School of Chemical and Environmental Engineering , Shanghai Institute of Technology , Shanghai 201418 , China.
Anal Chem. 2018 Mar 6;90(5):3149-3155. doi: 10.1021/acs.analchem.7b04395. Epub 2018 Feb 14.
A simple, noncovalent modification strategy was proposed to synthesize poly-l-lysine-black phosphorus (pLL-BP) hybrid. BP nanoflakes were prepared with a water-phase exfoliation method. pLL can adhere to the surface of BP via hydrophobic interaction between butyl chains of pLL and the BP surface as well as the electrostatic interaction between the protonated amino groups on pLL and the negative charge on deprotonated PO groups remaining on BP. The as-synthesized pLL-BP hybrid turns out to be an ideal matrix for hemoglobin immobilization and direct electron transfer. Good conductivity and biocompatibility of BP maintain the native structure and the bioactivity of hemoglobin (Hb), facilitating the direct electron transfer between the electroactive center of Hb and electrode. The rate constant ( k) for direct electron transfer of Hb@pLL-BP is calculated to be 11.24 s. The constructed Hb-pLL-BP based enzymatic electrochemical biosensor displays excellent catalytic activity toward the reduction of oxygen and hydrogen peroxide. The electrochemical response toward HO exhibits a linear dependence on hydrogen peroxide concentration ranging between 10 μM and 700 μM. The results demonstrate that the pLL-BP hybrid can act as a biocompatible building block for the construction of novel biofuel cells, bioelectronics, and biosensors.
提出了一种简单的非共价修饰策略，用于合成聚赖氨酸-黑磷（pLL-BP）杂化物。通过水相剥离法制备 BP 纳米片。pLL 可以通过 pLL 的丁基链与 BP 表面之间的疏水相互作用以及 pLL 上质子化的氨基与 BP 上残留的去质子化 PO 基团之间的静电相互作用附着在 BP 表面上。所合成的 pLL-BP 杂化物是血红蛋白固定和直接电子转移的理想基质。BP 的良好导电性和生物相容性保持了血红蛋白（Hb）的天然结构和生物活性，促进了 Hb 活性中心与电极之间的直接电子转移。Hb@pLL-BP 的直接电子转移速率常数（k）计算为 11.24 s。基于 Hb-pLL-BP 的构建的酶电化学生物传感器对氧气和过氧化氢的还原表现出优异的催化活性。对 HO 的电化学响应对过氧化氢浓度在 10 μM 至 700 μM 之间表现出线性依赖性。结果表明，pLL-BP 杂化物可用作构建新型生物燃料电池、生物电子学和生物传感器的生物相容性构建基块。
