Analyzing HDPE Thermal and Catalytic Degradation in Hydrogen Atmosphere: A Model-Free Approach to the Activation Energy
Abstract
:1. Introduction
2. Theoretical Approach
3. Results
3.1. Catalyst Characterization
3.2. Thermogravimetric Analysis
3.3. Thermal and Catalytic Cracking Kinetics
3.3.1. Apparent Activation Energy (Ea)
3.3.2. Effect of Adding a Metallic Source (Ni, Pt, Pd) to H-USY (15) and H-ZSM-5 (11.5) on the Kinetic Parameters
4. Materials and Methods
4.1. Materials
4.2. Catalyst Preparation
4.3. Catalyst Characterization
4.4. Thermogravimetric Analysis Procedure
5. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
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Method | Expression | Plot |
---|---|---|
Flynn-Wall-Ozawa (FWO) | vs. 1/T | |
Kissinger–Akahira–Sunose (KAS) | vs. 1/T |
Catalyst | Crystallinity (%) | Sext (m2/g) | Vmicro (cm3/g) | Vmeso (cm3/g) | Vtotal (cm3/g) | Weak Acidity (μmol/g) | Strong Acidity (μmol/g) | Total Acidity (μmol/g) |
---|---|---|---|---|---|---|---|---|
H-USY (15) | 100 | 189 | 0.25 | 0.23 | 0.48 | 332 | 319 | 651 |
Ni (5)/H-USY (15) | 97.4 | 170 | 0.24 | 0.24 | 0.48 | 288 | 245 | 533 |
Pt (0.5)/H-USY (15) | 93.7 | 184 | 0.24 | 0.24 | 0.48 | 364 | 256 | 620 |
Pd (0.5)/H-USY (15) | 93.7 | 180 | 0.24 | 0.23 | 0.47 | 324 | 301 | 625 |
HZSM-5 (11.5) | 100 | 114 | 0.13 | 0.10 | 0.23 | 740 | 530 | 1270 |
Ni (5)/H-ZSM-5 (11.5) | 91.2 | 78 | 0.12 | 0.07 | 0.19 | 670 | 500 | 1170 |
Pt (0.5)/H-ZSM-5 (11.5) | 95.7 | 61 | 0.10 | 0.05 | 0.15 | 650 | 530 | 1180 |
Pd (0.5)/H-ZSM-5 (11.5) | 97.6 | 77 | 0.10 | 0.06 | 0.17 | 650 | 500 | 1150 |
Sample | β (°C/min) | Temperature (°C) | |||
---|---|---|---|---|---|
T5% | T50% | T95% | Tm | ||
HDPE | 5 | 433 | 463 | 473 | 468 |
10 | 433 | 478 | 488 | 480 | |
15 | 455 | 484 | 494 | 488 | |
20 | 463 | 489 | 501 | 493 | |
HDPE + H-USY (15) | 5 | 255 | 354 | 398 | 392 |
10 | 271 | 370 | 410 | 399 | |
15 | 289 | 382 | 418 | 408 | |
20 | 292 | 394 | 431 | 418 | |
HDPE + H-ZSM-5 (11.5) | 5 | 283 | 362 | 397 | 389 |
10 | 318 | 407 | 428 | 421 | |
15 | 325 | 413 | 430 | 432 | |
20 | 329 | 421 | 443 | 442 |
x | FWO | KAS | |||||
---|---|---|---|---|---|---|---|
Ea (kJ/mol) | ln(A/G(x)) | R2 | Ea (kJ/mol) | ln(A/G(x)) | R2 | ||
HDPE | 0.2 | 212.5 | 33.8 | 1.000 | 211.2 | 33.5 | 1.000 |
0.3 | 220.9 | 34.9 | 1.000 | 220.0 | 34.8 | 1.000 | |
0.4 | 226.9 | 35.8 | 0.999 | 226.2 | 35.6 | 0.999 | |
0.5 | 229.2 | 36.0 | 0.999 | 228.6 | 35.9 | 0.999 | |
0.6 | 232.0 | 36.3 | 0.999 | 231.5 | 36.2 | 0.999 | |
0.7 | 232.7 | 36.3 | 0.999 | 232.3 | 36.2 | 0.999 | |
0.8 | 233.0 | 36.2 | 0.999 | 233.0 | 36.1 | 0.999 | |
0.9 | 234.1 | 36.3 | 0.999 | 233.7 | 36.1 | 0.999 | |
Av. | 227.7 | 35.7 | 0.999 | 227.1 | 35.6 | 0.999 | |
HDPE+ H-USY (15) | 0.2 | 83.8 | 16.1 | 0.919 | 78.3 | 14.4 | 0.899 |
0.3 | 93.1 | 17.4 | 0.976 | 87.7 | 15.8 | 0.971 | |
0.4 | 104.7 | 19.1 | 0.998 | 99.5 | 17.6 | 0.997 | |
0.5 | 115.0 | 20.5 | 0.988 | 110.2 | 19.3 | 0.985 | |
0.6 | 126.0 | 22.2 | 0.979 | 121.6 | 21.1 | 0.975 | |
0.7 | 137.0 | 23.9 | 0.970 | 133.0 | 22.9 | 0.965 | |
0.8 | 148.8 | 25.7 | 0.967 | 145.3 | 24.9 | 0.961 | |
0.9 | 172.2 | 29.6 | 0.988 | 157.5 | 23.8 | 0.810 | |
Av. | 122.6 | 21.8 | 0.973 | 116.6 | 20.0 | 0.946 | |
HDPE+ H-ZSM-5 (11.5) | 0.2 | 60.6 | 10.9 | 0.889 | 53.3 | 7.8 | 0.849 |
0.3 | 63.5 | 11.1 | 0.900 | 56.1 | 8.6 | 0.865 | |
0.4 | 69.5 | 11.9 | 0.904 | 62.2 | 9.6 | 0.873 | |
0.5 | 76.6 | 13.0 | 0.909 | 69.6 | 10.8 | 0.882 | |
0.6 | 84.3 | 14.2 | 0.915 | 77.5 | 12.2 | 0.892 | |
0.7 | 91.2 | 15.3 | 0.918 | 84.7 | 13.4 | 0.897 | |
0.8 | 98.5 | 16.4 | 0.926 | 92.2 | 14.7 | 0.908 | |
0.9 | 106.9 | 17.7 | 0.929 | 122.2 | 17.1 | 0.994 | |
Av. | 81.4 | 13.8 | 0.911 | 77.2 | 11.8 | 0.895 |
x | Ni/H-USY (15) | Pt/H-USY (15) | Pd/H-USY (15) | |||
Ea (kJ/mol) | ln(A/G(x)) | Ea (kJ/mol) | ln(A/G(x)) | Ea (kJ/mol) | ln(A/G(x)) | |
0.2 | 153.4 | 30.4 | 219.3 | 45.1 | 202.2 | 43.8 |
0.3 | 149.7 | 28.8 | 182.5 | 36.1 | 180.4 | 35.4 |
0.4 | 141.3 | 26.6 | 165.3 | 31.8 | 161.2 | 32.3 |
0.5 | 134.3 | 24.8 | 153.4 | 28.9 | 149.7 | 29.2 |
0.6 | 131.4 | 23.9 | 144.0 | 26.6 | 144.5 | 28.5 |
0.7 | 132.9 | 23.9 | 136.6 | 24.7 | 132.2 | 26.7 |
0.8 | 137.7 | 24.5 | 131.5 | 23.4 | 123.5 | 25.3 |
0.9 | 159.6 | 28.2 | 130.0 | 22.7 | 127.6 | 24.5 |
Av.* | 142.5 | 26.4 | 157.8 | 29.9 | 152.6 | 30.7 |
x | Ni/H-ZSM-5 (11.5) | Pt/H-ZSM-5 (11.5) | Pd/H-ZSM-5 (11.5) | |||
Ea (kJ/mol) | ln(A/G(x)) | Ea (kJ/mol) | ln(A/G(x)) | Ea (kJ/mol) | ln(A/G(x)) | |
0.2 | 92.2 | 17.8 | 70.4 | 12.0 | 68.3 | 15.3 |
0.3 | 95.3 | 18.1 | 72.2 | 12.0 | 70.1 | 16.1 |
0.4 | 101.9 | 19.0 | 77.8 | 12.8 | 73.4 | 16.1 |
0.5 | 109.2 | 20.2 | 85.4 | 14.0 | 77.2 | 15.1 |
0.6 | 117.8 | 21.6 | 93.1 | 15.2 | 83.2 | 15.4 |
0.7 | 126.6 | 23.0 | 99.9 | 16.3 | 87.2 | 16.1 |
0.8 | 133.4 | 24.1 | 107.5 | 17.5 | 90.5 | 17.1 |
0.9 | 147.3 | 26.4 | 115.3 | 18.8 | 98.2 | 18.7 |
Av.* | 115.5 | 21.3 | 90.2 | 14.8 | 87.0 | 16.2 |
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Costa, C.S.; Fernandes, A.; Munoz, M.; Ribeiro, M.R.; Silva, J.M. Analyzing HDPE Thermal and Catalytic Degradation in Hydrogen Atmosphere: A Model-Free Approach to the Activation Energy. Catalysts 2024, 14, 514. https://doi.org/10.3390/catal14080514
Costa CS, Fernandes A, Munoz M, Ribeiro MR, Silva JM. Analyzing HDPE Thermal and Catalytic Degradation in Hydrogen Atmosphere: A Model-Free Approach to the Activation Energy. Catalysts. 2024; 14(8):514. https://doi.org/10.3390/catal14080514
Chicago/Turabian StyleCosta, Cátia S., A. Fernandes, Marta Munoz, M. Rosário Ribeiro, and João M. Silva. 2024. "Analyzing HDPE Thermal and Catalytic Degradation in Hydrogen Atmosphere: A Model-Free Approach to the Activation Energy" Catalysts 14, no. 8: 514. https://doi.org/10.3390/catal14080514