非晶态镍硼/石墨烯复合材料的制备及其蒎烯催化加氢活性

doi:10.11949/j.issn.0438-1157.20151703

化工学报 ›› 2016, Vol. 67 ›› Issue (6): 2363-2370.DOI: 10.11949/j.issn.0438-1157.20151703

• 催化、动力学与反应器 • 上一篇下一篇

非晶态镍硼/石墨烯复合材料的制备及其蒎烯催化加氢活性

张家华, 蒋丽红, 伍水生, 王红琴, 王亚明

昆明理工大学化学工程学院, 云南昆明 650500

收稿日期:2015-11-11 修回日期:2016-03-05 出版日期:2016-06-05 发布日期:2016-06-05
通讯作者: 王亚明
基金资助:
国家自然科学基金联合基金重点支持项目(U1202265)。

Preparation of amorphous Ni-B/graphene composites for catalytic hydrogenation of pinene

ZHANG Jiahua, JIANG Lihong, WU Shuisheng, WANG Hongqin, WANG Yaming

Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, Yunnan, China

Received:2015-11-11 Revised:2016-03-05 Online:2016-06-05 Published:2016-06-05
Supported by:
supported by the National Natural Science Foundation of China (U1202265).

摘要/Abstract

摘要：

以鳞片石墨为原料,采用Hummers法制得氧化石墨,经超声分散后制得稳定的氧化石墨烯(GO)分散液。以化学还原法一步制得非晶态Ni-B/rGO复合催化剂,并以蒎烯加氢为探针反应考察了催化剂的性能。结果表明,该催化剂对蒎烯加氢反应具有较高的催化活性,对生成顺式蒎烷具有较高对映选择性,达到96.5%以上,性能优于大多数传统的镍系催化剂甚至贵金属催化剂。该催化剂亦具有较好的稳定性,重复使用8次后,其转化率及对映选择性依然保持在较高水平。采用XRD、XPS、TEM等技术手段,研究了复合催化剂材料的结构与性质,初步探讨了非晶态Ni-B/rGO催化剂的构效关系。

关键词: 石墨烯, 非晶, 催化, 复合材料, 加氢

Abstract:

Graphite oxide was prepared from flake graphite by Hummers method and dispersed by ultrasonic treatment. The amorphous Ni-B/rGO composite catalysts were prepared by one-step chemical reduction with NaBH₄ as reducing agent, and tested in the catalytic hydrogenation of pinene as the probing reaction. It shows that the as-prepared catalysts exhibit high catalytic activity and relatively high enantioselectivity of 96.5% for cis-pinane, which is better than the traditional Raney nickel and even noble metal catalysts. The catalyst possessed good stability, evidenced by that after 8-times testing cycles, both the conversion of pinene and the enantioselectivity to cis-pinane remained at a good level. The structure and properties of amorphous Ni-B/rGO composite catalysts were measured by XRD, XPS, TEM techniques, and the relationship between the catalytic performance and the structure was explored. The higher activity of the Ni-B/rGO amorphous catalyst could be attributed to the highly uniform dispersion of the Ni-B active species with unique electronic structure, and the interaction between Ni-B active species and the rGO in the composite catalysts．

Key words: grapheme, amorphous, catalysis, composites, hydrogenation

中图分类号:

TB333

张家华, 蒋丽红, 伍水生, 王红琴, 王亚明. 非晶态镍硼/石墨烯复合材料的制备及其蒎烯催化加氢活性[J]. 化工学报, 2016, 67(6): 2363-2370.

ZHANG Jiahua, JIANG Lihong, WU Shuisheng, WANG Hongqin, WANG Yaming. Preparation of amorphous Ni-B/graphene composites for catalytic hydrogenation of pinene[J]. CIESC Journal, 2016, 67(6): 2363-2370.

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非晶态镍硼/石墨烯复合材料的制备及其蒎烯催化加氢活性

Preparation of amorphous Ni-B/graphene composites for catalytic hydrogenation of pinene

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