负载于二氧化硅上的小尺寸氧化亚铜物种促进丙烯选择性氧化生成丙烯醛

doi:10.1016/S1872-2067(20)63636-1

催化学报 ›› 2021, Vol. 42 ›› Issue (2): 320-333.DOI: 10.1016/S1872-2067(20)63636-1

负载于二氧化硅上的小尺寸氧化亚铜物种促进丙烯选择性氧化生成丙烯醛

郭玲玲^a^,^h, 虞静^c, 王伟伟^d, 刘家旭^e^,^$(), 郭洪臣^e, 马超^f^,^¥(), 贾春江^d^,^#(), 陈俊翔^g, 司锐^a^,^b^,^*()

^a中国科学院上海应用物理研究所, 上海201800
^b张江实验室上海同步辐射光源, 上海201204
^c上海市计量测试技术研究院, 上海200233
^d山东大学化学与化工学院胶体与界面化学教育部重点实验室, 特种功能聚集体材料教育部重点实验室, 山东济南250100
^e大连理工大学化学与化工学院, 精细化工国家重点实验室, 辽宁大连116023
^f湖南大学材料科学与工程学院, 湖南长沙410082
^g泰逻集团科技有限公司中国事业部, 上海200090
^h中国科学院大学, 北京100049

收稿日期:2020-03-29 接受日期:2020-05-11 出版日期:2021-02-18 发布日期:2021-01-21
通讯作者: 刘家旭,马超,贾春江,司锐
基金资助:
国家自然科学基金(21773288);国家自然科学基金(21805167);国家自然科学基金(21771117);国家重点基础研究项目(2017YFA0403402);国家自然科学基金杰出青年科学家基金(21622106);山东省杰出人才科学基金(JQ201703);山东省博士基金(ZR2018BB010);山东省泰山学者项目;中央高校基本科研专项资金

Small-sized cuprous oxide species on silica boost acrolein formation via selective oxidation of propylene

Ling-Ling Guo^a^,^h, Jing Yu^c, Wei-Wei Wang^d, Jia-Xu Liu^e^,^$(), Hong-Chen Guo^e, Chao Ma^f^,^¥(), Chun-Jiang Jia^d^,^#(), Jun-Xiang Chen^g, Rui Si^a^,^b^,^*()

^aShanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China
^bShanghai Synchrotron Radiation Facility, Zhangjiang Laboratory, Shanghai 201204, China
^cShanghai Institute of Measurement and Testing Technology, Shanghai 200233, China
^dKey Laboratory for Colloid and Interface Chemistry, Ministry of Education, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, Shandong, China
^eState Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116023, Liaoning, China
^fCollege of Materials Science and Engineering, Hunan University, Changsha 410082, Hunan, China
^gDivision of China, TILON Group Technology Limited, Shanghai 200090, China
^hUniversity of Chinese Academy of Science, Beijing 100049, China

Received:2020-03-29 Accepted:2020-05-11 Online:2021-02-18 Published:2021-01-21
Contact: Jia-Xu Liu,Chao Ma,Chun-Jiang Jia,Rui Si
About author:^¥Tel: +86-731-88821727; E-mail: cma@hnu.edu.cn
^$Tel: +86-411-84986162; E-mail: liujiaxu@dlut.edu.cn;
^#Tel: +86-531-88363683; E-mail: jiacj@sdu.edu.cn;
^*Tel: +86-21-33932079; E-mail: sirui@sinap.ac.cn;
Supported by:
National Natural Science Foundation of China(21773288);National Natural Science Foundation of China(21805167);National Natural Science Foundation of China(21771117);National Key Basic Research Program of China(2017YFA0403402);Excellent Young Scientists Fund from NSFC(21622106);Outstanding Scholar Fund(JQ201703);Doctoral Fund from the Science Foundation of Shandong Province(China)(ZR2018BB010);Taishan Scholar Project of Shandong Province(China);Fundamental Research Funds for the Central Universities(China)

摘要/Abstract

摘要：

氧化物负载的含铜材料是丙烯选择性氧化制备丙烯醛的理想催化剂, 一直以来都受到人们的广泛关注. 然而, 对于该催化体系的结构与性能之间的关系仍不是很清楚. 因此, 我们以碳酸钠为沉淀剂, 通过沉积沉淀法将铜负载于高比表面的二氧化硅载体上, 从而得到了均匀分散且小尺寸的Cu/SiO₂催化剂. 另外, 采用浸渍法制得了相同负载量的分散不均匀、大尺寸的Cu/SiO₂催化剂. 丙烯选择性氧化反应活性测试发现, 沉积沉淀法制备的催化剂比浸渍法制备的更有利于丙烯醛的生成, 表现出了优异的催化性能: 在300 °C反应时, 丙烯的转化率达到25.5%, 丙烯醛的选择性达到66.8%, 对应的丙烯醛的生成速率高达10.5 mmol·h^-1·g_cat.^-1或111.2 mmol·h^-1·g_Cu^-1, 远远超出了浸渍法制备的催化剂性能(1.7 mmol·h^-1·g_cat.^-1或17.2 mmol·h^-1·g_Cu^-1)和文献中报道的结果. 结合高角度环形暗场扫描透射电子显微镜(HAADF-STEM)和X射线吸收精细结构(XAFS)技术, 对沉积沉淀法制备的催化剂进行表征, 发现在反应后铜物种的结构发生了明显的变化, 由小尺寸的氧化铜(CuO)团簇转变为氧化亚铜(Cu₂O)团簇, 并且铜物种的尺寸没有明显的增大. 为了进一步探索铜物种在预处理(氢气还原)以及催化反应时(丙烯+氧气)的结构变化, 对不同方法合成的两种催化剂进行了原位X射线粉末衍射测试, 发现不同尺寸的铜物种在还原和反应时都经历了从氧化铜(CuO)变为金属Cu再到Cu₂O的结构变化, 并且Cu₂O在320 min的反应过程中可以稳定存在, 说明它是该催化反应的活性物种. 另外, 通过原位双光束傅里叶变换红外光谱追踪反应时气体分子在催化剂表面的吸脱附状态, 发现丙烯可以有效地吸附在小尺寸Cu/SiO₂催化剂表面, 随着Cu₂O的形成, 检测到了烯丙基中间体(CH₂=CHCH₂*)的产生, 该物种可以与邻近Cu₂O上的一个氧发生反应, 从而生成丙烯醛, 因此结合N₂O滴定实验, 我们可认为, 高度分散的小尺寸的Cu₂O物种是丙烯进行高效选择性氧化反应生成丙烯醛的活性物种.

关键词: 丙烯选择性氧化, 氧化亚铜团簇, 形成丙烯醛, 活性物种, 原位表征

Abstract:

Oxide-supported copper-containing materials have attracted considerable research attention as promising candidates for acrolein formation. Nevertheless, the elucidation of the structure-performance relationships for these systems remains a scientific challenge. In this work, copper oxide clusters deposited on a high-surface-area silica support were synthesized via a deposition-precipitation approach and exhibited remarkable catalytic reactivity (up to 25.5% conversion and 66.8% selectivity) in the propylene-selective oxidation of acrolein at 300 °C. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy combined with X-ray absorption fine structure measurements of the catalyst before and after the reaction confirmed the transformation of the small-sized copper oxide (CuO) clusters into cuprous oxide (Cu₂O) clusters. With the aid of in situ X-ray diffraction and in situ dual beam Fourier transform infrared spectroscopy (DB-FTIR), the allyl intermediate (CH₂=CHCH₂*) was clearly observed, along with the as-formed Cu₂O species. The intermediate can react with oxygen atoms from neighboring Cu₂O species to form acrolein during the catalytic process, and the small-sized Cu₂O clusters play a crucial role in the generation of acrolein via the selective oxidation of propylene.

Key words: Propylene selective oxidation, Cuprous oxide cluster, Acrolein formation, Active species, In situ characterization

郭玲玲, 虞静, 王伟伟, 刘家旭, 郭洪臣, 马超, 贾春江, 陈俊翔, 司锐. 负载于二氧化硅上的小尺寸氧化亚铜物种促进丙烯选择性氧化生成丙烯醛[J]. 催化学报, 2021, 42(2): 320-333.

Ling-Ling Guo, Jing Yu, Wei-Wei Wang, Jia-Xu Liu, Hong-Chen Guo, Chao Ma, Chun-Jiang Jia, Jun-Xiang Chen, Rui Si. Small-sized cuprous oxide species on silica boost acrolein formation via selective oxidation of propylene[J]. Chinese Journal of Catalysis, 2021, 42(2): 320-333.

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https://www.cjcatal.com/CN/Y2021/V42/I2/320

图/表 11

Table 1 Catalytic performance of catalysts with different Cu weight percentages and particle sizes in propylene oxidation.

Sample	T (°C)	Conversion (%)	Selectivity (%)						r_acrolein (mmol·h^-1·g_Cu)	r_acrolein (mmol·h^-1·g_cat)	D_Cu2O^a (nm)
Sample	T (°C)	Conversion (%)	Acrolein	CO₂	PO	Acetone	Propanal	Aldehyde	r_acrolein (mmol·h^-1·g_Cu)	r_acrolein (mmol·h^-1·g_cat)	D_Cu2O^a (nm)
5Cu-DP	300	13.6	72.8	24.5	0.9	0.4	0.2	1.2	127.1	6.1	2.6
10Cu-DP	225	0.7	41.6	43.1	11.8	1.3	0.5	1.7	1.9	0.2	2.5
10Cu-DP	250	3.4	49.6	40.9	6.7	1.0	0.3	1.5	11.1	1.0	2.5
10Cu-DP	275	12.7	57.9	38.8	1.6	0.2	0.2	1.3	47.9	4.5	2.7
10Cu-DP	300	25.5	66.8	30.7	0.4	0.1	0.1	1.9	111.2	10.5	2.8
10Cu-DP	325	29.5	61.0	36.5	0.2	0.1	0.1	2.1	117.4	12.7	3.1
15Cu-DP	300	32.7	63.3	34.2	0.2	0.1	0.1	2.1	85.3	12.7	3.5
5Cu-IM	300	2.5	75.5	20.8	0.7	0.3	0.5	2.2	23.2	1.2	12.8
10Cu-IM	300	3.8	74.7	22.0	0.4	0.6	0.4	1.9	17.2	1.7	20.3
15Cu-IM	300	4.3	72.5	23.9	0.8	0.5	0.4	1.9	12.8	1.9	28.3

Fig. 1. Catalytic performance of the Cu/SiO2 catalysts. (a) Temperature dependence of the catalytic activity of 10Cu-DP in the range 225-325 °C; (b) Cu-loading dependence of the catalytic activity of the copper-silica catalysts at 300 °C; Comparisons of (c) the propylene conversion and acrolein selectivity with time on stream and (d) the acrolein formation rates of 10Cu-DP and 10Cu-IM in the selective oxidation of propylene at 300 °C. Reaction conditions: 0.1 g catalyst, C3H6:O2:N2/Ar = 2.5:2.5:45, 30000 cm3·h-1·gcat-1.

Fig. 2. XRD patterns of the copper-silica catalysts prepared by deposition-precipitation method. (a) Fresh; (b) used.

Fig. 3. Cu K-edge XANES profiles (a, c) and EXAFS fitting results (b, d) in R space for fresh (a, b) and used (c, d) copper-silica samples prepared by the deposition-precipitation method.

Table 2 EXAFS fitting results for fresh copper-silica samples with different Cu loadings.

Sample	Cu-O		Cu-Cu
Sample	R (Å)	CN	R (Å)	CN
CuO 5Cu-DP	1.948 1.89 ± 0.01	4 2.9 ± 0.2	2.935 2.99 ±0.02	10 2.3 ± 0.6
10Cu-DP	1.93 ± 0.01	4.7 ± 0.2	2.96 ± 0.01	3.1 ± 0.6
15Cu-DP	1.93 ± 0.01	4.7 ± 0.2	2.96 ± 0.01	3.0 ± 0.6

Table 3 EXAFS fitting results of used 10Cu-DP samples.

Sample	Cu-O		Cu-Cu
Sample	R (Å)	CN	R (Å)	CN
Cu₂O	1.849	2	3.019	12
Cu₂O	3.540	6	3.019	12
10Cu-DP-275-used	1.87 ± 0.01	1.9 ± 0.1	2.56 ± 0.01	3.1 ± 1.2
10Cu-DP-275-used	3.51 ± 0.02	2.9 ± 0.6	2.94 ± 0.02	3.3 ± 1.6
10Cu-DP-300-used	1.87 ± 0.01	2.3 ± 0.1	3.00 ± 0.01	4.4 ± 1.4
10Cu-DP-300-used	3.55 ± 0.03	2.0 ± 0.7	3.00 ± 0.01	4.4 ± 1.4
10Cu-DP-325-used	1.87 ± 0.01	2.3 ± 0.1	3.00 ± 0.01	4.8 ± 1.5
10Cu-DP-325-used	3.55 ± 0.02	2.3 ± 0.7	3.00 ± 0.01	4.8 ± 1.5

Fig. 4. Aberration-corrected HAADF-STEM images of (a) fresh and (b) used 10Cu-DP. (c) Schematic of the synthesis and structural transformation of 10Cu-DP.

Fig. 5. Structural evolution of the Cu/SiO2 catalysts. In situ XRD patterns of 10Cu-DP (a, b) and 10Cu-IM (c, d) during hydrogen reduction at different temperatures (a, c) and the propylene oxidation reaction (b, d).

Fig. 6. Dissociation adsorption ability of 10Cu-DP. In situ DB-FTIR results for 10Cu-DP during (a) propylene adsorption at 300 °C under a flowing mixture of propylene and nitrogen gases at a time on stream of 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 12, 14, 16, 18, 20, 22, 24, 26, 28, and 30 min (0.01 g catalyst, C3H6:N2 = 2.5: 90, 92.5 mL·min-1, 1 atm), and (b) propylene and oxygen coadsorption at 300 °C under a flowing mixture of propylene, oxygen, and nitrogen gases at a time on stream of 1, 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, and 90 min (0.01 g catalyst, C3H6:O2:N2 = 2.5:2.5:90, 95 mL·min-1, 1 atm).

Fig. 7. Dissociation adsorption ability of 10Cu/SiO2-IM. In situ DB-FTIR results for 10Cu/SiO2-IM during (a) propylene adsorption at 300 °C under a flowing mixture of propylene and nitrogen gases at a time on stream of 2, 5, 10, 15, 20, 25, and 30 min (0.01 g catalyst, C3H6:N2 = 2.5:90, 92.5 mL·min-1, 1 atm), and (b) propylene and oxygen coadsorption at 300 °C under a flowing mixture of propylene, oxygen, and nitrogen gases with a time on stream of 1, 5, 10, 15, 20, 30, 40, 50, 60, 70, 80, and 90 min (0.01 g catalyst, C3H6:O2:N2 = 2.5:2.5:90, 95 mL·min-1, 1 atm).

Fig. 8. H2-TPR profiles of 10Cu-DP and 10Cu-IM. Dashed and solid lines are the hydrogen consumption profiles measured for the first (after O2 pretreatment) and second (after N2O oxidation) runs, respectively.

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负载于二氧化硅上的小尺寸氧化亚铜物种促进丙烯选择性氧化生成丙烯醛

Small-sized cuprous oxide species on silica boost acrolein formation via selective oxidation of propylene

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