PdAg/CDs复合催化剂的制备及其葡萄糖氢解性能研究

陈德权; 王安; 包桂蓉; 高鹏; 罗嘉; 吉学武; 邓文瑶; 刘力

doi:10.1016/S1872-5813(23)60340-8

PdAg/CDs复合催化剂的制备及其葡萄糖氢解性能研究

doi: 10.1016/S1872-5813(23)60340-8

陈德权^{1, 2,},
王安^{1, 2,},
包桂蓉^{1, 2, ,},
高鹏^{1, 2,},
罗嘉^3,,
吉学武^{1, 2,},
邓文瑶^{1, 2,},
刘力^{1, 2,}

1.
昆明理工大学冶金与能源工程学院, 云南昆明 650093
2.
省部共建复杂有色金属资源清洁利用国家重点实验室, 云南昆明 650093
3.
中国科学院西双版纳热带植物园, 云南昆明 650223

基金项目: 国家自然科学基金(51966008)项目资助

详细信息

作者简介:
陈德权(1997-),男，硕士研究生，主要从事以碳点为载体双金属纳米催化剂的制备及性能研究工作。E-mail:1092860687@qq.com

通讯作者:
E-mail: 1633940830@qq.com

中图分类号: TK6
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- 被引次数: 0
出版历程
- 收稿日期: 2022-11-13
- 修回日期: 2023-01-11
- 录用日期: 2023-01-13
- 网络出版日期: 2023-02-27
- 刊出日期: 2023-09-30

Preparation of the PdAg/CDs composite and its catalytic performance in the hydrogenolysis of glucose

CHEN De-quan^{1, 2
,},
WANG An^{1, 2
,},
BAO Gui-rong^{1, 2
, ,},
GAO Peng^{1, 2
,},
LUO Jia^3
,,
JI Xue-wu^{1, 2
,},
DENG Wen-yao^{1, 2
,},
LIU Li^{1, 2
,}

1.
Faculty of Metallurgy and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China
2.
State Key Laboratory of Complex Non-ferrous Metal Resource Utilization, Kunming 650093, China
3.
Xishuangbanna Tropical Botanical Garden, Chinese Academy of Sciences, Kunming 650223, China

Funds: The project was supported by the National Natural Science Foundation of China (51966008)

摘要

摘要: 以碳点（carbon dots, CDs）为还原剂和载体，采用简便的光照还原法制备出了PdAg/CDs复合催化剂。XRD、TEM、FT-IR和XPS等技术对催化剂的表征分析，结果表明该催化剂平均粒径为10.45 nm，Pd和Ag主要以零价态的合金形式负载在碳点表面。将PdAg/CDs复合催化剂用于水中葡萄糖的氢解，催化评价结果表明，在初始H₂压力为4 MPa、葡萄糖100 mg、催化剂25 mg、反应温度140 ℃的条件下反应3 h，该催化剂显示出较好的氢解活性，葡萄糖的转化率为68.85%，氢解产物丙酮醇的收率达到8.36%。
- PdAg/CDs复合催化剂 /
- 葡萄糖 /
- 氢解 /
- 碳点
Abstract: With carbon dots (CDs) as the reducing agent and support, a PdAg/CDs composite catalyst was prepared by simple light reduction method. The results of XRD, TEM, FT-IR and XPS characterization indicate that the PdAg/CDs composite has an average particle size of about 10.45 nm, where Pd and Ag exist on the surface of CDs mainly in the alloy form of zero valence. The catalytic performance of the PdAg/CDs composite was evaluated in the hydrogenolysis of glucose in water. The results illustrate that the PdAg/CDs composite catalyst is highly active in the glucose hydrogenolysis; after reaction for 3 h under 140 °C, 4 MPa of initial H₂ pressure, 100 mg of glucose and 25 mg of catalyst, the conversion of glucose is 68.85% and the yield of acetol reaches 8.36%.
- PdAg/CDs catalyst /
- glucose /
- hydrogenolysis /
- carbon dots

HTML全文

FIG. 2670. FIG. 2670.

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图 1 PdAg/CDs复合催化剂的EDS元素分析

Figure 1 EDS elemental analysis of the PdAg/CDs composite catalyst

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图 2 CDs与PdAg/CDs复合催化剂的XRD谱图

Figure 2 XRD patterns of the CDs support and PdAg/CDs composite catalyst

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图 3 (a)CDs和(b) PdAg/CDs复合催化剂的TEM照片

Figure 3 TEM analysis of the CDs support (a) and PdAg/CDs composite catalyst (b)

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图 4 PdAg/CDs复合催化剂的EDS mapping分析

Figure 4 EDS mapping analysis of the PdAg/CDs composite catalyst: (a) electron image; EDS elemental mapping of (b) Ag, (c) Pd

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图 5 CDs与PdAg/CDs复合催化剂的FT-IR谱图

Figure 5 FT-IR spectra of the CDs support and PdAg/CDs composite catalyst

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图 6 PdAg/CDs复合催化剂的XPS能谱谱图

Figure 6 XPS spectrum of PdAg/CDs composite catalyst： (a) full spectrum; high-resolution spectrum of (b) C 1s, (c) O 1s; (d) N 1s; (e) Pd 3d; (f) Ag 3d

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图 7 PdAg/CDs复合催化剂的制备机理示意图

Figure 7 Preparation mechanism of PdAg/CDs composite catalyst

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图 8 葡萄糖催化/非催化氢解产物的GC-MS总离子流图

Figure 8 GC-MS total ion chromatograms of the products from glucose hydrogenolysis without and with the PdAg/CDs catalyst

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图 9 葡萄糖催化氢解的反应路径示意图

Figure 9 Proposed reaction pathways of glucose hydrogenolysis over the PdAg/CDs composite catalyst

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表 1 葡萄糖催化氢解的产物成分

Table 1 Product components of glucose catalyzed hydrogenolysis

Serial number	Substance		Relative content /%
Serial number	Substance		without catalyst	Pd/CDs	Ag/CDs	PdAg/CDs
1	formic acid	acids	1.33	2.34	2.33	1.3
2	acetic acid		4.12	13.8	14.07	5.48
3	3-deoxy-d-mannonic acid		14.1	13.1	−	10.19
4	4-methyloctanoic acid		−	−	−	2.06
	subtotal of acids		19.55	29.24	16.4	19.03
5	DL-arabinose	saccharide	4.88	−	−	3.39
6	other sugars	saccharide	33.83	−	−	−
	subtotal of saccharides		38.71	−	−	3.39
7	1-hydroxy-2-butanone	ketones	−	1.79	1.49	4.07
8	1,3-dihydroxyacetone		3.72	−	−	5.17
9	3-hydroxydihydro-2(3H)-furanone		1.25	−	−	−
10	furaneol		0.88	1.19	4.05	4.63
11	4H-pyran-4-one		2.26	−	0.68	−
	subtotal of ketones		8.11	2.98	6.22	13.87
12	acetol	alcohols	10.71	33.94	44.72	40.28
13	2,6-dimethyl-3-heptanol		−	−	−	3.23
14	tetrahydropyran-2-methanol		−	−	2.23	1.07
	subtotal total of alcohols		10.71	33.94	46.95	44.58
15	5-hydroxymethylfurfural	aldehydes	22.92	−	−	0.99
	subtotal total of alcohols		22.92	−	−	0.99
16	others		−	33.84	30.43	18.14
	total		100	100	100	100
Reaction condition: 100 mg glucose; 25 mg catalyst; 30 mL deionized water; reaction temperature 140 ℃; reaction time 3 h and 4 MPa H₂

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表 2 不同催化剂对葡萄糖氢解转化率及产物收率的影响

Table 2 Conversion of glucose and yield of products for the glucose hydrogenolysis over different catalysts

Catalyst	Conversion/%	Yield/%
Catalyst	Conversion/%	acetol	5-hydroxymethylfurfural	others
Without catalyst	31.45	2.09	14.78	14.58
Ag/CDs	37.60	6.23	0	31.37
Pd/CDs	51.46	5.41	0	46.05
PdAg/CDs	68.85	8.36	0.68	59.81

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