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INTRODUCTION
The depletion of fossil feedstocks, economic and market risks
Typically, inherent trade-os exist among biocatalyst yield,
titer, and production rates. For example, lower fermentation
yields may be oset by achieving higher production rates and
to investments, and growing concern over global warming
vice versa. Determining such trade-os is necessary to guide
impacts are driving interest in the development of new
biocatalyst technology development by setting performance
technologies for the conversion of agricultural and forestry
targets to the technology development team.79 The aim of this
materials to fuels and chemicals.14 One way to convert such work is to determine the existence of generalities in the area of
biobased feedstocks to valuable products is using biocatalysts.5 biobased commodity chemical production, which can be used
Advances in the elds of synthetic biology and metabolic by technology development teams to quickly assess the
engineering have made it possible to modify microbial economic potential and environmental sustainability of early
metabolism to develop ecient industrial biocatalysts that are stage biocatalytic technologies as well as to guide the
used to make commodity chemicals and fuels from biobased development of these new technologies.
feedstocks. Signicant investment has been made by both In this work, we analyzed the economic and environmental
government and industry in research and development (R&D) performance of a range of biobased commodity chemical
of new biocatalytic technologies for the conversion of biobased production processes that were chosen to be representative of a
feedstocks to fuels and chemicals. Many of these investments wide range of such production processes to determine if general
have incurred losses and, so far, few technologies have been trends in the area of biobased commodity chemical production
commercialized.6 exist. Criteria including nature of cultivation (aerobic/
To avoid potential losses to R&D investments, it is necessary anaerobic), the type of product separation and purication
to screen early stage biocatalytic technologies before large processes, and the availability of data for the process
investments are made and to ensure the technologies developed simulations were considered while selecting the range of
are environmentally benign. Development of environmentally biobased commodity chemical production processes. Speci-
benign biocatalytic technologies is necessary to reduce GHG cally, the economic and environmental potential of processes
emissions of chemical and fuel industry. Assessing the for the biocatalytic production of succinic acid, adipic acid,
economic and environmental potential of new biocatalytic isobutanol, 1,3-propanediol, and 3-hydroxy propionic acid (3-
technologies requires expertise of process modeling, techno- HPA) were determined and used for this analysis.
economic analysis (TEA), and life cycle analysis (LCA).7 Often,
the biocatalyst development teams do not have expertise in Received: May 31, 2017
these areas and such assessments require considerable resource Revised: July 18, 2017
investment. Published: July 23, 2017
Table 1. Model Molecules for Analyzing Multiple Microbial Pathways Using the Feasible Space Approach
biobased commodity chemical resistance to pHa type of separation type of cultivation theoretical yield (g/g)b [source]
succinic acid high (23) distillation anaerobic/ 0.57 [32]
microaerobic
adipic acid low (57) distillation anaerobic 0.52 [29]
isobutanol high (79) distillation anaerobic 0.35 [33]
1,3-propanediol high (79) LLEc microaerobic 0.51 [35]
1,3-propanediol high (79) LLE aerobic 0.34 [34]
3-HPA medium (45) LLE anaerobic 0.60 [30]
3-HPA medium (45) LLE microaerobic 0.55 [31]
a
Values in the parentheses represent the desired pH during the production of biocommodity chemicals. bAll these products are growth-associated
products. Above theoretical yields are computed at the specic growth rate of 0.1 g biomass/g glucoseh. cLiquid-Liquid Extraction.
The GHG emissions (g CO2 equiv/kg), energy consumption After the cell clarication step, adsorption, distillation, or solvent
(MJ/kg), and the MSP ($/kg) of analyzed biobased extraction processes can be used to extract a product from the claried
commodity chemical production processes were found to be culture media.15 The low capacity and troublesome solids handling of
adsorption process made this process not suitable for the extraction of
nearly same for a given combination of titer, yield, and
a product from the claried culture media.19 In the third and nal step,
productivity. However, these performance metrics did vary with the product is puried using processes such as crystallization or ion-
the nature of cultivation (aerobic/anaerobic). General cost, exchange.16 Among the three separation and purication process steps,
energy, and GHG contour plots were created for the aerobic the second step dominates the total separations cost, energy
and anaerobic/micro-aerobic production of biobased commod- consumption, and GHG emissions. This is due to the fact that energy
ity chemicals, and these plots can be used to determine consumption and operating costs of a separation unit process are
economic and environmental feasibility. The results of the plots directly related to the volume of a feed from which the product is
can also serve as a guide in the development of new processes extracted.16
Processes with intracellular chemical production require two
to produce biobased commodity chemicals using biocatalysts.
B DOI: 10.1021/acssuschemeng.7b01729
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method based on delivered cost of process equipment.22 Capital costs and productivity. But, for a particular fermentation yield only a
of biocommodity chemical production plants will be dierent for 200% increase in MSP is noticed when the titer is reduced to 10
dierent titers and productivities. A combination of titer of 100 g/L from 200 g/L. The high eect of yield is mainly because the
and productivity of 2 g/Lh has been chosen to represent capital costs entire upstream of biobased commodity chemical production
of biocommodity chemical production processes. These numbers will
provide a general idea of the capital costs associated with the (including production of corn, production of glucose from corn
production of biocommodity chemicals. The total capital costs ($ using the dry grind process, and the production of a chemical
MM) associated with the production of adipic acid, succinic acid, 1,3- from glucose in a bio reactor) are aected by any variation in
propanediol (microaerobic conditions), 1,3-propanediol (aerobic the fermentation yield value.
conditions), 3-HPA (microaerobic conditions), 3-HPA (anaerobic The MSP of biobased commodity chemicals, except those
conditions), and isobutanol are 149, 151, 134, 272, 145, 139, 137, produced aerobically, is found to be nearly constant for a given
respectively. titer, yield, and productivity. For example, the calculated MSP
The material and energy balances of each chemical production of 1,3-propanediol that is produced under microaerobic
process were obtained from the process simulations. The material
fermentation is 1.13 ($/kg) for the yield of 0.6 g/g, volumetric
balance was used to calculate the required quantity of raw materials,
and the energy balance was utilized to determine steam and electricity productivity of 2 g/Lh, and the titer of 50 g/L (Figure S5). For
requirements. The raw material and utility prices, labor and the same process parameter values, the MSP of aerobically
maintenance costs, and local taxes used in this analysis are listed in produced 1,3-propanediol is estimated at 1.66 ($/kg). Such an
Table S1. The discounted cash ow analysis (DCA) method was used increase of MSP is due to the requirement of high capital and
to compute the biobased commodity chemical MSP. A discount rate of operating costs for the aerobic cultivation as compared to
10% was employed in the DCA.16 anaerobic/microaerobic fermentation. The current available
Estimation of Life Cycle Energy Use and GHG Emissions. The agitator size limits the aerobic reactor volume to 4000 kL.14
cradle-to-gate energy consumption and GHG emissions of biobased The cost advantages due to economies of scale are, therefore,
commodity chemical production processes were calculated using LCA
methodology. The LCA system boundary covers all activities from
minimized for an aerobic reactor, which increases the capital
corn production to the production of a biobased commodity chemical. cost of aerobic cultivation processes. The compressor energy
The functional unit was dened as 1 kg of biocommodity chemical requirements and the energy losses in gassing systems increase
production. The life cycle GHG emissions and energy consumption of the operating costs of aerobic cultivation processes.14
steam, electricity, and corn production processes were obtained from The addition of acid or base to maintain medium or high pH
the Ecoinvent database in SimaPro 7.2 software.23 The 2007 in the production fermentor is found to have negligible impact
Intergovernmental Panel on Climate Change (IPCC) Global Warming on the production cost of biobased commodity chemicals. For
Potentials (GWPs) method was employed to convert GHG emissions example, ammonium hydroxide is added to the fermentor
to CO2 eq emissions. The economic allocation approach was used to
during adipic acid production to maintain the pH around 5.28
partition energy consumption and GHG emissions of biobased
commodity chemical production process among the product and The addition of such base is not necessary for the succinic acid
coproduct DDGS.24 fermentation as the genetically modied yeast strain can make
We calculated MSP, energy consumption, and GHG emissions of succinic acid under low pH conditions.28 However, the
biobased commodity chemical production processes for a wide range estimated production costs of adipic and succinic acids for a
of yield, titer, and volumetric productivity values. The performance given combination of titer, yield, and productivity are nearly the
contour plot for cost was created by mapping biobased commodity same (Figure S6). It should be noted that the salts formed due
chemical MSP to the corresponding yield, titer, and volumetric to the addition of acid or base will end up in the DDGS, and it
productivity. Similarly, performance contour plots for energy and is assumed in this analysis that the presence of salts do not
GHG were created. The energy consumption and GHG emissions of
petroleum based adipic acid, succinic acid, isobutanol, 3-HPA, and 1,3-
aect the market price of DDGS. Please refer to the Supporting
propanediol production processes were obtained from the liter- Information on this paper for the sensitivity analysis if the salt is
ature.25,26 The market prices of these chemicals were obtained from assumed to be a waste stream and the impact that the
ICIS chemicals.27 The performance metrics of conventional processes additional cost of salt waste treatment will have on the MSP of
and performance contour plots were used to determine feasible curves the biocommodity chemical.
of cost, energy, and GHG. The feasible space of each biobased The downstream processing costs of biobased commodity
commodity chemical production process was dened by graphing the chemical production processes are found to be nearly the same
feasible curves of cost, energy, and GHG along with yield, titer, and for a given titer even with dierent number and type of
volumetric productivity constraints. The maximum attainable yield, separation processes. For example, distillation and solvent
titer, and production rates were used to determine yield, titer, and
volumetric productivity constraints, respectively.7 extraction processes are used to extract isobutanol and 3-HPA
Figure 1. General cost contour plots for anaerobic production of a biobased commodity chemical with a productivity of (a) 1, (b) 2, and (c) 3 g/Lh;
for aerobic production of a commodity chemical with a productivity of (d) 1, (e) 2, and (f) 3 g/Lh. The cost contour lines represent MSP ($/kg) of
biocommodity chemicals.
data of MSP of 3-HPA is used to generate cost contour plots productivity to 3 from 2 g/Lh causes only a slight decrease in
for the anaerobic/microaerobic process, and the data of MSP of the MSP of a biobased commodity chemical (Figure 1). For a
1,3-propanediol that is produced via aerobic cultivation is used given titer and yield, the biobased commodity chemical MSP is
to generate general cost contour plots for the aerobic process. reduced approximately 3.5% when the productivity is improved
Comparison of general cost contour plots of anaerobic/ to 3 from 2 g/Lh (Figure 1). A similar comparison for the
microaerobic processes indicates that improving volumetric aerobic based commodity chemical production demonstrates a
D DOI: 10.1021/acssuschemeng.7b01729
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Figure 2. General energy and GHG contour plots. (a) Energy plot for the anaerobic/microaerobic production of biobased commodity chemical (b)
and for aerobic production of biobased commodity chemical; (c) GHG plot for the anaerobic/microaerobic production of biobased commodity
chemical (d) and for aerobic production of biobased commodity chemical; energy contour lines represent total energy consumption (MJ/kg) of
biocommodity chemical production; GHG contour lines represent total GHG emissions (g CO2 equiv/kg) of biocommodity chemical production.
16% decrease in MSP (Figure 1). This is mainly due to there investments to develop a biocatalyst that synthesize glucaric
being no economy of scale advantage for aerobic processes. acid from glucose will not be protable.
A nonlinear relationship is found between the biocommodity Performance cost targets can be set to the biocatalyst
chemical MSP and the product titers. The economic benets of development team using the general contour plots of cost. For
improving fermentation titer beyond 125 g/L are found to be example, the average market price of adipic acid is 1.80
low for both aerobic and anaerobic/microaerobic biobased ($/kg.).27 For this target price, general cost contour plots in
commodity chemical production processes. For a certain Figure 1 shows various economically viable combinations of
productivity and yield, increasing titer to 200 from 125 g/L productivity, yield, and titer for making the adipic acid from
causes the biocommodity chemical MSP to drop only by 2% glucose using a biocatalyst. The yield, titer, and volumetric
(Figure 1). Thus, investments for pushing titers beyond 125 g/ productivity targets for the technology development team can
L must be avoided. be determined by selecting one viable combination. This
Use of General Cost Contour Plots of Biobased
selection can be done by comparing development time and
Commodity Chemical Production. The economic viability
costs that are required to develop a biocatalyst that exhibits
of new processes for the production of biobased commodity
chemicals using biocatalysts can be determined by utilizing each viable combination of process parameters. Such develop-
general cost contour plots. For example, glucaric acid can be ment time and costs can be qualitatively computed by the
made from sugar using E. coli under anaerobic conditions.28 management and research teams.
The theoretical yield and production rates of glucaric acid General Energy and GHG Contour Plots of Biobased
production are estimated at 0.3 g/g and 2 g/Lh, respectively, Commodity Chemical Production. The data of estimated
from stoichiometric calculations.29 The current market price of energy consumption and GHG emissions of biobased
glucaric acid is 0.80 ($/kg).27 For this market price, cost commodity chemical production processes are used to create
contour plots in Figure 1 shows that yields of greater than 0.8 contour plots of energy and GHG, respectively (Figures S8 and
g/g are necessary to make a process for the production of S9). The energy, GHG, and cost contour plots of biobased
glucaric acid that is economically viable. Since the required commodity chemical production processes have resulted in a
glucaric acid yield is greater than the theoretical yield, similar shape (Figures S5, S8, and S9). This indicates that there
E DOI: 10.1021/acssuschemeng.7b01729
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ACS Sustainable Chemistry & Engineering Research Article
Figure 3. Feasible space of processes for the production of (a) 3-HPA (anaerobic), (b) 1,3-propanediol (anaerobic), (c) adipic acid, (d) succinic
acid, (e) isobutanol, and (f) 3-HPA (microaerobic). The green curve represents the feasible cost curve, the red curve represents the feasible energy
curve, and the blue curve represents the feasible GHG curve. The purple vertical straight line indicates theoretical yields of biocommodity chemical
production.
is a correlation between economic and environmental perform- market prices are obtained from the ICIS chemicals pricing
ance metrics for the cases studied here. report.27 The cradle-to-gate energy consumption (MJ/kg) of
The comparison of GHG and energy contour plots indicates conventional adipic acid, succinic acid, isobutanol, 1,3-propane-
that the energy consumption and GHG emissions of biobased diol, and 3-HPA production processes are 124, 110, 60, 150,
commodity chemical production processes, except those made and 120, respectively.25,26 The cradle-to-gate GHG emissions
using aerobic cultivation, are found to be nearly the same for a (kg CO2 equiv/kg) of conventional adipic acid, succinic acid,
given combination of titer, yield, and productivity (Figures S8 isobutanol, 1,3-propanediol, and 3-HPA production processes
and S9). In addition, the decrease in the energy consumption are 9, 12, 3, 12, and 7, respectively.25,26 The feasible cost curves
and GHG emissions of anaerobic/microaerobic processes are are determined using both the market prices of chemicals and
found to be very low (0) when the volumetric productivity is general cost contour plots. For example, the market price of
increased from 1 to 2 g/Lh. The decrease in the energy adipic acid is 1.80 ($/kg.).27 The contour line of 1.80 in Figure
consumption (MJ/kg) and GHG emissions (kg CO2 equiv/kg) 1b represents the feasible MSP curve for adipic acid production.
of the aerobic process is around 2% and 0.2%, respectively, Similarly, feasible energy and GHG curves are determined using
when the productivity is increased from 1 to 2 g/Lh for a given general energy and GHG contour plots as well as cradle-to-gate
titer and yield (data is not shown). Like the biobased energy consumption and GHG emissions of conventional
commodity chemical MSP, the general counter plots of GHG processes, respectively.
and energy are generated for the processes of biobased The 2D-feasible space of biobased adipic acid, succinic acid,
commodity chemical production (Figure 2). Like the MSP isobutanol, 1,3-propanediol, and 3-HPA production processes
contour plots, the general GHG and energy contour plots are dened by graphing feasible cost, energy, and GHG curves
shown in Figure 2 can be used to screen early stage biobased along with yield, titer, and productivity constraints (Figure 3).
commodity chemical processes in terms of environmental The theoretical yields of biobased commodity chemicals are
performance and to set environmental performance targets for used to determine the yield constraints (Table 1). Titer of 200
new biocatalytic technology developments by governmental g/L and productivity of 2 g/Lh are assumed as titer and
policy makers. volumetric productivity constraints, respectively. We have
2D-Feasible Spaces of Biobased Commodity Chem- provided justication for the selected limits on titer and
ical Production. Conventionally, adipic acid, succinic acid, productivity in the supplement materials. The bounded space
isobutanol, 1,3-propanediol, and 3-HPA can be produced from between feasible energy or GHG curve and constraints of yield
a petroleum feedstock.25,26 The market prices ($/kg) of adipic and titer is dened as the environmental feasible space (Figure
acid, succinic acid, isobutanol solvent, 1,3-propanediol, and 3- 3). Similarly, feasible cost space is dened as a space between
HPA are 1.80, 1.80, 2.2, 1.70, and 1.60 respectively. These the feasible cost curve and constraints of yield and titer (Figure
F DOI: 10.1021/acssuschemeng.7b01729
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ACS Sustainable Chemistry & Engineering Research Article
3). For the selected constraint values, the feasible space is not Detailed PFDs, modeling assumptions, microbial pro-
found for the production of 1,3-propanediol via aerobic duction pathways, operating cost assumptions, micro-
cultivation. This is because the requirement of high capital aerobic reactor cost, DDGS price sensitivity, and
and operating costs for the aerobic cultivation process. additional information about results (PDF)
The comparison of feasible spaces of processes for the
production of biobased commodity chemicals shows that a AUTHOR INFORMATION
biocatalyst must exhibit titers of at least 45 g/L (Figure 3). If Corresponding Author
the toxicity of a biobased commodity chemical to biocatalyst *E-mail: anex@wisc.edu.
limits the concentration of a chemical in the fermentation
systems to lower than 45 g/L, the additional investments to ORCID
increase the yield and product rates of the biocatalyst will Sampath Gunukula: 0000-0001-7297-3993
become unviable (Figure 3). In such cases, the investments Notes
should be diverted to develop an alternate biocatalyst to make The authors declare no competing nancial interest.
the biobased commodity chemical. Similarly, a biocatalyst
development team must achieve biobased commodity chemical
yields of at least 0.32 g/g (Figure 3). To avoid potential losses,
ACKNOWLEDGMENTS
This work was supported by the National Science Foundation
R&D investments to develop biocatalysts should be avoided [grant no. EEC-0813570/1158833].
when theoretical yields of biobased commodity chemicals are
less than 0.32 g/g. These values of yield and titer can be used as
general guidelines in the development of biocatalytic
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H DOI: 10.1021/acssuschemeng.7b01729
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