制备溶剂对NiCoB非晶态合金催化剂结构及糠醛加氢性能的影响

郭海军; 唐伟超; 张海荣; 彭芬; 王璨; 黄前霖; 熊莲; 陈新德; 欧阳新平; 邱学青

制备溶剂对NiCoB非晶态合金催化剂结构及糠醛加氢性能的影响

郭海军^{1, 2, 3, 4, 5},
唐伟超^{1, 2, 3, 4},
张海荣^{1, 2, 3, 4},
彭芬^{1, 2, 3, 4},
王璨^{1, 2, 3, 4},
黄前霖^{1, 2, 3, 4, 6},
熊莲^{1, 2, 3, 4},
陈新德^{1, 2, 3, 4, ,},
欧阳新平⁵,
邱学青⁵

1.
中国科学院可再生能源重点实验室, 广东广州 510640
2.
广东省新能源和可再生能源研究开发与应用重点实验室, 广东广州 510640
3.
中国科学院广州能源研究所, 广东广州 510640
4.
中国科学院广州能源研究所盱眙凹土研发中心, 江苏盱眙 211700
5.
华南理工大学化学与化工学院, 广东广州 510640
6.
中国科学院大学, 北京 100049

基金项目:

国家自然科学基金 21406229

江苏省科技计划项目 BE2014101

广东省新能源和可再生能源研究开发与应用重点实验室基金 Y709jh1001

详细信息

通讯作者:
陈新德, Tel/Fax: 020-37213916，E-mail: cxd_cxd@hotmail.com

中图分类号: O643.32
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- 文章访问数: 85
- HTML全文浏览量: 32
- PDF下载量: 8
- 被引次数: 0
出版历程
- 收稿日期: 2017-03-20
- 修回日期: 2017-05-05
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-07-10

Effects of the preparation solvent on structure and catalytic properties of NiCoB amorphous alloy catalysts for hydrogenation of furfural

GUO Hai-jun^{1, 2, 3, 4, 5},
TANG Wei-chao^{1, 2, 3, 4},
ZHANG Hai-rong^{1, 2, 3, 4},
PENG Fen^{1, 2, 3, 4},
WANG Can^{1, 2, 3, 4},
HUANG Qian-lin^{1, 2, 3, 4, 6},
XIONG Lian^{1, 2, 3, 4},
CHEN Xin-de^{1, 2, 3, 4
, ,},
OUYANG Xin-ping⁵,
QIU Xue-qing⁵

1.
Key Laboratory of Renewable Energy, Chinese Academy of Sciences, Guangzhou 510640, China
2.
Guangdong Key Laboratory of New and Renewable Energy Research and Development, Guangzhou 510640, China
3.
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
4.
R & D Center of Xuyi Attapulgite Applied Technology, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Xuyi 211700, China
5.
School of Chemistry & Chemical Engineering, South China University of Technology, Guangzhou 510640, China
6.
University of Chinese Academy of Sciences, Beijing 100049, China

Funds:

the National Natural Science Foundation of China 21406229

the Program of Jiangsu Province Science and Technology BE2014101

Guangdong Provincial Key Laboratory Foundation of New and Renewable Energy Research and Development Y709jh1001

摘要

摘要: 采用化学还原法在不同单一和复配溶剂体系中制备了一系列NiCoB非晶态合金催化剂，对其液相糠醛加氢性能进行了考察，并采用N₂吸附-脱附等温线、ICP、FE-SEM、HRTEM、XRD、XPS等手段进行了表征。结果表明，在相同反应条件下，制备溶剂的表面张力、黏度、极性大小和溶解度常数等对NiCoB非晶态合金催化剂的组成、形貌和结构及其糠醛加氢反应性能均产生重要影响。由甲醇/乙二醇复配溶剂（MEG，体积比1:1）制备的NiCoB-MEG催化剂具有最理想的糠醛液相加氢制糠醇性能，糠醛转化率达到96.4%，糠醇选择性达到83.49%，这可归因于甲醇和乙二醇之间的协同作用促进了金属组分的分散和还原。
- 糠醛加氢 /
- 制备溶剂 /
- NiCoB /
- 非晶态合金催化剂 /
- 糠醇
Abstract: A series of NiCoB amorphous alloy catalysts were prepared by chemical reduction method in different single and mixed solvent systems and their performance for liquid phase hydrogenation of furfural (FUR) was evaluated. The catalysts were also characterized by N₂ adsorption-desorption, ICP, FE-SEM, HRTEM, XRD and XPS. The results showed that the surface tension, viscosity, polarity and solubility parameter of preparation solvent had important effects on the composition, morphology, structure and the catalytic properties of FUR hydrogenation of the NiCoB amorphous alloy catalyst. The NiCoB-MEG catalyst prepared by the mixed solvent of methanol/ethylene glycol (MEG, volume ratio of 1:1) showed the optimum liquid phase hydrogenation performance of FUR to furfuryl alcohol (FA) with a FUR conversion of 96.4% and a FA selectivity of 83.49%. It can be due to the improvement of dispersion and reduction of metallic components by the synergistic effect between methanol and ethylene glycol.
- hydrogenation of furfural /
- preparation solvent /
- NiCoB /
- amorphous alloy catalysts /
- furfuryl alcohol

HTML全文

图 1 由不同单一溶剂制备的NiCoB催化剂的N₂吸附-脱附等温线(a)和BJH孔径分布(b)

Figure 1 N₂ adsorption-desorption isotherms (a) and BJH pore size distribution (b) of NiCoB catalysts prepared from different single solvent

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图 2 由不同单一溶剂制备的NiCoB催化剂的XRD谱图及NiCoB-E催化剂的SAED照片

Figure 2 XRD patterns of NiCoB catalysts prepared from different single solvent and the SAED picture of NiCoB-E catalyst

a: NiCoB-W; b: NiCoB-M; c: NiCoB-E; d: NiCoB-EG; e: NiCoB-PEG; f: NiCoB-isoP; g: NiCoB-nP

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图 3 由不同复配溶剂制备的NiCoB催化剂的XRD谱图

Figure 3 XRD patterns of NiCoB catalysts prepared from different mixed solvent

a: NiCoB-MW; b: NiCoB-EW; c: NiCoB-EGW; d: NiCoB-ME; e: NiCoB-MEG; f: NiCoB-EEG; g: NiCoB-MEEG; h: NiCoB-MEEGW

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图 4 由不同单一溶剂制备的NiCoB催化剂的FE-SEM照片

Figure 4 FE-SEM images of fresh NiCoB catalysts prepared from different single solvent

(a): NiCoB-W; (b): NiCoB-M; (c): NiCoB-E; (d): NiCoB-EG; (e): NiCoB-PEG; (f): NiCoB-isoP; (g): NiCoB-nP

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图 5 由不同单一溶剂制备的NiCoB催化剂的XPS谱图

Figure 5 XPS spectra of fresh NiCoB catalysts prepared from different single solvent

a: NiCoB-W; b: NiCoB-M; c: NiCoB-E; d: NiCoB-EG; e: NiCoB-PEG; f: NiCoB-isoP; g: NiCoB-nP

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图 6 NiCoB-MEG催化剂在不同放大倍数下的FE-SEM照片

Figure 6 FE-SEM images of fresh NiCoB-MEG catalyst with different magnification times

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图 7 NiCoB-MEG催化剂的HRTEM照片和SAED照片

Figure 7 HRTEM images and SAED picture of fresh NiCoB-MEG catalyst

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图 8 NiCoB-M (a)、NiCoB-MEG (b)和NiCoB-EG (c)催化剂的XPS谱图

Figure 8 XPS spectra of fresh NiCoB-M (a), NiCoB-MEG (b) and NiCoB-EG (c) catalysts

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表 1 不同溶剂的物理参数^[27]

Table 1 Physical parameters of different solvent

表 2 由不同单一溶剂制备的NiCoB催化剂的织构参数和组成

Table 2 Textural parameters and composition of NiCoB catalysts prepared from different single solvent

表 3 由不同复配溶剂制备的NiCoB催化剂的织构参数

Table 3 Textural parameters of NiCoB catalysts prepared from different mixed solvent

表 4 由不同单一溶剂制备的NiCoB催化剂的糠醛加氢反应性能

Table 4 Hydrogenation results of furfural over the NiCoB catalysts prepared from different single solvent^a

表 5 由不同复配溶剂制备的NiCoB催化剂的糠醛加氢反应性能

Table 5 Hydrogenation results of furfural over the NiCoB catalysts prepared from different mixed solvent^a

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