Emerging Research and Opportunities in Chemicals and Fuels

Andreas S. BommariusGeorgia Institute of Technology

ChBERenewable Bioproducts: Advances

in Lignocellulosic Processes and ProductsAtlanta, GA; Oct. 1-2, 2014

Engineered Biosystems Building (EBB, May 2015):Chemical Biology, Systems Biology, Developmental Biology

Non-Ideal Biocatalyst

Reaction Constraints

Compromised Process

Conventional Development

Reaction Constraints

Create the Ideal Biocatalyst

“Ideal” Process

Ideal Development

Paradigm shift in biotechnology process development

S.G. Burton, D.A. Cowan, and J.M. Woodley, "The Search for the Ideal Biocatalyst", Nature Biotechnol. 2002, 20, 37-45

Biocatalysis: Basics

Biocatalysis at commercial scale: myths and realities

1. Enzymes are too expensive < 10 c/lb2. Enzymes are too unstable t1/2 > 30 d3. Productivities of biocatalytic processes are too low4. Redox cofactors cannot be recycled cost-effectively5. Enzymes do not catalyze industrially interesting

reactions

Actual performance: 1 kg/(L·d), TTN > 100 000 > 107 cycles of cofactor

reference: Dave Rozzell, Chimica Oggi 1999 (6/7), 42-47

PerspectivePathway to developing a biocatalyst useful in synthesis has evolved

A.S. Bommarius, J.K. Blum, and M.J. Abrahamson, Curr. Opin. Chem. Biol. 2011, 15, 194-200

2,5-FDCA (2,5-furandicarboxylic acid): building block for biopolymers

2,5-FDCA is a building block for polyethylene furoate (PEF) or polypropylene furoate (PPF) polyesters from renewables

PET Plastic• Petroleum-based• Food packaging (e.g., soda

and water bottles)• Textiles (e.g., polyester)• 19.1 Megatons by 2017

Smithers Pira organization. 2012.

PEF Plastic• Bio-based

• From Hydroxymethylfurfural(HMF)

• Avantium (YXY), Bird Engineering (Netherlands)

• Material properties superior to those of PET

Poly(ethylene terephthalate) vs. poly(ethylene furoate)

O

OO

O

n

OO

OO

O

n

Burgess, et al. Macromolecules 2014. dx.doi.org/10.1021/ma5000199

Bio Process for Soronatm: an example of both Metabolic Engineering and Biocatalysis

OOH

OHHOHO

OH

HO OH

HO OHOH

HO OPO3=O

O

O O

O

n 3G

3GT

HO OPO3=OH

HO OGene 3

Gene 4

Gene 1

Gene 2Glucose

“T”

Biological route to indigo: dioxygenation of indol-type compounds

Chemical synthesis of indigo:

- practiced since 1907

- environmentally unfriendly (KOH melt)

- atom-uneconomical

Biological route to indigo: dioxygenation of indol-type compounds

Chotani, G., Biochimica et Biophysica Acta 1543 (2000) 434-455

Improvement required: pretreatment

B.E. Dale & R.G. Ong, Biotech. Progr. 2012, 28, 893-98

MI Pretreatment on Lignocelluloses

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Solid loading (g/L)

SBL SEWSSEB SELP

MI Ctrl

Temp: 25°CTime: 5 min

MI: 100%

Mechanical mixture of Avicel and lignin (1:1 w/w)

• MI – efficient delignifier• Extract lignin without dissolving, degrading or altering cellulose crystal structure Bagasse (SEB) and Wheat straw (SEWS) provided by Dr. G. Zacchi

1-methylimidazole m.p. b.p.

MI - 6oC 198oC

Project 2: capturing CO2 from air: novel route to 2,5-FDCA (2,5-furandicarboxylic acid)

- collaborative NSF project with Matthew Realff, Chris Jones, David Sholl, and Krista Walton (all ChBE)

Development of a (de)carboxylase for the carboxylation reaction to 2,5-furandicarboxylic acid, a DOE platform chemical

Summary and Perspective

• Process opportunities exist for cellulose, hemicellulose, and lignin

• To succeed, products from renewables have to feature superior properties w.r.t. products from non-renewables, not just feature “Greenness”

• Request: set the goal to RBI (i.e. the faculty) to develop process routes (incl. catalysts, solvents) – from defined raw materials to defined products, or– to products with defined properties.