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江西师范大学化学化工学院,江西 南昌 330022
Received:06 July 2020,
Revised:2020-09-17,
Online First:03 November 2020,
Published:05 November 2020
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冷杰, 罗晶晶, 宋崇虎, 周言, 李章敏, 陶端健. Co-N-C催化剂的制备及“一锅法”合成N-亚苄基苯胺[J]. 化工学报, 2020, 71(11): 5016-5024
LENG Jie, LUO Jingjing, SONG Chonghu, ZHOU Yan, LI Zhangmin, TAO Duanjian. Preparation of Co-N-C catalysts and “one-pot method” for synthesis of N-benzyl aniline[J]. CIESC Journal, 2020, 71(11): 5016-5024
冷杰, 罗晶晶, 宋崇虎, 周言, 李章敏, 陶端健. Co-N-C催化剂的制备及“一锅法”合成N-亚苄基苯胺[J]. 化工学报, 2020, 71(11): 5016-5024 DOI: 10.11949/0438-1157.20200906.
LENG Jie, LUO Jingjing, SONG Chonghu, ZHOU Yan, LI Zhangmin, TAO Duanjian. Preparation of Co-N-C catalysts and “one-pot method” for synthesis of N-benzyl aniline[J]. CIESC Journal, 2020, 71(11): 5016-5024 DOI: 10.11949/0438-1157.20200906.
以甲酰胺为氮源和碳源,乙酸钴为钴源,采用预先缩合/高温焙烧两步法制备了一系列Co-N-C催化剂,利用XRD、TEM、N
2
吸附-脱附以及XPS等表征了催化剂结构,考察了催化剂用于硝基苯与苯甲醇“一锅法”合成
N
-亚苄基苯胺的催化性能及其稳定性。结果表明,焙烧温度和掺杂氮元素对Co-N-C催化剂性能影响显著,催化剂Co-N-C/800具有最好的催化性能,0.6 MPa氮气气氛下,温度140℃,反应12 h,硝基苯转化率达99%,
N
-亚苄基苯胺选择性达99%,催化剂重复使用5次,其活性无明显下降。
A series of Co-N-C catalysts were prepared by
a two-step process including pre-condensation and high-temperature calcination
as well as formamide was used as both nitrogen and carbon sources
and cobalt acetate was employed as the source of cobalt. Then the characterizations of XRD
TEM
N
2
adsorption-desorption
and XPS were carried out to investigate the morphology and textural properties of as-prepared Co-N-C catalysts. Moreover
the catalytic activity and reusability of such Co-N-C catalysts were further studied for one-pot synthesis of
N
-benzyl aniline from nitrobenzene and benzyl alcohol. The results demonstrated that the annealing temperature and nitrogen-doping have remarkable influence on the catalytic activity of Co-N-C catalysts. The Co-N-C/800 catalyst exhibited the best catalytic performance
in which the conversion of nitrobenzene was 99%
and the selectivity of
N
-benzyl aniline was 99% under 0.6 MPa nitrogen
temperature of 140℃
and reaction time of 12 h. The catalyst was used repeatedly for 5 times
and its activity did not decrease significantly.
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