:
江苏省自然科学基金(No.BK2010387) (No.BK2010387)

国家自然科学基金(No.41172239) (No.41172239)

中央高校基础科研业务费专项基金(No.1118020513, 1106020513)资助项目。 (No.1118020513, 1106020513)

摘要: 使用浸渍负载-还原法及化学镀法制备了活性炭负载的CoB催化剂, 研究了这些催化剂催化硼氢化钠水解制氢反应的性能。在温度为20℃, 反应液为1% NaBH₄+5% NaOH的条件下, 浸渍负载-还原法制备的CoB/C催化剂的产氢活性为2 022 mL·min^-1·g^-1 (Co), 而化学镀法制备的CoB/C催化剂的产氢活性可达2 503 mL·min^-1·g^-1 (Co), 相同条件下非负载的CoB催化剂的产氢活性仅为1 351 mL·min^-1·g^-1 (Co)。化学镀法制备的CoB/C催化剂重复使用5次后其活性仍能保持初始活性的70%, 而浸渍负载的CoB/C催化剂及非负载的CoB催化剂的活性分别降至初始活性的30%和10%, 化学镀法制备的CoB/C催化剂显示出更好的催化性能。此外该催化剂在空气中放置30 d后催化活性没有明显下降, 这为其存储和使用带来了便利。进一步的物理化学表征表明, 非负载的CoB极易团聚, 形成的二次粒子粒径在400~800 nm, 而活性炭负载的CoB催化剂团聚现象则大大减弱, CoB的分散性明显好于非负载催化剂。载体的存在可进一步阻止CoB活性组分在催化反应过程中发生团聚而避免活性下降。化学镀法制备的催化剂中, 载体与CoB之间有更强的相互作用而使得后者结合紧密, 分散良好, 不易流失, 催化剂整体上具有更好的稳定性。

关键词:

合金;非晶材料;炭;制氢;多相催化;硼氢化钠;化学镀

English

Catalytic Performance of CoB/C for Hydrolysis of NaBH₄ Aqueous Solution

1.
1 Key laboratory of Mesoscopic Chemistry of MOE, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;
Received Date: 13 November 2012
Fund Project:
江苏省自然科学基金(No.BK2010387)

国家自然科学基金(No.41172239)

中央高校基础科研业务费专项基金(No.1118020513, 1106020513)资助项目。

Abstract: The activated carbon supported CoB catalysts were prepared by using impregnation-reduction method (denoted as CoB/C-Imp) and electroless deposition method (denoted as CoB/C-ED), respectively. The catalytic properties were studied on the hydrolysis of NaBH₄ aqueous solution. The catalytic activity of CoB/C-ED, CoB/C-Imp and unsupported CoB was 2 022, 2 503 and 1 351 mL·min^-1·g^-1 (Co), respectively. After 5 cycles, the CoB/C-ED could retain 70% initial activity, but CoB/C-Imp and unsupported CoB could only retain 30% and 10% initial activity. The CoB/C-ED shows the best catalytic performance. Furthermore, no obvious decrease in the activity is observed for CoB/C-ED even after it is exposed to air for 30 days, this good anti-oxidation property is favorable for storage and use. Further physicochemical characterization of these catalysts reveals that the unsupported CoB is easily agglomerated and the size of the secondary particles is in the range of 400~800 nm. After CoB supported on carbon, the agglomeration is greatly restrained. The dispersion of CoB for the CoB/C catalysts is improved compared to the unsupported CoB. The support could also reduce the agglomeration of CoB particles during the catalytic reaction. The CoB particles combine much stronger with the activated carbon support for the CoB/C-ED catalyst, thus resulting in better dispersion and stability, and lesser leaching.

Key words:

alloy;non-crystalline materials;carbon;hydrogen generation;Heterogeneous catalysis;sodium borohydride;electroless deposition

1. [1] Marrero-Alfonso E Y, Beaird A M, Davis T A, et al. Ind. Eng. Chem. Res., 2009,48(3):3703-3712[1] Marrero-Alfonso E Y, Beaird A M, Davis T A, et al. Ind. Eng. Chem. Res., 2009,48(3):3703-3712
2. [2] Rangel C M, Fernandes V R, Slavkov Y, et al. Int. J. Hydrogen Energy, 2009,34(10):4587-4591[2] Rangel C M, Fernandes V R, Slavkov Y, et al. Int. J. Hydrogen Energy, 2009,34(10):4587-4591
3. [3] Kunowsky M, Weinberger B, Lamari Darkrim F, et al. Int. J. Hydrogen Energy, 2008,33(12):3091-3095[3] Kunowsky M, Weinberger B, Lamari Darkrim F, et al. Int. J. Hydrogen Energy, 2008,33(12):3091-3095
4. [4] Binwale R B, Rayalu S, Devotta S, et al. Int. J. Hydrogen Energy, 2008,33(1):360-5[4] Binwale R B, Rayalu S, Devotta S, et al. Int. J. Hydrogen Energy, 2008,33(1):360-5
5. [5] Eberle U, Felderhoff M, Schuth F. Angew. Chem. Int. Ed., 2009,48(36):6608-6630[5] Eberle U, Felderhoff M, Schuth F. Angew. Chem. Int. Ed., 2009,48(36):6608-6630
6. [6] Kojima Y, Suzuki K, Fukumoto K, et al. Int. J. Hydrogen Energy, 2002,27(10):1029-1034[6] Kojima Y, Suzuki K, Fukumoto K, et al. Int. J. Hydrogen Energy, 2002,27(10):1029-1034
7. [7] Kojima Y, Suzuki K, Fukumoto K, et al. J. Power Sources, 2004,125(1):22-26[7] Kojima Y, Suzuki K, Fukumoto K, et al. J. Power Sources, 2004,125(1):22-26
8. [8] Demirci U B, Garin F. J. Alloys Compd., 2008,463(1-2):107-111[8] Demirci U B, Garin F. J. Alloys Compd., 2008,463(1-2):107-111
9. [9] Jeong S U, Cho E A, Nam S W, et al. Int. J. Hydrogen Energy, 2007,32(12):1749-1754[9] Jeong S U, Cho E A, Nam S W, et al. Int. J. Hydrogen Energy, 2007,32(12):1749-1754
10. [10] Ingersoll J C, Mani N, Thenmozhiyal J C, et al. J. Power Sources, 2007,173(1):450-457[10] Ingersoll J C, Mani N, Thenmozhiyal J C, et al. J. Power Sources, 2007,173(1):450-457
11. [11] Murat R, Saim Ö. Catal. Today, 2012,183(1):17-25[11] Murat R, Saim Ö. Catal. Today, 2012,183(1):17-25
12. [12] Ye W, Zhang H M, Xu D Y, et al. J. Power Sources, 2007, 164(2):544-548[12] Ye W, Zhang H M, Xu D Y, et al. J. Power Sources, 2007, 164(2):544-548
13. [13] Xu D Y, Dai P, Guo Q J, et al. Int. J. Hydrogen Energy, 2008,33(24):7371-7377[13] Xu D Y, Dai P, Guo Q J, et al. Int. J. Hydrogen Energy, 2008,33(24):7371-7377
14. [14] Moulder J F, Stickle W F, Sobol P E, et al. Handbook of X- ray Photoelectron Spectroscopy. Eden Prairie: Physical Electronics Inc., 1995:38-39,82-83[14] Moulder J F, Stickle W F, Sobol P E, et al. Handbook of X- ray Photoelectron Spectroscopy. Eden Prairie: Physical Electronics Inc., 1995:38-39,82-83
15. [15] Gorbunova K M, Ivanov M V, Moiseev V P. J. Electrochem. Soc., 1973,120(5):613-618[15] Gorbunova K M, Ivanov M V, Moiseev V P. J. Electrochem. Soc., 1973,120(5):613-618
16. [16] Mallory G O, Hajdu J B. Electroless Plating-Fundamentals and Applications. New York: William Andrew Publishing/ Noyes, 1990:463-511[16] Mallory G O, Hajdu J B. Electroless Plating-Fundamentals and Applications. New York: William Andrew Publishing/ Noyes, 1990:463-511

扫一扫看文章

计量

PDF下载量: 236
文章访问数: 1049
HTML全文浏览量: 181

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

CoB/C催化硼氢化钠水解制氢的性能

English

Catalytic Performance of CoB/C for Hydrolysis of NaBH₄ Aqueous Solution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CoB/C催化硼氢化钠水解制氢的性能

English

Catalytic Performance of CoB/C for Hydrolysis of NaBH4 Aqueous Solution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Catalytic Performance of CoB/C for Hydrolysis of NaBH₄ Aqueous Solution

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs