| 两种功能化纳米金粒子固酶电极的催化性能 |
| Catalytic Effect of Two Kinds of Functionalized Nano-Gold Particles with Immobilized Enzymes Modified Electrodes |
|
| 摘要: 以合成的4-巯基苯甲酸功能化纳米金粒子和聚乙烯基吡啶包覆纳米金粒子分别作为固酶载体,制备了2种新型固酶电极,在此基础上组装了2种酶燃料电池。采用电化学方法结合紫外可见分光光度法、透射电镜技术等手段研究了固酶载体的形貌,酶-载体间相互作用对电极表面固定酶分子的光谱学性质,酶-电极间直接电子迁移能力和催化底物反应性能的影响,进一步评估和比较了两种酶燃料电池的能量输出性能。实验结果表明：4-巯基苯甲酸功能化纳米金粒子固酶基电极可以实现酶-电极间的直接电子迁移而且对葡萄糖和氧气具有良好的催化性能(催化反应起始电位分别为-0.03和0.96 V,底物转化频率分别是1.3和0.5 s-1),其催化性能的重现性、长期使用性能、酸碱耐受性和热稳定性良好,随着自组装固酶层数的增加,催化性能随之增强直至达到极限催化电流;电池性能测试结果表明4-巯基苯甲酸功能化纳米金粒子固酶基燃料电池的开路电压为0.88 V,最大输出能量密度：864.0 μW·cm-2,长期使用性能优异(储存3 周后仍可达到最佳能量输出的80%以上)。 |
| 关键词: 漆酶 葡萄糖氧化酶 功能化纳米金粒子 直接电子迁移 催化性能 酶燃料电池 |
| 基金项目: 国家自然科学基金(No.21363024),新疆师范大学博士科研启动基金(No.XJNUBS1228),新疆维吾尔自治区2013年度高校科研计划青年 教师培育项目(No.XJEDU2013S29)和新疆师范大学研究生科技创新项目(No.XSY201502009)资助。 |
| Abstract: Synthesized 4-mercaptobenzoic acid functionalized nano-gold particles and poly(vinylpyridine) overlapped nanogold-particles, were used as enzyme carriers to prepare two kinds of novel enzyme-based electrodes, respectively. Two prototypes of enzyme-based fuel cells were fabricated on the basis of previously described electrodes. Morphology of matrix with immobilized enzymes, influences of interaction between enzyme molecules and carriers on spectrometric characteristics of electrode surface anchored enzyme molecules, direct electron transfer dynamics between enzyme active centers and electrodes and catalytic function in substrate involved reaction, were investigated by the means of electrochemical method together with such techniques as ultra-violet/visible spectrometry(UV-Vis) and transmission electron microscope(TEM). Energy out-put performances for two kinds of fabricated enzyme-based fuel cells were evaluated and compared systematically. Results from test indicated 4-mercaptobenzoic acid surface-tailored nano-gold particles with enzymes modified electrodes displayed direct electron transfer between enzyme active sites and electrode, revealing favorable catalytic effect on glucose electro-oxidation and oxygen electro-reduction(catalytic reaction onset potential for glucose oxidationn and oxygen reduction: -0.03 and 0.96 V, turn-over frequency of substrates: 1.3 and 0.5 s-1, respectively). Reproducibility, long-term usability, acid/base endurance and thermal stability in catalytic function of previously mentioned electrode were preferable. Catalytic effect in substrate-related reaction of enzyme-based electrode increased with the thickness of self-assembled immobilized enzyme layers until approaching to maximal catalytic current. Test on performance of fuel cell showed open circuit voltage(OCV, 0.88 V), maximal out-put energy density(864.0 μW·cm-2) and excellent long-term stability(retaining above 80% of optimal energy out-put after storage for 3 weeks). |
| Keywords: laccase glucose oxidase functionalized nano-gold particle direct electron transfer catalytic function enzymatic biofuel cell |
| 投稿时间：2015-08-30 修订日期：2015-10-20 |
| 摘要点击次数: 1496 |
| 全文下载次数: 2051 |
| 曾涵,杨阳,赵淑贤.两种功能化纳米金粒子固酶电极的催化性能[J].无机化学学报,2015,31(12):2305-2314. |
| 查看全文 查看/发表评论 下载PDF阅读器 |
| Support information: 相关附件： file150536_支持信息专门文档修改稿.doc |
|
|
|
|
|
|
