Yan Yi-Ming, Yehezkeli Omer, Willner Itamar
Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
Chemistry. 2007;13(36):10168-75. doi: 10.1002/chem.200700806.
Integrated, electrically contacted beta-nicotinamide adenine dinucleotide- (NAD(+)) or beta-nicotinamide adenine dinucleotide phosphate- (NADP(+)) dependent enzyme electrodes were prepared on single-walled carbon nanotube (SWCNT) supports. The SWCNTs were functionalized with Nile Blue (1), and the cofactors NADP(+) and NAD(+) were linked to 1 through a phenyl boronic acid ligand. The affinity complexes of glucose dehydrogenase (GDH) with the NADP(+) cofactor or alcohol dehydrogenase (AlcDH) with the NAD(+) cofactor were crosslinked with glutaric dialdehyde and the biomolecule-functionalized SWCNT materials were deposited on glassy carbon electrodes. The integrated enzyme electrodes revealed bioelectrocatalytic activities, and they acted as amperometric electrodes for the analysis of glucose or ethanol. The bioelectrocatalytic response of the systems originated from the biocatalyzed oxidation of the respective substrates by the enzyme with the concomitant generation of NAD(P)H cofactors. The electrocatalytically mediated oxidation of NAD(P)H by 1 led to amperometric responses in the system. Similarly, an electrically contacted bilirubin oxidase (BOD)-SWCNT electrode was prepared by the deposition of BOD onto the SWCNTs and the subsequent crosslinking of the BOD units using glutaric dialdehyde. The BOD-SWCNT electrode revealed bioelectrocatalytic functions for the reduction of O(2) to H(2)O. The different electrically contacted SWCNT-based enzyme electrodes were used to construct biofuel cell elements. The electrically contacted GDH-SWCNT electrode was used as the anode for the oxidation of the glucose fuel in conjunction with the BOD-SWCNT electrode in the presence of O(2), which acted as an oxidizer in the system. The power output of the cell was 23 muW cm(-2). Similarly, the AlcDH-SWCNT electrode was used as the anode for the oxidation of ethanol, which was acting as the fuel, with the BOD-SWCNT electrode as the cathode for the reduction of O(2). The power output of the system was 48 microW cm(-2).
在单壁碳纳米管(SWCNT)载体上制备了集成的、电接触的β-烟酰胺腺嘌呤二核苷酸(NAD(+))或β-烟酰胺腺嘌呤二核苷酸磷酸(NADP(+))依赖性酶电极。用尼罗蓝(1)对SWCNT进行功能化处理,辅酶NADP(+)和NAD(+)通过苯基硼酸配体与1相连。葡萄糖脱氢酶(GDH)与NADP(+)辅酶的亲和复合物或乙醇脱氢酶(AlcDH)与NAD(+)辅酶的亲和复合物用戊二醛交联,然后将生物分子功能化的SWCNT材料沉积在玻碳电极上。集成酶电极显示出生物电催化活性,可作为安培电极用于分析葡萄糖或乙醇。该系统的生物电催化响应源于酶对相应底物的生物催化氧化,并伴随产生NAD(P)H辅酶。1对NAD(P)H的电催化介导氧化导致系统产生安培响应。同样,通过将胆红素氧化酶(BOD)沉积在SWCNT上,然后用戊二醛对BOD单元进行交联,制备了电接触的BOD-SWCNT电极。BOD-SWCNT电极显示出将O(2)还原为H(2)O的生物电催化功能。不同的电接触SWCNT基酶电极用于构建生物燃料电池元件。在O(2)存在的情况下,电接触的GDH-SWCNT电极用作阳极,用于氧化葡萄糖燃料,而BOD-SWCNT电极用作阴极,O(2)在系统中作为氧化剂。该电池的功率输出为23 μW cm(-2)。同样,AlcDH-SWCNT电极用作阳极,用于氧化作为燃料的乙醇,BOD-SWCNT电极用作阴极,用于还原O(2)。该系统的功率输出为48 μW cm(-2)。