J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, Dolejskova 3, 18223 Prague 8, Czech Republic.
Phys Chem Chem Phys. 2019 Feb 13;21(7):4063-4071. doi: 10.1039/c8cp06961a.
The effect of doping on the electronic properties in bulk single-walled carbon nanotube (SWCNT) samples is studied for the first time using a new in situ Raman spectroelectrochemical method, and further verified by DFT calculations and photoresponse. We use p-/n-doped SWCNTs prepared by diazonium reactions as a versatile chemical strategy to control the SWCNT behavior. The measured and calculated data testify an acceptor effect of 4-aminobenzenesulfonic acid (p-doping), and a donor effect (n-doping) in the case of benzyl alcohol. In addition, pristine and covalently functionalized SWCNTs were used for the preparation of photoactive film electrodes. The photocathodic current in the photoelectrochemical cell is consistently modulated by the doping group. These results validate the in situ Raman spectroelectrochemistry as a unique tool box for predicting the electronic properties of functionalized SWCNTs in the form of thin films and their operational functionality in thin film devices for future optoelectronic applications.
首次使用新型原位拉曼光谱电化学方法研究了掺杂对体相单壁碳纳米管 (SWCNT) 样品电子性质的影响,并通过 DFT 计算和光响应进一步验证。我们使用重氮反应制备的 p-/n-掺杂 SWCNT 作为一种通用的化学策略来控制 SWCNT 的行为。测量和计算数据证明了 4-氨基苯磺酸(p-掺杂)的受主效应,以及苯甲醇情况下的给体效应(n-掺杂)。此外,还使用原始和共价功能化的 SWCNT 来制备光活性薄膜电极。光电化学电池中的光阴极电流被掺杂基团一致地调制。这些结果验证了原位拉曼光谱电化学作为一种独特的工具包,可用于预测以薄膜形式的功能化 SWCNT 的电子性质及其在薄膜器件中的操作功能,用于未来的光电应用。