Estabilidade de Fases em Processos Industriais de Polimerização

Transcrição

Estabilidade de Fases em Processos Industriais de
Polimerização de Eteno a Alta Pressão
Gloria Meyberg Nunes Costa
TESE SUBMETIDA AO CORPO DOCENTE DO PROGRAMA DE PÓSGRADUAÇÃO EM ENGENHARIA INDUSTRIAL DA UNIVERSIDADE FEDERAL
DA BAHIA COMO PARTE DOS REQUISITOS NECESSÁRIOS PARA A
OBTENÇÃO DO GRAU DE DOUTOR EM CIÊNCIAS EM ENGENHARIA
INDUSTRIAL.
Aprovada1 por:
PRIMEIRA TESE DE DOUTORADO EM ENGENHARIA DO ESTADO DA BAHIA
SALVADOR, BA - BRASIL
SETEMBRO DE 2009
1
Por unanimidade e com distinção. De acordo com o Regimento do Programa, o conjunto de orientadores
tem direito a um único voto na banca de avaliação.
C837
Costa, Gloria Meyberg Nunes
Estabilidade de fases em processos industriais de
polimerização de eteno a alta pressão / Gloria Meyberg Nunes
Costa. – Salvador, 2009.
366 f. : il. color.
Orientador: Prof. Marcelo Embiruçu
Prof. Silvio Alexandre Beisl Vieira de Melo
Prof. Fernando Luiz Pelegrini Pessoa
Tese (Doutorado) – Universidade Federal da Bahia. Escola
Politécnica, 2009.
1. Polietileno. 2. Polimerização. 3. Processos químicos. I.
Embiruçu, Marcelo. II. Melo, Silvio Alexandre Beisl Vieira de.
III. Pessoa, Fernando Luiz Pelegrini. IV. Universidade Federal da
Bahia. V. Título.
CDD.: 547.7
Costa, G.-Tese de D.Sc., PEI/EP/UFBA, 2009
Preliminares
Agradecimentos
Em primeiro lugar gostaria de agradecer imensamente meus orientadores professores
Marcelo Embiruçu, Silvio Alexandre Beisl Vieira de Melo e Fernando Luiz Pelegrini
Pessoa pela maravilhosa orientação, imensa gama de conhecimento que sempre me
passaram, incentivo, ajuda, dedicação, atenção e principalmente a eterna amizade que
nos une meus amigos irmãos. Agradeço pela oportunidade e ajuda de transformar em
realidade um sonho. Com toda certeza vocês são exemplo de dignidade do mais alto
nível, são símbolo de tudo de mais maravilhoso que um ser humano possa ter. Sou
eternamente grata por tudo.
Agradeço a meus filhos, Tissiana, Talita e Raoni, meu marido Pedro Luiz, minhas
amigas irmãs, Zunara Leite e Rosana Melo, meus amigos e amigas pelo carinho, atenção
incentivo, enfim por tudo.
À Fapesb pelo apoio financeiro.
A Denise Sara Key pela cooperação, ajuda e atenção na correção dos textos em inglês.
iii
Preliminares
Dedicatória
Dedico esta tese a meus filhos Tissiana, Talita, Raoni e meu marido Pedro Luiz, por
tudo que representam para mim.
iv
Preliminares
Índice
Capítulo I. Introdução
I.1.
Motivação e importância
3
I.2.
Os objetivos e a organização do trabalho realizado
5
Referências bibliográficas
8
Capítulo II. Modelagem do equilíbrio de fases em sistemas poliméricos
II.1.
II.1.1.
Introdução
Descrição sucinta da planta de PEBD (PoliEtileno de Baixa
13
15
Densidade)
II.1.2.
Descrição sucinta da planta de PELBD (PoliEtileno Linear de
18
Baixa Densidade)
II.2.
II.2.1.
Revisão bibliográfica
Equações de estado cúbicas e regras de mistura
24
24
II.2.1.1.
Regras de mistura do tipo van der Waals
26
II.2.1.2.
Regras de mistura que incorporam modelos de GE
26
II.2.1.3.
Modelagem de sistemas poliméricos usando equações de
32
estado que incorporam modelos de GE
II.2.2.
Modelos de rede
34
II.2.2.1.
Equação de Sanchez e Lacombe
36
II.2.2.2.
Modelagem de sistemas poliméricos usando a equação de
38
Sanchez e Lacombe
II.2.3.
Modelos de perturbação
42
II.2.3.1.
Equações de estado para moléculas constituídas por cadeias
42
II.2.3.2.
Equações de estado para fluidos que se associam
45
II.2.3.3.
Equação de estado PC-SAFT
46
II.2.3.4.
Modelagem de sistemas poliméricos utilizando as equações
47
SAFT e PC-SAFT
II.2.4.
II.3.
Estabilidade de fases
Modelagem Termodinâmica
52
66
II.3.1.
Modelagem do equilíbrio de fases
66
II.3.2.
Equações de estado
67
II.3.2.1.
Equação de estado de Soave-Redlich-Kwong
67
v
Preliminares
II.3.2.1.1.
Regras de mistura
68
II.3.2.1.2.
Modelo de Bogdanic e Vidal para GE
71
II.3.2.2.
Equação de estado de Sanches e Lacombe
73
II.3.2.3.
Equação de estado PC-SAFT
75
II.3.3.
II.3.3.1.
II.4.
Estabilidade de fases
Análise da distância do plano tangente
80
80
Conclusões
87
88
Capítulo III. Predição do equilíbrio líquido-vapor e do equilíbrio líquido-líquido
para sistemas poliméricos: comparação de modelos de coeficiente de atividade
III.1.
Introduction
106
III.2.
Thermodynamic models
107
III.3.
Results and discussion for vapor liquid equilibrium
112
III.4.
Results and discussion for liquid-liquid equilibrium
127
III.5.
Conclusion
137
List of symbols
139
Greek letters
139
Superscripts
139
Subscripts
140
Abbreviations
140
References
142
Capítulo IV. Simulação da separação flash em processos industriais de polietileno:
comparação das equações de estado SRK e SL
IV.1.
Introduction
148
IV.2.
Process description
150
IV.2.1.
Low-density polyethylene (LDPE) processing
150
IV.2.2.
Linear low density polyethylene (LLDPE) processing
151
IV.3.
153
IV.3.1.
Sanchez–Lacombe (SL)
153
IV.3.2.
Soave-Redlich-Kwong equation of state
154
IV.3.3.
Mixing rules
154
IV.3.3.1.
van der Waals one-fluid (VDW) mixing rule [28]
154
IV.3.3.2.
Wong-Sandler mixing rule
155
vi
Preliminares
IV.3.3.3.
LCVM mixing rule
156
IV.3.3.4.
Excess Gibbs free energy (GE) model
156
IV.4.
Results and discussion
159
IV.4.1.
General observations
159
IV.4.2.
Assumptions used to obtain the experimental data in the
161
separation stage of the process in LDPE plant
IV.4.3.
Assumptions used to obtain experimental data in the separation
162
stage of the LLDPE processing plant
IV.4.4.
IV.4.4.1.
Simulation results
Binary interaction parameters of the models for simulation of
165
166
the LPS (LDPE resin)
IV.4.4.2.
168
the HPS (LDPE resin)
IV.4.4.3.
178
the IPS separator (LLDPE resin)
IV.4.4.4.
Comparison of the LPS overhead composition for LDPE resin
181
IV.4.4.5.
Comparison of the HPS overhead and bottom compositions for 185
LDPE resin
IV.4.4.6.
Comparison of IPS overhead and bottom stream compositions
191
for LLDPE resin
IV.4.4.7.
Comparison of HPS overhead and bottom compositions for
195
LLDPE resin using parameter values estimated for LPS
IV.5.
Conclusions
198
List of symbols
199
Greek letters
200
Superscripts
200
Subscripts
200
References
202
Capítulo V. Modelagem do equilíbrio sólido-líquido para soluções de polietileno e
poliproplileno com equações de estado
V.1.
Introduction
212
V.2.
214
Solubility basic equation
214
V.2.1.
vii
Preliminares
V.2.2.
PC-SAFT equation of state
214
V.2.3.
SRK equation of state
215
V.2.3.1.
WS mixing rule
215
V.2.3.2.
LCVM mixing rule
216
V.2.3.3.
Excess Gibbs free energy model
216
Experimental data and general approach to calculate SLE
219
V.3.1.
Experimental data
219
V.3.2.
Polymer properties for thermodynamic models
222
V.3.3.
Numerical solution procedure
223
Results and discussion for SLE at atmospheric pressure
225
V.4.1.
Parameter estimation for non-associated systems
225
V.4.2.
Parameter estimation for associated systems
226
V.4.3.
Predictive correlations
227
Results and discussion for SLE at high pressure
229
V.5.1.
Parameter estimation
229
V.5.2.
Predictive correlations
230
V.5.3.
Graphic analysis of solvent, pressure range, polymer molecular
235
V.3.
V.4.
V.5.
weight and composition effects on model performance
V.5.3.1.
Calculations with average estimated parameters
235
V.5.3.2.
Calculations with predictive correlations
236
V.5.3.3.
Interpolating and extrapolating parameter correlations for systems 241
not used in parameter estimation
V.6.
Conclusions
244
List of symbols
246
Greek letters
247
Superscripts
247
Subscripts
247
Abbreviations
248
References
249
Appendix V.1. SLE calculations at high pressure with SRK+WS model
251
Capítulo VI. Cálculo da distância para a transição de fases em diagramas pressãotemperatura para soluções de polietileno
VI.1.
Introduction
259
viii
VI.2.
VI.2.1.
Preliminares
Mathematical model development
262
Polymer-solvent phase behavior and LLDPE process operating
262
conditions
VI.2.2.
Thermodynamic model
269
Calculation procedures, results and discussion
272
Binary systems
272
VI.3.1.1.
Calculation procedure for the LCST, LV and LLV curves
272
VI.3.1.2.
Calculation procedure for the crystallization boundary
273
VI.3.1.3.
274
Multicomponent systems
280
VI.3.2.1.
Calculation procedure for the LCST, LV and LLV curves
280
VI.3.2.2.
Calculation procedure of the crystallization boundary
282
VI.3.2.3.
282
Calculation of the distance from phase transition in pressure-
284
VI.3.
VI.3.1.
VI.3.2.
VI.3.3.
temperature diagrams for polyethylene solutions
VI.3.4.
Pressure-temperature-composition diagrams for varying polymer
289
molecular weights
VI.4.
Conclusions
292
List of symbols
293
Greek letters
293
Superscripts
293
Subscripts
294
Abbreviations
294
References
296
Capítulo VII. Conclusões e sugestões para trabalhos futuros
VII.1.
Comentários finais
302
VII.2.
Sugestões para trabalhos futuros
305
Lista de símbolos e abreviaturas
307
308
Apêndice A. Avaliação da estabilidade de fase pelo método de Michelsen
A.1
Introdução
311
A.2
Cálculos de estabilidade para hidrocarbonetos simples com a
312
equação SRK e parâmetros de interação binária nulos
ix
A.3
Preliminares
Cálculos de estabilidade para hidrocarbonetos simples com as
315
equações SRK e PC-SAFT e parâmetros de interação binária
estimados
A.4
Cálculos de estabilidade para sistemas poliméricos com a equação 325
PC-SAFT e parâmetros de interação binária estimados
A.5
Conclusões
326
327
Apêndice B. Solventes com baixa temperatura crítica: procedimentos de cálculo da
curva UCST em sistemas binários
B.1.
Introduction
330
B.2.
330
B.3.
Conclusions
340
List of symbols
341
Subscripts
341
Abbreviations
341
References
342
x
Preliminares
Lista de figuras
Figura II.1.
Fluxograma do processo de produção de polietileno a alta pressão
15
(HPPE). Planta de PEBD (Folie e Radosz [2]).
Figura II.2.
Fluxograma esquemático da planta PELBD. Polimerização em
19
solução. a) Bomba de alimentação do reator; b) Reator; c) Préaquecedor; d) Adsorverdor do catalisador; e) Separador de pressão
intermediária (IPS, Intermediate Pressure Separator); f) Separador
de baixa pressão (LPS, Low Pressure Separator); g) Silo; h)
Trocador de calor (resfriador); i) Unidade de purificação de
monômero [4].
Figura II.3.
Diagrama de fases [6].
Figure III.1.
Prediction of infinite dilution activity coefficients versus
22
121
experimental values for model M1.
Figure III.2.
121
Figure III.3.
122
Figure III.4.
122
Figure III.5.
123
Figure III.6.
123
Figure III.7.
124
Figure III.8.
124
Figure III.9.
125
Figure III.10. Carbon number distribution error for HDPE polymer.
136
Figure IV.1.
Simplified flowsheet of a LDPE plant.
151
Figure IV.2.
Simplified flowsheet of a LLDPE plant.
152
xi
Figure IV.3.
Preliminares
Regression of LCVM parameter λ with LDPE resin molecular
168
weight (β = Mw.10-5) for LPS.
Figure IV.4.
Sanchez-Lacombe parameters SL1ij and SL2ij as a function of LDPE 169
resin weight average molecular weight (Mw) and the mass ratio of
polyethylene to ethylene (%Pol/%Et) for HPS, where
α = log[Mw ⋅ (% Pol % Et )] .
Figure IV.5.
Modeling the LDPE-5: (a-top) and (b-bottom) using the normal
171
simulation (all 8 resins used in correlation estimation); (c-top) and
(d-bottom) using 6 resins in the estimation of the new correlation.
Figure IV.6.
Modeling the LDPE-6: (a-top) and (b-bottom) using the normal
172
simulation (all 8 resins used in correlation estimation); (c-top) and
(d-bottom) using 6 resins in the estimation of the new correlation.
Figure IV.7.
Wong-Sandler parameter WSij as a function of LDPE resin weight
176
average molecular weight (Mw) and the mass ratio of polyethylene
to ethylene (%Pol/%Et) for HPS, where
α = log[Mw ⋅ (% Pol % Et )] .
Figure IV.8.
LCVM parameter λ as a function of LDPE resin weight average
177
molecular weight (Mw) and the mass ratio of polyethylene to
ethylene (%Pol/%Et) for HPS, where α = log[Mw ⋅ (% Pol % Et )] .
Figure IV.9.
LPS overhead composition for LDPE resin: Experimental and
182
predicted data by SL EOS.
Figure IV.10. LPS overhead composition for LDPE resin: Experimental and
183
predicted data by SRK-LCVM EOS.
184
predicted data by SRK-WS EOS.
185
predicted data by SRK-VDW EOS.
Figure IV.13. HPS overhead compositions for LDPE resin: Experimental and
187
Figure IV.14. HPS bottom compositions for LDPE resin: Experimental and
188
Figure IV.15. HPS bottom composition for LDPE resin: Experimental and
190
predicted data by SRK-LCVM EOS.
xii
Preliminares
191
Figure IV.17. IPS overhead compositions for LLDPE resin: Experimental and
192
Figure IV.18. IPS bottom compositions for LLDPE resin: Experimental and
193
Figure IV.19. IPS overhead compositions for LLDPE resin: Experimental and
194
Figure IV.20. IPS bottom compositions for LLDPE resin: Experimental and
194
195
predicted data by SRK-LCVM EOS with parameter λ estimated
from low and high pressure plant data.
196
predicted data by SRK-WS EOS with parameter WSij estimated
from low and high pressure plant data.
197
predicted data by SL EOS with parameters estimated from low and
high pressure plant data.
Figure V.1.
Solid-fluid phase transitions of the polyethylene + pentane system:
235
Mw=121000, wt=5 (system 44).
Figure V.2.
Solid-fluid phase transitions of the polyethylene + ethylene system: 236
(a) Mw=7000, wt=2 (system 45); (b) Mw=23625, wt=2 (system 46).
Figure V.3.
Solid-fluid phase transitions of the polyethylene + ethane system:
237
(a) Mw=7000, wt=2 and 20 (systems 21 and 22); (b) Mw=23625,
wt=2 and 20 (systems 23 and 24); (c) Mw=52000, wt=20 (system
25).
Figure V.4.
Solid-fluid phase transitions of the polyethylene + propane system:
239
(a) Mw=7000, wt=2 and 2.7 (systems 26 and 27); (b) Mw=7000,
wt=7.4 and 17.5 (systems 28 and 29); (c) Mw=13600, wt=0.25 and
2 (systems 30 and 31); (d) Mw=13600, wt=5 and 10 (systems 32
and 33); (e) Mw=23625, wt=2 and 6.9 (systems 34 and 35); (f)
Mw=23625, wt=17 (system 36).
xiii
Figure V.5.
Preliminares
240
(a) Mw=42900, wt=0.06 and 3 (systems 37 and 38); (b) Mw=52000,
wt=2, 7.3 and 17 (systems 39, 40 and 41); (c) Mw=59300, wt=2
(system 42); (d) Mw=119600, wt=7.5 (system 43).
Figure V.6.
241
(a) Zoom on Figure V.4c; (b) Zoom on Figure V.4d; (c) Zoom on
Figure V.5a; (d) Zoom on Figure V.5d.
Figure V.7.
Solid-fluid phase transitions of polyethylene + propane systems not 242
used in parameter estimation: (a) Mw=23625, wt=1.9 (system 47);
(b) Mw=42900, wt=1 (system 48); (c) Mw=52000, wt=1.9 (system
49); (d) Mw=119600, wt=0.25 and 3.5 (systems 50 and 51).
Figure VI.1.
Schematic pressure-temperature diagram for an amorphous and
263
monodisperse polymer-hydrocarbon solvent binary system [25]: (A)
Complete diagram; (B) Details of LCST and UCST curves for a
polymer solution.
Figure VI.2.
Estimated P-T diagram for the system ethylene/polyethylene [27].
265
Figure VI.3.
Estimated P-T diagram for the system n-hexane/polyethylene [27].
265
Figure VI.4.
Polyethylene-solvent phase diagram [28].
267
Figure VI.5.
Process operating conditions relative to polymer/solvent phase
268
diagram [11].
Figure VI.6.
Phase diagrams for LLDPE (Mw=15500 g/mol) + n-hexane.
275
Figure VI.7.
276
Figure VI.8.
277
Figure VI.9.
278
Figure VI.10. Phase diagrams for LLDPE (Mw=124000 g/mol) + n-hexane.
279
Figure VI.11. Phase diagrams for LLDPE (Mw=177000 g/mol) + n-hexane: (a) to 280
(d); and for LLDPE (Mw=382800 g/mol) + n-hexane: (e) and (f).
Figure VI.12. Phase diagrams for LLDPE (Mw=52000 g/mol) + n-hexane+
284
ethylene.
Figure VI.13. Algorithm to calculate the distance from phase transition in P-T
288
diagrams for polyethylene solutions and to locate this point with
respect to the different region types.
xiv
Preliminares
Figure VI.14. Algorithm to calculate the distance from phase transition in P-T
289
diagrams for polyethylene solutions and to locate this point with
respect to the different region types: simplified version using Tf
instead of Tm.
Figure VI.15. 3D plot (temperature-polymer fraction-pressure) for LLDPE
290
(Mw=15500 g/mol) + n-hexane.
291
291
Figure B.1.
Phase diagrams for LLDPE + ethylene (a) Mw=21000 g/mol, (b)
333
Mw=42000 g/mol.
Figure B.2.
Phase diagrams for LLDPE (Mw=52000 g/mol) + ethylene.
334
Figure B.3.
Phase diagram for LLDPE + ethylene (Mw=53000 g/mol).
335
Figure B.4.
336
Figure B.5.
337
Figure B.6.
338
xv
Preliminares
Lista de tabelas
Tabela II.1.
Constantes para as integrais – equação de estado PC-SAFT
78
Table III.1.
Models: identification and application
107
Table III.2.
Number of systems and data points contained in the database used
113
for finite concentration calculations
Table III.3.
Mean percentage deviation between experimental and predicted
115
solvent activities at finite concentration
Table III.4.
Summary of prediction results of finite activity coefficients by
118
different models for polymer-solvent systems
Table III.5.
Database used for infinite dilution calculations
120
Table III.6.
Summary of results of infinite dilution activity coefficients
126
calculated by different models for polymer-solvent systems
Table III.7.
Database used for liquid-liquid equilibrium calculations
128
Table III.8.
Comparison between calculated and experimental LLE data
130
Table III.9.
Comparison between M4 and M5 models according to the polymer 133
Table III.10.
Comparison between M3 and M2 models according to polymer
133
Table III.11.
Comparison between M7 and M9 models according to polymer
134
Table III.12.
Comparison between calculated and experimental LLE data for M9 135
model – extra database
Table IV.1.
Identification of the models and their parameters
160
Table IV.2.
LDPE molecular weight and separators operational conditions
162
Table IV.3.
LPDE feed range composition in the HPS and LPS separators
162
Table IV.4.
LLDPE resins and IPS operational conditions
164
Table IV.5.
LLDPE feed range composition in the IPS separator
165
Table IV.6.
Pure component or segment parameters used in Sanchez–Lacombe
165
EOS
Table IV.7.
Binary interaction parameters of EOS used for LPS simulation
167
(LDPE resin with any solvent)
Table IV.8.
Binary interaction parameters of EOS used for HPS simulation
168
(LDPE resin)
Table IV.9.
Polymer polydispersity caracterization
174
xvi
Table IV.10.
Preliminares
Comparison between monodisperse and polydisperse results using
175
Sanchez-Lacombe EOS
Table IV.11.
Binary interaction parameters of EOS used for IPS simulation
180
(LLDPE resin)
Table V.1.
Data points contained in the database used for solid-liquid 219
calculations at atmospheric pressure: non-associated systems
Table V.2.
calculations at atmospheric pressure: associated systems
Table V.3.
calculations at high pressure
Table V.4.
Data points contained in the database used to test the correlations 222
for solid-liquid calculations at high pressure
Table V.5.
Average and maximum percentile temperature errors for non- 226
associated systems in solid-liquid equilibrium at atmospheric
pressure
Table V.6.
Average and maximum percentile temperature errors for associated 227
systems in solid-liquid equilibrium at atmospheric pressure
Table V.7.
Parameter correlation with temperature for non-associated systems 228
in solid-liquid equilibrium at atmospheric pressure
Table V.8.
Average and maximum percentile temperature errors and averaged 230
parameters for solid-liquid equilibrium at high pressure
Table V.9.
PC-SAFT parameter correlation at high pressure
231
Table V.10.
SRK+LCVM parameter correlation at high pressure
232
Table V.11.
Average percentile temperature error obtained with correlated 234
parameters for solid-liquid equilibrium at high pressure
Table V.12.
Polyethylene + propane temperature calculation with correlated 243
parameters
Table V.13.
Polyethylene + propane temperature calculation with SRK+WS 252
model without correlating adjusted parameters with molecular
weight and polymer concentration
Table VI.1.
Experimental cloud point data for a polyethylene and n-hexane 273
system (some of these data are used for parameter estimation and
others are used only for correlation validation)
xvii
Table VI.2.
Preliminares
Experimental data used to generate the cloud point (LCST), LV and 281
LLV for polyethylene, hexane and ethylene system
Tabela A.1.
Dados experimentais utilizados na avaliação do método de 313
Michelsen
Tabela A.2.
Resultados da aplicação do método de estabilidade de Michelsen 317
para sistemas simples (equações de estado: SRK e PC-SAFT)
Tabela A.3.
Resultados da aplicação do método de estabilidade de Michelsen 321
para sistemas simples (equação de estado SRK)
Table B.1.
Experimental cloud point data for polyethylene and ethylene system 330
(some of these data are used for parameter estimation and others are
only used for correlation validation)
Table B.2.
PC-SAFT parameter coefficient for polyethylene and ethylene 332
systems
xviii
Preliminares
Resumo da Tese apresentada ao PEI/UFBA como parte dos requisitos necessários para a
obtenção do grau de Doutor em Ciências (D.Sc.)
Estabilidade de Fases em Processos Industriais de
Polimerização de Eteno a Alta Pressão
Setembro/2009
Orientadores: Marcelo Embiruçu
Silvio Alexandre Beisl Vieira de Melo
Fernando Luiz Pellegrini Pessoa
Programa: Engenharia Industrial
Embora os polímeros possuam uma larga faixa de aplicações, a modelagem do
equilíbrio de fases de sistemas poliméricos permanece ainda uma tarefa desafiadora. A
previsão precisa do equilíbrio de fases de misturas poliméricas necessita de modelos
termodinâmicos que sejam capazes de lidar com grandes diferenças de tamanho entre as
moléculas e de levar em conta grandes desvios do comportamento ideal em largas faixas
de condições de operação. A habilidade em modelar e prever equilíbrios de fase em
sistemas poliméricos é importante em todas as fases da produção e do processamento
dos polímeros, e é essencial para controlar as propriedades finais e de processamento
deste material. O sucesso da simulação das fases em equilíbrio depende da predição
correta do número e das composições das fases presentes a uma dada temperatura,
pressão e composição global.
O principal objetivo desta tese é descrever o equilíbrio de fases entre o
polietileno e o solvente em cada uma das etapas de processamento de processos de
produção de polietileno a alta pressão. O estudo inclui também descrever as fronteiras
que envolvem várias regiões distintas nas quais existem diferentes combinações de fases
sólida, líquida e gás em condições de equilíbrio. Para assegurar condições operacionais
em uma determinada fase (descrita por uma temperatura e pressão específicas) e
monitorar a faixa destas variáveis para manter estas condições, foi desenvolvida uma
estratégia para calcular a distância entre um ponto operacional (pressão e temperatura) e
xix
Preliminares
o ponto correspondente na interface, fixados o peso molecular do polímero e a fração
em peso. Os comportamentos de equilíbrio líquido-vapor, líquido-líquido e sólidolíquido são investigados exaustivamente, através de dados experimentais da literatura e
de uma aplicação industrial de interesse, e avaliados com quatro modelos diferentes,
baseados nas equações de estado Sanchez-Lacombe e PC-SAFT e na equação cúbica de
Soave-Redlich-Kwong. Esta última equação é testada com duas regras de mistura
diferentes, LCVM e Wong-Sandler, incorporadas com o modelo Bogdanic e Vidal de
coeficiente de atividade. Uma estratégia para construir a curva de temperatura de
separação (LCST) de sistemas poliméricos usando a equação PC-SAFT é desenvolvida
para descrever o equilíbrio de fases, e uma estratégia global é descrita para construir
todas as interfaces entre as fases para sistemas poliméricos multicomponente. É também
desenvolvida uma estratégia para calcular a distância entre um ponto operacional dado
(especificado através de uma pressão e de uma temperatura) e o ponto correspondente
na interface, para um peso molecular e uma fração em peso do polímero fixados.
xx
Preliminares
Abstract of Thesis presented to PEI/EP/UFBA as a partial fulfillment of the
requirements for the degree of Doctor of Science (D.Sc.)
Phase Stability in High Pressure Ethylene Polymerization
Industrial Processes
September/2009
Advisors:
Marcelo Embiruçu
Silvio Alexandre Beisl Vieira de Melo
Fernando Luiz Pellegrini Pessoa
Programme:
Industrial Engineering
Although polymers are found in a wide range of applications, modelling phase
equilibria of polymer systems remains a challenging task. Accurate predictions of phase
equilibria of polymer mixtures require thermodynamic models that are able to deal with
large size differences between molecules and also to account for strong deviations from
ideal behavior over a wide range of operational conditions. The ability to model and
predict phase equilibria in polymer systems is important in all stages of polymer
manufacturing and processing and it is essential for controlling the processing and final
properties of the polymer. The success in phase equilibrium simulation depends on the
correct prediction of the number and the compositions of the actual phases present at a
given temperature, pressure and overall mixture composition.
The main objective of this thesis is to describe the polyethylene-solvent phase
equilibrium in each of the production and processing steps of high pressure polyethylene
processes. The study also includes a description of the boundaries that separate several
distinct regions where different combinations of solid, liquid and gas phases exist under
equilibrium conditions. In order to guarantee the operational conditions at a specified
phase (described by specific pressure and temperature) and to monitor the range of these
variables to maintain these operational conditions, a strategy was developed to calculate
the distance between an operational point (specified through pressure and temperature)
xxi
Preliminares
and its corresponding point in the interface, for a fixed molecular weight of the polymer
and a fixed weight fraction. Vapor-liquid, liquid-liquid and solid-liquid equilibria
behaviors are thoroughly investigated through literature, experimental data and through
an interesting industrial application, and these equilibria are evaluated with four
different models based on Sanchez-Lacombe and PC-SAFT equations of state and on
Soave-Redlich-Kwong cubic equation of state. This last equation of state is tested with
two different mixing rules, LCVM and Wong-Sandler, coupled with the Bogdanic and
Vidal activity coefficient model. A strategy is developed to build up the separation
temperature line (LCST) of polymeric systems using PC-SAFT as the equation
describing the phase equilibria, and a comprehensive strategy is described to construct
all the phase borderlines of multicomponent polymeric systems. A strategy is also
developed to calculate the distance between a given operational point (specified through
a given pressure and a given temperature) and the corresponding point in the interface
for a fixed molecular weight and a fixed polymer fraction weight.
xxii
Preliminares
Lista de Publicações
Artigos em periódicos indexados:
•
Costa, G. M. N.; Dias, T.; Cardoso, M.; Guerrieri, Y.; Pessoa, F. L. P.; Vieira
de Melo, S. A. B.; Embiruçu, M. Prediction of vapor-liquid and liquid-liquid
equilibria of polymer systems: comparison of activity coefficients models.
Fluid Phase Equilibria, v. 267, p. 140-149, 2008.
•
Costa, G. M. N.; Guerrieri, Y.; Kislansky, S.; Pessoa, F. L. P.; Vieira de
Melo, S. A. B.; Embiruçu, M. Simulation of flash separation in polyethylene
industrial processing: comparison of SRK and SL equations of state.
Industrial Eng. Chem. Research, v. 48, p. 8613-8628, 2009.
•
Costa, G. M. N.; Guerrieri, Y.; Kislansky, S.; Vieira de Melo, S. A. B.;
Embiruçu, M.; Pessoa, F. L. P. Computational aspects for optimization of
high pressure phase equilibrium for polymer industrial systems. ComputerAided Chemical Engineering, v. 27, p. 405-410, 2009.
•
Costa, G. M. N.; Kislansky, S.; Oliveira, L. C.; Pessoa, F. L. P.; Vieira de
Melo, S. A. B.; Embiruçu, M. Modeling solid-liquid equilibrium for
polyethylene and polypropylene solutions with equations of state. Fluid Phase
Equilibria, submitted.
•
Costa, G. M. N.; Kislansky, S.; Gerrieri, Y.; Pessoa, F. L. P.; Vieira de Melo,
S. A. B.; Embiruçu, M. Calculation of pressure-temperature diagrams and
distance to phase transition for polyethylene solutions. Industrial Eng. Chem.
Research, submitted.
•
Costa, G. M. N.; Kislansky, S.; Ribeiro, T. S.; Pessoa, F. L. P.; Vieira de
Melo, S. A. B.; Embiruçu, M. Evaluation of phase stability for hydrocarbon
mixtures: the influence of the equation of state in the method of Michelsen.
Journal of Industrial and Engineering Chemistry, submitted.
Artigos completos em anais de congresso:
• Costa, G. M. N.; Guerrieri, Y.; Kislansky, S.; Embirucu, M.; Vieira de Melo,
S. A. B.; Pessoa, F. L. P. Modelagem do Equilíbrio Líquido-Vapor em
Separador Industrial de Polietileno usando a Equação Sanchez-Lacombe. In:
Anais do V Congresso Nacional de Engenharia Mecânica – CONEM (em
CD-ROM), Salvador-BA, Brasil, 2008.
xxiii
•
Preliminares
Costa, G. M. N.; Kislansky, S.; Embirucu, M.; Vieira de Melo, S. A. B.;
Guerrieri, Y., Pessoa, F. L. P. Modeling High-Pressure Vapor-Liquid
Equilibrium for Polyethylene Industrial Systems. In: 9th International
Symposium on Supercritical Fluids, Arcachon, França, 2009.
•
Costa, G. M. N.; Kislansky, S.; Guerrieri, Y.; Embiruçu, M.; Pessoa, F. L. P.;
Vieira de Melo, S. A. B. High-Pressure Flash Simulation in Low-Density
Polyethylene Separators. In: 8th World Congress of Chemical Engineering,
Montreal, Canadá, 2009.
xxiv
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