Fabrication, characterization, and functionalization of dual carbon electrodes as probes for scanning electrochemical microscopy (SECM).
Fabrication, characterization, and functionalization of dual carbon electrodes as probes for scanning electrochemical microscopy (SECM).
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DOI：
10.1021/ac401476z
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发表时间：
2013-08-06
影响因子：
7.4
通讯作者：
Unwin, Patrick R.
中科院分区：
文献类型：
--
作者：
McKelvey, Kim;Nadappuram, Binoy Paulose;Actis, Paolo;Takahashi, Yasufumi;Korchev, Yuri E.;Matsue, Tomokazu;Robinson, Colin;Unwin, Patrick R.
通过将热解碳沉积到石英 theta 纳米管中，可以快速、轻松且廉价地制造双碳电极 (DCE)。 DCE 的尺寸可以通过调整用于制造纳米管的牵引参数来控制。当在生成/收集 (G/C) 模式下运行时，电极之间的微小间距可实现约 10% 的合理收集效率。 30%。开发了三维有限元法 (FEM) 模拟来预测这些电极的电流响应，作为估计探头几何形状的一种方法。单个电极的伏安测量与生成/收集测量相结合，为电极尺寸提供了合理的指导。 DCE 用于扫描电化学显微镜 (SECM) 配置，并且考虑了它们在接近曲线和成像方面的用途。 G/C 方法曲线测量显示对基材的性质特别敏感，绝缘表面会提高收集效率，而导电表面会导致收集效率降低。作为概念验证，DCE 进一步用于局部生成人工电子受体，并在孤立的类囊体膜上的光合作用过程中跟踪该物种的通量及其还原形式。此外，报告并分析了单个类囊体膜的二维图像，以证明 G/C 测量对局部表面过程的高灵敏度。最后表明，可以通过在 DCE 中的两个电极之一上选择性沉积铂，同时使另一个电极保持不变，从而对单个纳米尺寸电极进行功能化。这表明了此类探针在纳米级测量和成像方面的未来多功能性。
Dual carbon electrodes (DCEs) are quickly, easily, and cheaply fabricated by depositing pyrolytic carbon into a quartz theta nanopipet. The size of DCEs can be controlled by adjusting the pulling parameters used to make the nanopipet. When operated in generation/collection (G/C) mode, the small separation between the electrodes leads to reasonable collection efficiencies of ca. 30%. A three-dimensional finite element method (FEM) simulation is developed to predict the current response of these electrodes as a means of estimating the probe geometry. Voltammetric measurements at individual electrodes combined with generation/collection measurements provide a reasonable guide to the electrode size. DCEs are employed in a scanning electrochemical microscopy (SECM) configuration, and their use for both approach curves and imaging is considered. G/C approach curve measurements are shown to be particularly sensitive to the nature of the substrate, with insulating surfaces leading to enhanced collection efficiencies, whereas conducting surfaces lead to a decrease of collection efficiency. As a proof-of-concept, DCEs are further used to locally generate an artificial electron acceptor and to follow the flux of this species and its reduced form during photosynthesis at isolated thylakoid membranes. In addition, 2-dimensional images of a single thylakoid membrane are reported and analyzed to demonstrate the high sensitivity of G/C measurements to localized surface processes. It is finally shown that individual nanometer-size electrodes can be functionalized through the selective deposition of platinum on one of the two electrodes in a DCE while leaving the other one unmodified. This provides an indication of the future versatility of this type of probe for nanoscale measurements and imaging.
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影响因子：
7.4
作者：
Li, Yongxin;Bergman, David;Zhang, Bo
通讯作者：
Zhang, Bo
影响因子：
6.6
作者：
Fushimi, Koji;Matsushita, Ken-ichiro;Hasegawa, Yasuchika
通讯作者：
Hasegawa, Yasuchika
DOI：
10.1146/annurev-anchem-062011-143124
发表时间：
2012-01-01
期刊：
ANNUAL REVIEW OF ANALYTICAL CHEMISTRY, VOL 5
影响因子：
--
作者：
Cox, Jonathan T.;Zhang, Bo
通讯作者：
Zhang, Bo
影响因子：
--
作者：
BARD, AJ;MIRKIN, MV;WIPF, DO
通讯作者：
WIPF, DO
影响因子：
7.4
作者：
MIRKIN, MV;BARD, AJ
通讯作者：
BARD, AJ