Humphries A C, Mikheenko I P, Macaskie L E
School of Biosciences, The University of Birmingham, Edgbaston, Birmingham, United Kingdom.
Biotechnol Bioeng. 2006 May 5;94(1):81-90. doi: 10.1002/bit.20814.
Resting cells of Desulfovibrio vulgaris NCIMB 8303 and Desulfovibrio desulfuricans NCIMB 8307 were used for the hydrogenase-mediated reduction of Pd(II) to Pd(0). The resulting hybrid palladium bionanocatalyst (Bio-Pd(0)) was used in the reduction of Cr(VI) to the less environmentally problematic Cr(III) species. The reduction of Cr(VI) by free and agar-immobilized Bio-Pd(0) was evaluated. Investigations using catalyst suspensions showed that Cr(VI) reduction was similar ( approximately 170 nmol Cr(VI)/h/mg Bio-Pd(0)) when Bio-Pd(0) was produced using D. vulgaris or D. desulfuricans. Continuous-flow studies using D. vulgaris Bio-Pd(0) with agar as the immobilization matrix investigated the effect of Bio-Pd(0) loading, inlet Cr(VI) concentration, and flow rate on the efficiency of Cr(VI) reduction. Reduction of Cr(VI) was highest at a D. vulgaris Bio-Pd(0) loading of 7.5 mg Bio-Pd(0)/mL agar (3:1 dry cell wt: Pd(0)), an input [Cr(VI)] of 100 microM, and a flow rate of 1.75 mL/h (approx. 3.5 column volumes/h). A mathematical interpretation predicted the activity of the immobilized Bio-Pd(0) for a given set of conditions within 5% of the value found by experiment. Considering the system as an 'artificial enzyme' analog and application of applied enzyme kinetics gave an apparent K(m) value (K(m app)) of 430 microM Cr(VI) and a determined value of flow-through reactor activity which differed by 11% from that predicted mathematically.
利用普通脱硫弧菌NCIMB 8303和脱硫脱硫弧菌NCIMB 8307的静息细胞,通过氢化酶介导将Pd(II)还原为Pd(0)。所得的钯生物纳米复合催化剂(Bio-Pd(0))用于将Cr(VI)还原为对环境危害较小的Cr(III)物种。评估了游离的和琼脂固定化的Bio-Pd(0)对Cr(VI)的还原作用。使用催化剂悬浮液的研究表明,当使用普通脱硫弧菌或脱硫脱硫弧菌制备Bio-Pd(0)时,Cr(VI)的还原情况相似(约170 nmol Cr(VI)/h/mg Bio-Pd(0))。以琼脂为固定化基质,利用普通脱硫弧菌Bio-Pd(0)进行的连续流研究考察了Bio-Pd(0)负载量、进口Cr(VI)浓度和流速对Cr(VI)还原效率的影响。在普通脱硫弧菌Bio-Pd(0)负载量为7.5 mg Bio-Pd(0)/mL琼脂(干细胞重量与Pd(0)之比为3:1)、输入[Cr(VI)]为100 μM、流速为1.75 mL/h(约3.5柱体积/h)时,Cr(VI)的还原率最高。数学解释预测了固定化Bio-Pd(0)在给定条件下的活性,其预测值与实验值相差在5%以内。将该系统视为“人工酶”类似物并应用酶动力学,得到的表观K(m)值(K(m app))为430 μM Cr(VI),测定的流通式反应器活性值与数学预测值相差11%。