氮化SBA-15负载高分散过渡金属用于丙烷高效直接脱氢

doi:10.19964/j.issn.1006-4990.2022-0316

Abstract

Abstract:

Dehydrogenation catalysts with different transition metals of Co，Ni，Fe，Cu were prepared by impregnation method with SBA-15 modified by nitridation method as carrier.The mesoporous structure of the support after nitridation was confirmed by X-ray diffraction（XRD） and N₂ adsorption desorption analysis.Scanning electron microscopy（SEM） confirmed that the metal was in a good state of high dispersion.Temperature programmed reduction（H₂-TPR） and X-ray photoelectron spectroscopy（XPS） proved that nitriding SBA-15 changed the electronic structure of the metal，and the interaction between the carrier and the metal was significantly enhanced.Metal-loaded samples with a content of 1% were prepared by quantitative impregnation method，and their properties were evaluated.The experimental results showed that the order of catalytic PDH activity of different metals for propane dehydrogenation was Co-SBA-15N900-1%，Fe-SBA-15N900-1%，Cu-SBA-15N900-1%，Ni-SBA-15N900-1%.The Co-SBA-15N900-1% exhibited a propane conversion of 33% and a propylene selectivity of 88%，indicating its promising utilization in industry.

Key words: dehydrogenation of propane, transition metals, high dispersion, nitrided SBA-15

CLC Number:

O643.3

LI Haitao,ZHAO Yinfeng. Nitriding SBA-15 loaded highly dispersed transition metals for efficient direct dehydrogenation of propane[J]. Inorganic Chemicals Industry, 2023, 55(2): 141-148.

Figures/Tables 17

Fig.1

Fig.2

Table 1

Table 2

Fig.3

Fig.4

Fig.5

Table 3

Fig.6

Fig.7

Table 4

Fig.8

Table 5

Fig.9

Fig.10

Fig.11

Fig.12

References 21

1	杜凯敏，范杰.丙烷氧化脱氢制丙烯研究进展[J].化工进展，2019，38（6）：2697-2706.
	DU Kaimin， FAN Jie.Research progress on oxidative dehydrogenation of propane to propene[J].Chemical Industry and Engineering Progress，2019，38（6）：2697-2706.
2	杨文建，孟广莹，李晓云，等.球形氧化铝的制备及其在丙烷脱氢催化剂中的应用[J].无机盐工业，2020，52（6）：87-91.
	YANG Wenjian， MENG Guangying， LI Xiaoyun，et al.Preparation of spherical alumina and its application in PDH[J].Inorganic Chemicals Industry，2020，52（6）：87-91.
3	SHI Lei， DENG Gaoming， LI Wencui，et al.Al₂O₃ nanosheets rich in pentacoordinate Al³⁺ions stabilize Pt-Sn clusters for propane dehydrogenation[J].Angewandte Chemie，2015，54（47）：13994-13998.
4	李超，王红秋.美国页岩气开发对化工市场的影响[J].中外能源，2015，20（2）：18-22.
	LI Chao， WANG Hongqiu.The influence of US shale gas development on the chemical market[J].Sino-Global Energy，2015，20（2）：18-22.
5	江丽，刘春艳，王红娟，等.国内外页岩气开发环境管理现状及对比[J].天然气工业，2021，41（12）：146-155.
	JIANG Li， LIU Chunyan， WANG Hongjuan，et al.Domestic and foreign environmental management of shale gas development：Status and comparison[J].Natural Gas Industry，2021，41（12）：146-155.
6	SOEDER D J.The successful development of gas and oil resources from shales in North America[J].Journal of Petroleum Science and Engineering，2018，163：399-420.
7	LIAN Zan， SI Chaowei，JAN F，et al.Coke deposition on Pt-based catalysts in propane direct dehydrogenation：Kinetics，suppression，and elimination[J].ACS Catalysis，2021，11（15）：9279-9292.
8	HU Zhongpan， YANG Dandan， WANG Zheng，et al.State-of-the-art catalysts for direct dehydrogenation of propane to propylene[J].Chinese Journal of Catalysis，2019，40（9）：1233-1254.
9	SHAO Huaiqi， HE Qihui， WANG Delong，et al.The active sites and catalytic properties of CrO _x /Zn-Al₂O₃ catalysts for propane dehydrogenation[J].Applied Catalysis A：General，2022，637.Doi：10.1016/j.apcata.2022.118610 . doi: 10.1016/j.apcata.2022.118610
10	BENI′TEZ J J， DIAZ A， LAURENT Y，et al.Characterisation，surface hydrolysis and nitrogen stability in aluminophosphate oxynitride（AlPON） catalysts[J].Applied Catalysis A：General，1999，176（2）：177-187.
11	XIA Hongde， WEI Kai.Equivalent characteristic spectrum analysis in TG-MS system[J].Thermochimica Acta，2015，602：15- 21.
12	赵银峰，刘中民，于政锡，等.一种质谱定量在线分析气态物质的方法[P].中国，114624314A，2020-12-15.
13	王硕，白丽明.钇沉积的二氧化钛-SBA-15纳米催化剂制备及其应用[J].无机盐工业，2019，51（3）：77-81.
	WANG Shuo， BAI Liming.Preparation and application of yttriumdeposited TiO₂-SBA-15 nano-catalyst[J].Inorganic Chemicals Industry，2019，51（3）：77-81.
14	邵艳秋，张宇婷，姜振双，等.水解剂氟化铵对Fe-SBA-15结构及催化性能的影响[J].无机盐工业，2019，51（9）：97-101.
	SHAO Yanqiu， ZHANG Yuting， JIANG Zhenshuang，et al.Effects of hydrolysate NH₄F on structure and catalytic properties of Fe-SBA-15[J].Inorganic Chemicals Industry，2019，51（9）：97-101.
15	BIAN Zhoufeng， DEWANGAN N， WANG Zhigang，et al.Mesoporous-silica-stabilized cobalt（II） oxide nanoclusters for propane dehydrogenation[J].ACS Applied Nano Materials，2021，4（2）：1112-1125.
16	蔺丹丹.SBA-15分子筛负载钴催化剂催化乙醇水蒸气重整反应性能的研究[D].太原：太原理工大学，2016.
	LIN Dandan.The study on ethanol steam reforming over molecular sieve SBA-15 supported cobalt catalyst[D].Taiyuan：Taiyuan University of Technology，2016.
17	HE Sufang， ZHANG Lei， HE Suyun，et al.Ni/SiO₂ catalyst prepared with nickel nitrate precursor for combination of CO₂ reforming and partial oxidation of methane：Characterization and deactivation mechanism investigation[J].Journal of Nanomaterials，2015，2015.Doi：10.1155/2015/659402 . doi: 10.1155/2015/659402
18	MILE B， STIRLING D， ZAMMITT M A，et al.TPR studies of the effects of preparation conditions on supported nickel catalysts[J].Journal of Molecular Catalysis，1990，62（2）：179-198.
19	ZHANG Shoumin， HUANG Weiping， QIU Xiaohang，et al.Comparative study on catalytic properties for low-temperature CO oxidation of Cu/CeO₂ and CuO/CeO₂ prepared via solvated metal atom impregnation and conventional impregnation[J].Catalysis Letters，2002，80（1/2）：41-46.
20	LUO Mengfei.TPR and TPD studies of CuOCeO₂ catalysts for low temperature CO oxidation[J].Applied Catalysis A：General，1997，162（1/2）：121-131.
21	冉瑶，许彪，丁森，等.不同分散度Co/Al₂O₃催化丙烷脱氢反
	应性能[J].天然气化工—C1化学与化工，2021，46（6）：33- 39.
	RAN Yao， XU Biao， DING Sen，et al.Catalytic performance of Co/Al₂O₃ with different dispersion for propane dehydrogenation[J].Natural Gas Chemical Industry，2021，46（6）：33-39.

样品	S_BET/（m²·g^-1）	V_BJH/（cm³·g^-1）	D_BJH/nm
SBA-15	539	1.20	8.9
SBA-15N900	422	0.95	7.4

样品	w（金属）/%	w（氮）/%
Co-SBA-15N900	2.34	3.21
Ni-SBA-15N900	1.82
Fe-SBA-15N900	1.85
Cu-SBA-15N900	2.46

样品	S_BET/（m²·g^-1）	V_BJH/（cm³·g^-1）	D_BJH/nm
Co-SBA-15N900	383	0.73	7.7
Ni-SBA-15N900	355	0.77	8.1
Fe-SBA-15N900	325	0.74	8.2
Cu-SBA-15N900	353	0.79	8.0

价态	2p_1/2/eV	2p_3/2/eV	卫星峰/eV
Co³⁺	796.4	780.6	784.6 803.2
Co²⁺	797.6	782.1	784.6 803.2
Ni⁰	870.1	855.3	874.9
Ni²⁺	871.9	856.5	879.1、861.5
Fe³⁺	724.4	711.0	718.8
Fe²⁺	722.6	709.0	714.7
Cu²⁺	953.7	933.5	941.9、943.0
Cu⁰	952.5	933.0

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Nitriding SBA-15 loaded highly dispersed transition metals for efficient direct dehydrogenation of propane

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 17

References 21

Related Articles 1

Metrics

Comments

Recommended 0