Source: TDA RESEARCH, INC. submitted to NRP
A REGENERABLE SORBENT FOR DEEP DESULFURIZATION OF ALPHA PINENE
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
1000153
Grant No.
2013-33610-20945
Cumulative Award Amt.
$100,000.00
Proposal No.
2013-00224
Multistate No.
(N/A)
Project Start Date
Aug 15, 2013
Project End Date
Apr 14, 2014
Grant Year
2013
Program Code
[8.1]- Forests & Related Resources
Recipient Organization
TDA RESEARCH, INC.
12345 WEST 52ND AVENUE
WHEAT RIDGE,CO 80033
Performing Department
(N/A)
Non Technical Summary
The production of turpentine in the U.S. exceeded 301,000 tons in 2004 (Romney 2004) and the production of resin acids exceeded 800,000 ton in 2003 (Romney 2004), which also includes the production from directly tapping trees (e.g., gum turpentine, gum rosin). There is growing demand for bio-plastics (non-petroleum derived polymers); for example Pepsi announced it will be using bio-plastic bottles in all their products by 2018. Coca Cola is expected to follow suit, which will generate commercial interest for inexpensive bio-materials that can provide an alternative to bio-ethanol (expensive for a raw material). TDA believes that this is an emerging market with substantial growth potential. Worldwide production of pinenes is 0.33 million tons per year (FAO, 2011); 70% of this comes from CST produced as chemical pulping by-product. A major consequence of the pulping process is that sulfur compounds are introduced into the CST, which substantially degrades the quality of the pinenes. Sulfur compounds not only reduces the potency of the pinene flavor (as they usually smell bad), but also, they poison the noble metal and metal oxide catalysts used to in the fine chemical synthesis process (such as the Pt-based catalysts used in alpha pinene to beta pinene isomerization). Sulfur remaining in the fine chemicals are also undesirable. For example, sulfur imparts foul odors to the bio-plastics. Therefore, these terpene fractions must be desulfurized to increase value of the bio-products and the specialty chemicals that are made from them. The proposed outcome of this project is a sulfur sorbent capable of removing sulfur compounds from alpha pinene and other derivatives of turpentine (terpenes etc.). These pure fractions will generate increased market value for a range of applications, and their purity will make them suitable feedstocks for catalytic conversion to specialty chemicals
Animal Health Component
30%
Research Effort Categories
Basic
10%
Applied
30%
Developmental
60%
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
51106602000100%
Goals / Objectives
Turpentine is a by-product of the Kraft wood pulping process, and its derivatives (e.g., terpenes such as alpha pinene) are used as fragrances in a number of commercial products ranging from cosmetics to detergents. They can also be, and are, catalytically transformed into valuable chemicals by hydrogenation, oxidation and isomerization reactions. However, turpentine and its derivatives contain small but significant quantities of sulfur, which degrades the potency of pinenes used as fragrances. Sulfur is also a highly potent catalyst poison for the precious metal and metal oxide catalysts used in the conversion processes. TDA Research Inc. proposes to develop a new, high capacity, regenerable sorbent to remove sulfur species from alpha pinene and potentially from other terpene derivatives. The sorbent will be capable of reducing the sulfur concentration of the pinene to sub ppm levels to improve product quality and to be able to meet the cleanliness requirements of downstream catalytic conversion processes that convert alpha pinene into value added chemicals.
Project Methods
Conventional desulfurization techniques such as fractionation, absorption, hypochlorite treatment, and treatment with metals and activated carbons have not been very effective at desulfurizing CST and pinenes. Fractionation and absorption leaves a significant amount of sulfur in the pinene. Hypochlorite treatment (US Patent 3778486, US Patent 3660512 and US Patent 3778485) introduces chlorinated hydrocarbons that must in turn be removed by distillation and purification, greatly increasing the costs. The use of hydro-desulfurization catalysts (such as Co-MoS2) has been investigated, but these resulted in unselective hydrogenation of the pinene fractions, changing composition and degrading it (EP 243238 and EP 267833). Activated carbon-based physical adsorption processes do a good job of removing the sulfur and preserving product's integrity (US 3778486, FR 2243246), however, the sorbent replacement cost associated with one-time use activated carbon beds makes the process cost prohibitive. Therefore, more efficient low-cost sulfur removal methods which do not change in the composition of the turpentine still need to be developed. TDA Research proposes to develop a low-cost, high-capacity regenerable sorbent that can remove all the organic sulfur species from alpha pinene and other terpenes. Our sorbent uses a highly dispersed metal phase that removes sulfur compounds via chemical complexation. The active adsorptive phase will be highly dispersed on a mesoporous support that has large pores to allow the large organic sulfur compounds, (such as the dimethyl disulfide, propyl disulfide along with various mercaptans and alkyl thiophenes) to access the pores and adsorb over the metal sites. The proposed sorbent will be distinctly different in composition and in performance (based on the preliminary test results) than commercially available materials. We will use a state-of-the-art, fully-automated sorbent testing apparatus to assess sorbent performance. We will extract samples from the treated and untreated terpene fractions to assess the clean-up capability of the sorbent.

Progress 08/15/13 to 04/14/14

Outputs
Target Audience: Nothing Reported Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided? Nothing Reported How have the results been disseminated to communities of interest? We worked with two potential partners, both of whom are among the world's largest users of terpene chemicals. These companies would be users of our sorbent that removes sulfur species from the crude sulfate turpentine (CST) and alpha pinene fractions produced during Kraft pulping. Both these companies process the terpene fractions to produce fragrances, and one of them provided two batches of alpha-pinene feedstock that we used for our experiments during Phase I. Thus, we are actively working with the ultimate customers of our sorbent product. What do you plan to do during the next reporting period to accomplish the goals? Nothing Reported

Impacts
What was accomplished under these goals? Most of our Phase I efforts are revolved around the objective of developing a sorbent that had a high capacity for the large sulfur bearing molecules that contaminate the crude sulfate turpentine (CST) and alpha pinene fractions produced during Kraft pulping. To be commercially useful the new sorbent must: 1) have a good capacity for the sulfur contaminants, 2) remove virtually all of the contaminants (initially at 100 to 1000 ppm concentrations) to the high ppb range, be regenerable so that it can be reused many times, and 4) not oxidize the alpha-pinene. We prepared and screened more than 30 different sorbent formulations, first in batch (static) experiments that contained alpha-pinene and known concentrations of sulfur and hydrocarbons and then in flow reactor tests. We found three formulations consisting of metal and mixed metal oxides dispersed on high silica zeolites and mesoporous carbons that worked particularly well, removing virtually all the sulfur in the alpha-pinene fraction provided to us by one of our industrial partners from 100 ppm down to less than 0.1 ppmw (the detection limit of our analysis system, a gas chromatograph with a flame photometric detector, GC-FPD). Two of these sorbent formulations were evaluated in multi-cycle flow breakthrough tests, and one of them showed stable performance through multiple regenerations. We also optimized the adsorption and regeneration conditions during these adsorption/regeneration cycles to minimize (and almost eliminate) the side reactions; the conversion of the alpha-pinene into other isomers was less than 1%. Our best sorbent exhibited one of the highest sulfur adsorption capacity reported to date, removing 1.1 mg sulfur per gram of sorbent on a pre-breakthrough basis.

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