Simulation of Biomethanol Production from Green Syngas Through

Sustainable Process Design

Omar Y. Abdelaziz

, Mamdouh A. Gadalla

and Fatma H. Ashour

Department of Chemical Engineering, Cairo University, Giza 12613, Egypt

Department of Chemical Engineering, the British University, Cairo11837, Egypt

Keywords: Biomethanol, Process Simulation, Process Design, Rice Straw, Biorefinery.

Abstract: Methanol is considered an alternative energy source due to its various applicability and high octane. As a

fuel, it releases low emissions, and shows high performance and low risk of flammability. Egypt faces a

high population growth rate, which implies an increase in the agricultural production. At present, the

agriculture waste materials are burned leading to major environmental problems besides the loss of potential

resources. This work builds a design methodology for producing biomethanol fuel from green syngas. The

design methodology is based on rigorous model using the Aspen HYSYS® simulation software, and takes

into account both economics and environment. As a case study, the design methodology is applied to design

a plant that converts rice straw in Egypt into methanol. The raw materials for this process are selected from

the major regions in Egypt producing rice straw with a total capacity of 1.6 million tons per year. These

local regions are Kafr el Sheikh, Dakahlia and Sharkia governorates, located in northern part to Cairo. The

methanol produced from the process is estimated to be around 156 thousand metric tons per annum. The

process equipment capital costs are estimated to be 498 million dollars with total energy costs of 17 million

dollars per annum. On the other hand, an annual revenue of 537 million dollars is obtained. The simulation

model obtained in this study can be applied to any syngas coming from other gasification processes with

different biomass feedstock. In addition, the model provides a robust basis for further studies of process

integration leading to innovative and sustainable solutions to climatic and energy problems.

1 INTRODUCTION

Major environmental and economic problems as

global warming, climatic changes, and oil prices

fluctuating are caused by fossil fuels. These facts

drive the energy sector towards finding sustainable

and innovative solutions. Biofuels arose as an

effective alternative for the fossil fuels as a cleaner

renewable source of energy with fewer

environmental impacts. Thinking of new process

designs to reach sustainable goals is a challenge that

all industries must face.

Second generation biofuels derived from

lignocellulosic feedstocks are promising alternative

for energy that concerns environment (Damartzis

and Zabaniotou, 2011). Many innovative

technologies such as gasification and Fischer–

Tropsch synthesis created many opportunities for

thermochemical conversion of biomass into biofuels.

Gasification is considered as ancient as combustion,

although it is less developed since combustion is

dominant in its applications. Recently, the

significance of gasification has grown up to convert

biomass into gas or liquid valuable materials. The

motivating factors of gasification can be

summarized as its renewability, environmental

consciousness and sociopolitical benefits (Basu,

2010). As a result, different gasifier designs

differing in the biomass pyrolysis and tar cracking

mechanisms have been evolved. Researchers have

conducted different experimental setups and

changed various parameters via gasification on

different biomass feed stocks (Mertzis et al., 2014;

Olgun et al., 2011; Patil et al., 2011; Simone et al.,

2013; Xie et al., 2014).

It was stated by the Egyptian Central Agency for

Public Mobilization and Statistics (CAPMAS, 2012)

that the rice production in Egypt rose

31.2% in the

year 2011 reaching some 5.6 million tons, compared

with 4.3 million tons for 2010. Experts say that such

a production will generate more than 30 million tons

of waste per year. This will consequently lead to

major environmental problems as these wastes are

currently burned leading to what is called the black

677

Abdelaziz O., Gadalla M. and Ashour F..

Simulation of Biomethanol Production from Green Syngas Through Sustainable Process Design.

DOI: 10.5220/0005002906770684

In Proceedings of the 4th International Conference on Simulation and Modeling Methodologies, Technologies and Applications (SIMULTECH-2014),

pages 677-684

ISBN: 978-989-758-038-3

 2014 SCITEPRESS (Science and Technology Publications, Lda.)

cloud phenomena experienced in Egypt recently.

Finding solutions to such problem is a critical issue.

Methanol is considered as a liquid fuel that can

be used in fuel cells and as a chemical feed-stock in

addition to its use as a transportation liquid fuel

(Yang et al., 2004). Most methanol plants built all

over the world use natural gas for generation of

syngas to produce methanol. The scope of process

system engineering is increasing so as to achieve

more sustainable processes (Jegatheesan et al.,

2009). Design of plants converting biomass to

methanol is challenging; most existing design

approaches are just in the form of simulations to the

process and have not been commercialized yet. Few

researches (Abu Bakar et al., 2013; Bula et al., 2012;

Kumabe et al., 2008; Shabangu et al., 2014) have

simulated the methanol production from different

biomass feed stocks. The syngas required to produce

biomethanol could be attained from the process that

includes pre-treatment of the biomass, gasification

according to the biomass physical characteristics,

cleaning of the gas produced, and the final methanol

catalytic synthesis (Minteer, 2006). It is obvious that

tackling the environmental problems of biomass

residues is essential and requires design

methodologies and procedures.

The objective of this work is to build a design

methodology for producing methanol from biomass.

The new design methodology is rigorous simulation-

based and applicable to methanol production from

any source of biomass. Aspen Hysys simulator

(Hysys User Guide, 2004) is adopted to model the

production plant. The simulation model achieved in

the study is robust and can help for further

investigation studies, such as optimization, process

integration, dynamic control, sensitivity analysis,

scaling, etc. As a case study, the design

methodology is applied to design a plant that

produces methanol from rice straw in Egypt.

2 DESIGN AND SIMULATION

METHODOLOGY

Conventionally biomethanol is produced from the

synthesis gas that is rich in hydrogen and carbon

monoxide through a heterogeneous catalysis

mechanism. Figure 1 shows the ordinary process

flow schematic diagram for biomethanol production

from biomass gasification (Ohlstrom, 2001). In this

study some critical points are identified during the

process design: The low purity of H

in the waste

gas stream seems to be unsuitable for reuse. Thus,

purification of this H

stream can be considered.

Also, the CO

circulating in the process demands

high amount of energy. This calls for removal from

the syngas stream. Further, the presence of water

circulating in the process leads to high energy

wastage. This also calls for purification of the

syngas stream. Hence, the following structural

modifications are proposed based on the above

recommendations: installation of a separation unit to

improve the H

purity in the waste gas stream and

purification of the syngas feed stream by removing

and water components.

In this design the Aspen HYSYS Ver. 7.3

process simulator is used to model the given

process. Other process simulators can be employed

such as Aspen Plus, PRO/II, VMG, etc. The given

process is simulated on the basis of converting a

certain amount of syngas into green methanol fuel.

In this stage the feed streams are specified, and the

flow process design is described, further mass and

energy balances are performed. Finally individual

process equipments are designed. As a result of this

stage, temperatures, pressures, and flows of all

process streams and products are obtained in

addition to equipment dimensions, and heat and

cooling duties.

Process economics is considered in the

proceeding stage. Equipment capital costs, total

utilities costs, and raw material costs are estimated.

Finally the total profit is calculated. CAPCOST, a

powerful tool for evaluating full process economics

and profitability is used (Turton et al., 2009). In this

stage it is easy to assess the process feasibility.

After reaching a base case design with the

associated economics, the environmental

implications of the process is to be considered

consciousnessly. In this stage of design emissions

from the process is to be estimated also the potential

characterization of waste water is to be considered.

The aim of this stage is to reduce the local and

global CO

emissions in addition to minimizing the

release of harmful compounds from the process to

the atmosphere.

While the environment is considered in the

earlier phase, the energies of all process streams are

to be integrated with the objective of minimizing the

energy demands of all the process. Pinch Analysis

and heat integration principles are to be applied to

attain the best heat exchanger network (HEN) where

minimum amount of utility requirements are

required. An ideal solution of this phase is an

optimum heat integrated process.

Either the base case design or the environmental

based design is to be optimized by manipulating the

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678

operating and design parameters of the process to

minimize multiple objectives. These optimization

objectives may include the total costs, utility

requirements, CO

emissions or any other objective.

The sections below detail the new design

methodology.

Figure 1: Schematic for biomethanol production from

biomass.

2.1 Simulation Procedure and

Algorithm

Figure 2 summarizes the simulation algorithm for

biomethanol production from biomass. As shown in

the figure the algorithm illustrates the main phases

of simulation design. It starts by the biomass

gasification reaching the green syngas production,

and then follows to the process simulation part

through the model validation, analysis, costing and

optimization. More details will be presented in the

following sections.

Figure 2: Simulation algorithm for methanol production

from biomass.

2.2 Syngas Adjustment Stage

Methanol is one of the most important basic

chemicals that can be produced using synthesis gas

(a mixture of CO, CO

and H

). The typical

methanol process involves a reaction of syngas in

the presence of metal catalyst followed by

purification of the methanol. Here the feed is syngas

produced from biomass gasification which totally

differs from the syngas coming from the natural gas

in properties and conditions. The high percentage of

nitrogen found in the gas has to be separated first,

and then the syngas is sent to the reformer to convert

the existing methane to extra syngas. Water gas shift

reactor adjusts the reactor feed requirements by

providing the required amount of hydrogen through

the water gas shift reaction. Water and CO

are

removed, and then the make-up stream is ready to be

mixed with the recycle stream, and further fed to the

reactor. In one pass only, thermodynamic

equilibrium is reached before achieving 50%

conversion of the synthesis gas, therefore, after

methanol and water are condensed out and removed,

the remaining synthesis gas must be recycled to the

reactor. Adjustment stages are discussed in this

section.

2.2.1 Nitrogen Separation

Pressure swing adsorption (PSA) can be a cost-

effective method of onsite nitrogen generation for a

wide range of purity and flow requirements. So it is

used to separate 97.5 mole% of nitrogen that exists;

separation is assumed to be ideal in which the

separated nitrogen stream is pure nitrogen.

2.2.2 Methane Reformer

Since most biomass gasifiers produce significant

amount of methane and small amounts of other light

hydrocarbons, it is wise to use them to produce extra

amount syngas through steam reforming. The

reaction is carried out according to the following

highly endothermic reaction:



H



O↔CO3H



(1)

Acceptable conversion is achieved only at

relatively high temperatures (>800°C), conventional

steam reformers operate at temperature of up to

1000°C. Since the total number of moles of gas

increases significantly throughout the reaction,

reforming is also favored at lower pressures (1-

3.5MPa). Methane conversion in biomass systems

varies from 60-90% using Ni-based catalyst. Steam

is required not only for promoting the reaction but

START

END

timization

Process

Simulation

Biomass Feedstock

(Rice straw, Rice husk, Wood, etc.)

Gasification Model

Model

Validation

Anal

sis of Results

Costing

Yes

Air

Biomas

Distillation

Pretreatment

Steam

reformed

Gasification

Methanol S

nthesis

Removal of

, H

and H

WGSR

HRSG

PSA

Steam

Ash

SimulationofBiomethanolProductionfromGreenSyngasThroughSustainableProcessDesign

679

also to prevent carbon formation (coking), for that

steam to carbon ratio are recommended to be ≥ 3:1

which is achieved in the model.

2.2.3 Water Gas Shift Reactor

Syngas out of the reformer is then cooled before

being sent to a shift reactor that converts CO to H

via the water-gas shift reaction:

CO  H



O⇄CO



H



(2)

For methanol synthesis, the shift reactor is used

to increase H

to CO ratio which is found to be

essential in this process. Since the shift reaction is

exothermic, higher conversion levels are achieved at

lower temperatures. The reaction nearly proceeds to

completion with modern catalysts (ZnO-CuO) at

temperatures as low as 200°C. In this process, only

60% conversion is required to achieve the purpose

of having proper hydrogen amount in the make-up

gas. The water gas shift reactor (WGSR) operates at

200°C, design parameters is adjusted to reach the

required conversion. In this model no steam was

added to the shift reactor, the amount of steam in the

feed was already sufficient due to the extra steam

added in the reformer.

2.2.4 Water Removal

To reduce the water content in the syngas stream, a

condensation-separation process was proposed. At

pressure of 13 bar cooling the water to 110

C is

necessary so as to condense only the water rather

than other compounds flowing in the stream.

2.2.5 CO

Removal

The CO hydrogenation reaction is considered to be

the primary reaction in methanol formation. CO

hydrogenation reaction results in the loss of some of

the hydrogen as water that is why in ideal

circumstances there would be no CO

in the feed.

However small amount of CO

(1-2%) acts as a

promoter of the primary methanol synthesis and

helps maintain catalyst activity. As a matter of fact,

the use of membrane process for CO

removal from

syngas has been commercially available (Membrane

Technology & Research, 2010a). Using such

technology, CO

recovery with up to 80% at 95%

purity on volume basis can be obtained. In this

process 85% of the CO

found in the gas stream out

of the separator is assumed to be removed.

2.2.6 Compression

After leaving the carbon-dioxide membrane, dry

syngas enters the syngas compressor at 13 atm

where it is compressed to 50 atm, the pressure at

which the proposed low pressure Lurgi methanol

synthesis reactor operates. Inter-cooling appears

between the two compressors so as to decrease the

net power consumption.

2.2.7 Pre-reactor Heating

After the make-up stream in compressed and mixed

with the recycle stream, and before sending the

syngas to the methanol reactor, it is heated close to

the temperature in the methanol reactor (260

C).

This is necessary as temperatures lower than this

reaction temperature has the problem of low

equilibrium constants (slow reactions). Also catalyst

activity drops off sharply below 230°C (Katofsky,

1993).

2.3 Reaction Modeling

Feed syngas enters methanol reactor at temperature

of 260

C and pressure of 50 atm in the presence of

metal catalyst most common commercially is the

(Cu–ZnO–Al

O3). Two successive reactions take

place in the reactor:

CO  2H



⇌CH



OH

(3)



3H



⇌CH



OH  H



O

(4)

Since all of the above reactions are exothermic

reactions, heat removal from the reactor is a critical

issue. Water gas shift reaction may slightly occur

during the methanol synthesis which is ignored in

this design. Single pass conversion in the methanol

reactor ranges from 40 to 60 percent of CO and CO

To increase the conversion, the un-reacted gases

after methanol condensation are recycled back to the

reactor, in which up to 99.5 percent overall

conversion can be achieved (Vaswani, 2000).

Although modern methanol synthesis catalysts are

highly selective, some side reactions are possible,

such as:

2CH



OH ⇄ CH



OCH



H



O

(5)

CO  H



⇄CH



(6)

2nH



nCO⇄C





OH  n  1H



(7)

The formation of these species is limited by the

selectivity of the catalyst and the kinetics at the

reactor conditions. For simplicity, this model

considers dimethyl-ether as the only side product in

the system; the amount of dimethyl-ether produced

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680

is typically equal 2% wt of the methanol produced.

The make-up gas should be slightly hydrogen rich to

compensate the hydrogen consumed by reactions

and also that is lost in the purge stream. The quantity

of hydrogen in the make-up gas stream must satisfy

the stoichiometry of both methanol synthesis

reactions, and this could be typically determined by

the R-value which should be 2 or more:

R



CO



CO  CO



2

(8)

Due to hydrogen build up, the actual combined

R-value (make-up + recycle) reached more than 4 in

this model. Table 1 summarizes all reactors data.

2.4 Product Purification

Stream out of the reactor is cooled to 45°C. CH

OH,

DME and H

O condense out of the product gases. It

is assumed that a complete condensation of these

components takes place. Other components entering

the condenser leave as gases. Uncondensed gases

like CH

, N

, un-reacted CO, un-reacted CO

and

un-reacted H

are removed in a flash drum at the top

as a purge.

Then part of it (molar recycle ratio

approximately 4 of the makeup feed) is recycled

back to the reactor and the other part is used to

produce the pure hydrogen. The liquid fraction is

taken out at the bottom and it mainly consists of

OH, DME and H

O. A membrane process for

purification has also been widely used in the

refineries. The process has been claimed to be able

to recover up to 95% of H

at 99% purity on volume

basis (Membrane Technology & Research, 2010b).

Hence, these alternatives were implemented in the

HYSYS model of the base case process simulation.

In pre-distillation pressure relief valve, the pressure

of the outlet stream from the condenser is reduced

from 41.4 atm to 11.2 atm for the removal of

uncondensed gases and to allow the separation of the

DME tower at this operating pressure. Liquid out

from the separator post the reactor enters a relief

valve in which the pressure is reduced from 41.4 atm

to 11.2 atm for the removal of uncondensed gases

and to allow the separation of the DME tower at this

operating pressure feed to the distillation column is

at the boiling point of DME (45

C) at 11.2 atm. It is

assumed that complete recovery of DME takes place

in the top product. Water and methanol are assumed

to leave as bottoms of DME distillation column at

C. Fifteen trays, and with reflux ratio of 20 are

able to perform the distillation process. The bottom

exit from the DME distillation column consists of

OH and H

O at 11.6 bar and 157.2

C, the

pressure of this stream is first reduced to 3.4 atm

(the pressure at which methanol distillation occurs),

and then it is cooled to 45°C.The exit stream from

pre-methanol distillation column valve enters

methanol distillation column at 45

C and 3.4 atm. It

is assumed that 99.9 percent recovery of methanol in

top product takes place producing 99.9 percent pure

methanol on weight basis. Water with a trace

quantity of methanol is recovered at the bottom.

Forty-five trays, and with reflux ratio of 1.5 are able

to perform the distillation process.

The above algorithm and simulation procedure

will be applied to address a local environmental

problem in north Egypt. A case study will be

considered in the following section.

3 CASE STUDY

The raw materials for the case study are selected

from the major regions in Egypt producing rice

straw with a total capacity of 1.6 million tons per

year. These local regions are Kafr el Sheikh,

Dakahlia and Sharkia governorates, located in

northern part to Cairo (Bakker, 2011). After

gasification, the amount of volatile matter which is

mainly syngas represents about 60% of the biomass

feed (Basu, 2010), so that the synthetic gas feed to

methanol synthesis process (from gasifier) can be

calculated to be 0.96 million tons per year. In this

study 300 operational days are assumed per year.

Table 2 and Table 3 show an approximation for the

Table 1: Reactor simulation data.

Reaction Reactions equations Conversion (%) Reactor

Steam Reforming CH

O CO+3H

85 Steam Reforming

WGSR CO+H

O CO

60 WGSR

CO to Methanol CO+2H

OH 50

Methanol Reactor

to Methanol CO

+3H

OH+H

O 50

DME formation 2CO+4H

OCH

O 5

SimulationofBiomethanolProductionfromGreenSyngasThroughSustainableProcessDesign

681

syngas compositions and conditions coming from

the gasification process respectively (Patil et al.,

2011). It is assumed to use Peng-Robinson Fluid

package which is commonly used with

petrochemical compounds, but it is not

recommended by HYSYS when using dimethyl-

ether. So the SRK-Twu Fluid package is adopted in

the model instead.

Table 2: Syngas composition (Mole percent).

Component Mole %

CO 22.2

Hydrogen 10.9

Methane 4.5

CO2 11.5

Nitrogen 50.9

Table 3: Syngas conditions.

T (°C) 866

P (atm) 1

Mass Flow rate (kg/hr) 133,333

4 RESULTS AND DISCUSSION

Figure 3 shows the process flow diagram designed

in this study for methanol production from synthesis

gas generated from the biomass gasification process.

The figure shows the most important stages made on

the gasifier syngas so as to reach the desired

biomethanol product, such as the methane reforming

reactor, the water gas shift reactor and the methanol

synthesis reactor. The process is rigorously

simulated starting from the syngas adjustment stage

and reaching to the final product purification stage.

This simulation model provides a robust basis for

further studies of process integration, environmental

assessment, and optimization studies leading to

innovative solutions to the energy scarcity problems.

Moreover, it can be applied on any type of biomass

reaching to liquid methanol production as a

sustainable model of a biorefinery. Table 4 shows

the methane reformer steam conditions used in the

process necessary to convert the methane to syngas

with required R-value. The flow rate is adjusted so

as there is no need to enter steam in the WGSR.

Also, the pressure and temperature conditions are set

favoring the methane reforming reaction.

Table 4: Reformer steam conditions.

Flow rate (kgmole/hr) 5770

P (bar) 15

T (°C) 198.5

Economic analysis has been performed for this

case with the aid of CAPCOST tool. The methanol

obtained is estimated to be around 156 thousand

metric tons per year. The process equipment capital

costs are estimated to be 498 million dollars with

total utilities costs of 17 million dollars per year. On

the other hand, revenue of 537 million dollars is

obtained per year. Table 5 shows a summary of the

costs including capital and energy costs. It is

obvious that the operating costs of the process are

much lower than its raw material costs. This can

show an indication of the profitability of the process.

Table 6 shows a summary of the annual revenue

obtained from each product production.

Table 5: Summary of costs.

Total Cost of Equipment (MM$) 498

Annual Utilities Cost (MM$/Yr) 17

Cost of Raw Material (MM$) 41.5

Cost of Land (M$) 875

The annual revenue achieved from the methanol

which is the main product is estimated to be 81

million dollars. This value covers both the annual

operating and raw material costs. Also, the high

quantity of nitrogen can be useful if it is sold to

nearby plant that can use it in liquefaction purposes

as an example. Integration between hydrogen and

nitrogen products to produce ammonia (NH

) can be

useful as ammonia serves as an essential precursor

to food and fertilizers industries. Finally Figure 4

shows the cash flow diagram for this case

illustrating the tremendous increase in the project

value after around 4 years from the project life

implementation.

Table 6: Summary of revenues.

Material

Name

Price

($/kg)

Flowrate

(kg/h)

Annual

Revenue

(MM$)

Methanol 0.52 21593 81

Nitrogen 0.85 69972 428

Hydrogen 3.50 670 17

Carbon

Dioxide

0.02 50980 7.5

Dimethyl

Ether

0.68 655 3.5

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682

-1,0

0,0

1,0

2,0

3,0

4,0

5,0

6,0

012345678910111213141516171819202122232425

Project Value (millions of dollars)

Project Life (Years)

Figure 3: Biomethanol production process flow diagram.

Figure 4: Cash flow diagram (Acquired from CAPCOST).

5 CONCLUSIONS

In the present study, a design methodology was

developed for producing biomethanol out of the

green syngas coming from the biomass gasification

route. The design methodology is rigorous

simulation-based and can be applied to any source of

biomass for methanol production. The design

methodology was applied to design a plant that

produces methanol from rice straw in Egypt as a

case study. In addition, the economic analysis for the

case study was investigated. The simulation model

achieved is robust; Hence, as a recommendation

further investigation studies, such as optimization,

process integration, dynamic control, sensitivity

analysis, scaling, etc. have to be performed.

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SIMULTECH2014-4thInternationalConferenceonSimulationandModelingMethodologies,Technologiesand

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