Liu Rujia, Ma Yingfei, Shen Xiaoyue, Wang Dengchao
School of Chemical Sciences, University of Chinese Academy of Sciences Beijing 10049 P. R. China
Chem Sci. 2021 Oct 4;12(44):14752-14757. doi: 10.1039/d1sc04282c. eCollection 2021 Nov 17.
Conductive nanopipettes have been extensively used as powerful multifunctional probes for electrochemical and ion transport measurements, while the involved charge transfer processes have not been fully explored. In this paper, we use both experimental and simulation methods to de-convolute and quantify the respective electron transfer (ET) and ion transport (IT) contributions to the resulting current signals in carbon nanopipettes (CNPs). The results present that the current signals in CNPs are determined by ET in the case of low solution depth and long timescales, while IT becomes dominant at short timescales or high solution depth. In addition, the electrochemically and chemically irreversible ET processes in CNPs were also quantified. The elucidated and quantified charge transport processes inside CNPs will help control and optimize the IT and ET processes at the nanoscale, promoting better and broad usage of conductive nanopipettes in single-entity sensing and imaging applications.
导电纳米吸管已被广泛用作电化学和离子传输测量的强大多功能探针，但其涉及的电荷转移过程尚未得到充分探索。在本文中，我们使用实验和模拟方法来解卷积和量化电子转移（ET）和离子传输（IT）对碳纳米吸管（CNP）中所得电流信号的各自贡献。结果表明，在低溶液深度和长时间尺度的情况下，CNP中的电流信号由ET决定，而在短时间尺度或高溶液深度时，IT占主导地位。此外，还对CNP中电化学和化学不可逆的ET过程进行了量化。阐明和量化CNP内部的电荷传输过程将有助于在纳米尺度上控制和优化IT和ET过程，促进导电纳米吸管在单实体传感和成像应用中的更好和更广泛应用。
