Additively Manufactured 3D Micro-bioelectrodes for Enhanced Bioelectrocatalytic Operation.
Additively Manufactured 3D Micro-bioelectrodes for Enhanced Bioelectrocatalytic Operation.
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DOI：
10.1021/acsami.2c20262
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发表时间：
2023-03-10
影响因子：
9.5
通讯作者：
Tuck, Christopher
中科院分区：
文献类型：
--
作者：
Jodeiri, Keyvan;Foerster, Aleksandra;Trindade, Gustavo F.;Im, Jisun;Carballares, Diego;Fernandez-Lafuente, Roberto;Pita, Marcos;Lacey, Antonio L. De;Parmenter, Christopher;Tuck, Christopher
关键词：
基于酶的生物电子学的小型化推动了对三维（3D）微结构电极的需求，而使用传统制造工艺很难实现这种电极。与无电镀金属结合的增材制造使得能够生产具有高表面积的3D导电微架构，以用于此类器件中的潜在应用。然而，金属层和聚合物结构之间的界面脱层是主要的可靠性问题，其导致器件性能下降并最终导致器件失效。这项工作展示了一种方法，通过引入界面粘合层，在3D打印的聚合物微结构上产生具有强粘合力的高导电性和坚固的金属层。在3D打印之前，通过季戊四醇四丙烯酸酯（PETA）和3-巯基丙基三甲氧基硅烷（MPTMS）之间的硫醇-迈克尔加成反应，以1：1的化学计量比合成了具有烷氧基硅烷（−Si-（OCH 3）3）的多官能丙烯酸酯单体。烷氧基硅烷功能在投影微立体光刻（PμSLA）系统中的光聚合过程中保持完整，并在3D打印微结构的后功能化过程中用于与MPTMS的溶胶-凝胶反应，以构建界面粘合层。这导致在3D打印微结构的表面上实现丰富的硫醇官能团，其可以在化学镀期间充当金的强结合位点以改善界面粘附。通过该技术制备的3D导电微电极表现出2.2 × 107 S/m的优异电导率（体金的53%），即使在苛刻的超声处理和粘附胶带测试之后，金层与聚合物结构之间也具有强粘附力。作为概念验证，我们研究了用葡萄糖氧化酶修饰的3D金刚石晶格微电极作为单酶生物燃料电池的生物阳极。具有高催化表面积的晶格结构酶电极能够在0.35 V下产生2.5 μA/cm 2的电流密度，与立方体形状的微电极相比，电流输出增加约10倍。
The drive toward miniaturization of enzyme-based bioelectronics established a need for three-dimensional (3D) microstructured electrodes, which are difficult to implement using conventional manufacturing processes. Additive manufacturing coupled with electroless metal plating enables the production of 3D conductive microarchitectures with high surface area for potential applications in such devices. However, interfacial delamination between the metal layer and the polymer structure is a major reliability concern, which leads to device performance degradation and eventually device failure. This work demonstrates a method to produce a highly conductive and robust metal layer on a 3D printed polymer microstructure with strong adhesion by introducing an interfacial adhesion layer. Prior to 3D printing, multifunctional acrylate monomers with alkoxysilane (−Si–(OCH3)3) were synthesized via the thiol–Michael addition reaction between pentaerythritol tetraacrylate (PETA) and 3-mercaptopropyltrimethoxysilane (MPTMS) with a 1:1 stoichiometric ratio. Alkoxysilane functionality remains intact during photopolymerization in a projection micro-stereolithography (PμSLA) system and is utilized for the sol–gel reaction with MPTMS during postfunctionalization of the 3D printed microstructure to build an interfacial adhesion layer. This leads to the implementation of abundant thiol functional groups on the surface of the 3D printed microstructure, which can act as a strong binding site for gold during electroless plating to improve interfacial adhesion. The 3D conductive microelectrode prepared by this technique exhibited excellent conductivity of 2.2 × 107 S/m (53% of bulk gold) with strong adhesion between a gold layer and a polymer structure even after harsh sonication and an adhesion tape test. As a proof-of-concept, we examined the 3D gold diamond lattice microelectrode modified with glucose oxidase as a bioanode for a single enzymatic biofuel cell. The lattice-structured enzymatic electrode with high catalytic surface area was able to generate a current density of 2.5 μA/cm2 at 0.35 V, which is an about 10 times increase in current output compared to a cube-shaped microelectrode.
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影响因子：
5.4
作者：
CONRAD, JR;DODD, RA;QIU, X
通讯作者：
QIU, X
DOI：
10.1126/science.aav9750
发表时间：
2019-05-03
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Grigoryan B;Paulsen SJ;Corbett DC;Sazer DW;Fortin CL;Zaita AJ;Greenfield PT;Calafat NJ;Gounley JP;Ta AH;Johansson F;Randles A;Rosenkrantz JE;Louis-Rosenberg JD;Galie PA;Stevens KR;Miller JS
通讯作者：
Miller JS
影响因子：
7.4
作者：
Hu, Xue-Bo;Liu, Yan-Ling;Huang, Wei-Hua
通讯作者：
Huang, Wei-Hua
影响因子：
56.9
作者：
Ahn, Bok Y.;Duoss, Eric B.;Lewis, Jennifer A.
通讯作者：
Lewis, Jennifer A.
影响因子：
4.2
作者：
Kang, T;Park, Y;Yi, J
通讯作者：
Yi, J