Pt-Re-MCM-41催化剂的制备、表征及其催化热解玉米芯制呋喃类化合物

doi:10.3969/j.issn.0253-2417.2020.02.011

Abstract

Abstract:

A series of Pt-Re-MCM-41 catalysts with different metal loading were prepared by step impregnation method with MCM-41 as support. The physical and chemical properties of the catalysts were characterized by nitrogen adsorption-desorption, X-ray diffraction (XRD) and NH₃ temperature programmed desorption (NH₃-TPD). The effect of Pt-Re-MCM-41 on the catalytic conversion of corncob pyrolysis products to furan compounds, including its repeated using and regeneration performance, were discussed. The experimental results showed that Pt and Re were uniformly dispersed on the catalyst surface, and the structure and properties of MCM-41 were not changed after loading, but the surface area, pore volume of the catalyst decreased and the average pore diameter increased after loading. The catalyst system had weak acid and medium strong acid at the same time. After Pt and Re loading, the content of the two acid sites on the catalyst surface increased. The type and number of compounds detected by GC×GC were, about 4-5 times than that detected by GC. The addition of the catalyst inhibited the production of alcohols, acids, nitrogen and sugars, and promoted the formation of ketones, furan and hydrocarbons, but had little effect on esters and phenols. The Pt-Re-MCM-41 catalyst could increase the GC content of furan compounds. The GC content could reach 33.12% with 1.0%Pt-1.0%Re-MCM-41 as catalyst and the catalytic temperature was 450℃ and increased by 12.11 percentage point compared with that without catalyst. Low catalytic temperature (≤ 450℃) was favorable for the formation of 2 (5H) -furanone and 2-furan methanol, and high catalytic temperature (≥ 500℃) was beneficial for furfural, 2-methylfuran and 3-furfural formation. The activity of the 1.0%Pt-1.0%Re-MCM-41 catalyst was reduced after three times, and the activity was basically recovered after calcination. Among them, the furan compound GC antent reached 32.6%.

Key words: catalytic conversion, Py-GC×GC-MS, Pt-Re-MCM-41, furan compounds, activity

CLC Number:

TQ35

Wenbin LI,Yunwu ZHENG,Shuirong LI,Yi LU,Zhifeng ZHENG. Preparation, Characterization of Pt-Re-MCM-41 Catalyst and Its Catalytic Conversion of Corncob for Producting Furan Compounds[J]. Chemistry and Industry of Forest Products, 2020, 40(2): 83-92.

Figures/Tables 9

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催化剂 catalysts	BET比表面积/(m²·g^-1) BET surface area	孔容/(cm³·g^-1) pore volume	孔径/nm pore size
MCM-41	1106.77	1.12	3.04
0.5%Pt-MCM-41	378.03	0.98	6.87
0.5%Re-MCM-41	218.63	0.82	7.83
0.5%Pt-0.5%Re-MCM-41	227.13	1.0	9.66
0.5%Pt-1.0%Re-MCM-41	247.64	0.92	6.58
1.0%Pt-0.5%Re-MCM-41	224.60	0.74	8.13
1.0%Pt-1.0%Re-MCM-41	222.14	0.68	7.64

催化剂 catalyst	醇类 alcohols	酸类 acids	醛类 aldehydes	酮类 ketones	酯类 esters	呋喃类 furans	碳氢化合物 hydrocarbons	酚类 phenols	含氮类 nitrogens	糖类 sugars	其他 others
无none	5.06	5.65	3.37	12.18	2.96	21.01	1.86	23.71	12.60	7.36	4.24
MCM-41	3.95	2.52	0.86	18.25	2.44	28.10	7.42	28.84	3.37	1.67	2.58
0.5%Pt-MCM-41	4.35	1.90	2.05	17.79	2.55	30.49	4.60	27.13	5.14	1.51	2.49
0.5%Re-MCM-41	4.20	3.92	1.82	21.45	3.34	27.25	3.83	24.77	3.23	2.19	4.00
0.5%Pt-0.5%Re-MCM-41	2.30	1.48	3.04	17.83	2.22	28.20	9.71	22.26	6.62	0.73	5.61
1.0%Pt-0.5%Re-MCM-41	4.92	2.80	1.99	14.63	2.04	25.99	13.81	25.28	5.58	1.65	1.31
0.5%Pt-1.0%Re-MCM-41	2.16	3.21	2.84	12.71	3.20	31.17	11.14	21.27	6.95	0.20	5.15
1.0%Pt-1.0%Re-MCM-41	4.79	1.58	3.80	14.75	1.65	33.12	2.24	23.61	9.79	1.38	3.29

催化剂 catalysts	糠醛 furfural	2(5H)-呋喃酮 2(5H)-furanone	2, 3-二氢苯并呋喃 2, 3-dihydro-benzofuran	2-呋喃甲醇 2-furanmethanol	2-甲基呋喃 furan-2-methyl	3-糠醛 3-furaldehyde
无none	4.60	1.96	7.94	1.06	0	0
MCM-41	8.20	2.52	7.39	3.29	0	0.18
0.5%Pt-MCM-41	7.27	2.71	9.60	2.56	3.48	0.09
0.5%Pt-0.5%Re-MCM-41	7.34	3.00	9.25	2.57	2.08	0.15
0.5%Pt-1.0%Re-MCM-41	8.92	2.64	7.25	0	3.51	0.21
1.0%Pt-1.0%Re-MCM-41	6.75	3.08	10.55	0	4.03	0.30
1.0%Pt-0.5%Re-MCM-41	5.71	3.10	7.83	2.31	3.01	0.17
0.5%Re-MCM-41	8.06	1.92	8.23	1.83	2.86	0.34

催化温度/℃ catalytic temperature	糠醛 furfural	2(5H)-呋喃酮 2(5H)-furanone	2, 3-二氢苯并呋喃 2, 3-dihydro-benzofuran	2-呋喃甲醇 2-furanmethanol	2-甲基呋喃 furan-2-methyl	3-糠醛 3-furaldehyde
350	3.78	3.31	9.57	1.69	3.57	0.16
400	5.20	3.05	10.32	3.35	0.10	0.15
450	6.75	3.08	10.55	0	4.03	0.30
500	6.45	2.50	7.85	0.37	0	0.12
550	9.22	0.30	12.13	0	5.95	0.06
600	9.29	0	9.42	0	6.94	0.43

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Preparation, Characterization of Pt-Re-MCM-41 Catalyst and Its Catalytic Conversion of Corncob for Producting Furan Compounds

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