Browsing by Author "Renneckar, Scott"
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- Effects of acid hydrolysis conditions on cellulose nanocrystal yield and properties: A response surface methodology studyDong, Shuping (Virginia Tech, 2014-04-24)Cellulose nanocrystals (CNCs) are frequently prepared by sulfuric acid hydrolysis of a purified cellulose starting material. CNC yields, however, are generally low, often below 20%. This study employs response surface methodology to optimize the hydrolysis conditions for maximum CNC yield. Two experimental designs were tested and compared: the central composite design (CCD) and the Box–Behnken design (BBD). The three factors for the experimental design were acid concentration, hydrolysis temperature, and hydrolysis time. The responses quantified were CNC yield, sulfate group density, ζ-potential, z-average diameter, and Peak 1 value. The CCD proved suboptimal for this purpose because of the extreme reaction conditions at some of its corners, specifically (1,1,1) and (–1,–1, –1). Both models predicted maximum CNC yields in excess of 65% at similar sulfuric acid concentrations (~59 wt %) and hydrolysis temperatures (~65 °C). With the BBD, the hydrolysis temperature for maximum yield lay slightly outside the design space. All three factors were statistically significant for CNC yield with the CCD, whereas with the BBD, the hydrolysis time in the range 60–150 min was statistically insignificant. With both designs, the sulfate group density was a linear function of the acid concentration and hydrolysis temperature and maximal at the highest acid concentration and hydrolysis temperature of the design space. Both designs showed the hydrolysis time to be statistically insignificant for the ζ-potential of CNCs and yielded potentially data-overfitting regression models. With the BBD, the acid concentration significantly affected both the z-average diameter and Peak 1 value of CNCs. However, whereas the z-average diameter was more strongly affected by the hydrolysis temperature than the hydrolysis time, the Peak 1 value was more strongly affected by the hydrolysis time. The CCD did not yield a valid regression model for the Peak 1 data and a potentially data-overfitting model for the z-average diameter data. A future optimization study should use the BBD but slightly higher hydrolysis temperatures and shorter hydrolysis times than used with the BBD in this study (45–65 °C and 60–150 min, respectively).
- Environmental science and engineering applications of nanocellulose-based nanocompositesWei, Haoran; Rodriguez, Katia; Renneckar, Scott; Vikesland, Peter J. (The Royal Society of Chemistry, 2014-06-26)Compared with cellulose, the primary component of the paper we use every day, nanocellulose has a much smaller diameter (typically <10 nm) that renders it many unique properties. Amongst many others, these properties include high mechanical strength, large surface area and low visual light scattering. Nanocellulose can be obtained by disintegration of plant cellulose pulp or by the action of specific types of bacteria. Once produced, nanocellulose can be used to make transparent films, fibers, hydrogels, or aerogels that exhibit extraordinary mechanical, thermal, and optical properties. Each of these substrates is a suitable template or carrier for inorganic nanoparticles (NPs), thus enabling production of nanocomposites that possess properties of the two constituents. In this review, we focus on the preparation of nanocellulose, nanocellulose films, and nanocellulose papers, and introduce nanocellulose-based nanocomposites and their environmental applications.
- New insights into enzymatic hydrolysis of heterogeneous cellulose by using carbohydrate-binding module 3 containing GFP and carbohydrate-binding module 17 containing CFPGao, Shuhong; You, Chun; Renneckar, Scott; Bao, Jie; Zhang, Yi-Heng P. (2014-02-19)Background The in-depth understanding of the enzymatic hydrolysis of cellulose with heterogeneous morphology (that is, crystalline versus amorphous) may help develop better cellulase cocktail mixtures and biomass pretreatment, wherein cost-effective release of soluble sugars from solid cellulosic materials remains the largest obstacle to the economic viability of second generation biorefineries. Results In addition to the previously developed non-hydrolytic fusion protein, GC3, containing a green fluorescent protein (GFP) and a family 3 carbohydrate-binding module (CBM3) that can bind both surfaces of amorphous and crystalline celluloses, we developed a new protein probe, CC17, which contained a mono-cherry fluorescent protein (CFP) and a family 17 carbohydrate-binding module (CBM17) that can bind only amorphous cellulose surfaces. Via these two probes, the surface accessibilities of amorphous and crystalline celluloses were determined quantitatively. Our results for the enzymatic hydrolysis of microcrystalline cellulose (Avicel) suggested that: 1) easily accessible amorphous cellulose on the surface of Avicel is preferentially hydrolyzed at the very early period of hydrolysis (that is, several minutes with a cellulose conversion of 2.8%); 2) further hydrolysis of Avicel is a typical layer-by-layer mechanism, that is, amorphous and crystalline cellulose regions were hydrolyzed simultaneously; and 3) most amorphous cellulose within the interior of the Avicel particles cannot be accessed by cellulase. Conclusions The crystallinity index (CrI), reflecting a mass-average (three-dimensional) cellulose characteristic, did not represent the key substrate surface (two-dimensional) characteristic related to enzymatic hydrolysis.
- Preparation and evaluation of nanocellulose-gold nanoparticle nanocomposites for SERS applicationsWei, Haoran; Rodriguez, Katia; Renneckar, Scott; Leng, Weinan; Vikesland, Peter J. (The Royal Society of Chemistry, 2015-06-09)Nanocellulose is of research interest due to its extraordinary optical, thermal, and mechanical properties. The incorporation of guest nanoparticles into nanocellulose substrates enables production of novel nanocomposites with a broad range of applications. In this study, gold nanoparticle/bacterial cellulose (AuNP/BC) nanocomposites were prepared and evaluated for their applicability as surface-enhanced Raman scattering (SERS) substrates. The nanocomposites were prepared by citrate mediated in situ reduction of Au3+ in the presence of a BC hydrogel at 303 K. Both the size and morphology of the AuNPs were functions of the HAuCl4 and citrate concentrations. At high HAuCl4 concentrations, Au nanoplates form within the nanocomposites and are responsible for high SERS enhancements. At lower HAuCl4 concentrations, uniform nanospheres form and the SERS enhancement is dependent on the nanosphere size. The time-resolved increase in the SERS signal was probed as a function of drying time with SERS ‘hot-spots’ primarily forming in the final minutes of nanocomposite drying. The application of the AuNP/BC nanocomposites for detection of the SERS active dyes MGITC and R6G as well as the environmental contaminant atrazine is illustrated as is its use under low and high pH conditions. The results indicate the broad applicability of this nanocomposite for analyte detection.