Provincial Key Laboratory of Oil & Gas Chemical Technology, Institute of New Energy Chemistry and Environmental Science, College of Chemistry and Chemical Engineering, Northeast Petroleum University , Daqing 163318, P. R. China.
J Phys Chem B. 2017 Mar 2;121(8):1900-1907. doi: 10.1021/acs.jpcb.6b12272. Epub 2017 Feb 16.
The solar thermal electrochemical process (STEP) has sustainably accounted for the solar thermo- and electrochemical oxidation of sodium dodecyl benzene sulfonate (SDBS) fully driven by solar energy, gaining a high efficiency with a fast rate by the combination of thermochemistry and electrochemistry. In this article, thermoinduced electrochemistry was resolved for an in-depth understanding of the STEP degradation of SDBS. We employed thermodependent cyclic voltammetry, temperature-dependent fluorescence-electrochemical spectroscopy, and time-dependent electrochemical current spectroscopy for studying the electrochemistry, including the reaction, pathway, and mechanism. First, thermodependent cyclic voltammetric spectra indicated that the SDBS in sodium chloride solution is oxidized via an indirect process initialized by active chlorine, substantially accelerating and completing the oxidation process. Second, temperature-dependent fluorescence-electrochemical spectra displayed the pathway and kinetics by finding the initial desulfonation and the subsequent breaking of the alkyl side chain and benzene ring. Finally, time-dependent electrochemical current spectra demonstrated that the initial desulfonation is the fast step by generating the high current and the subsequent breaking is the slow one by a low current response, which is in agreement with the temperature-dependent fluorescence-electrochemical spectra. A panoramic view is proposed and schemed for fully understanding the process and mechanism of the STEP degradation of SDBS. Moreover, the efficiency and effectiveness of SDBS degradation were proven to be significantly enhanced by using the STEP in outdoor and indoor tests. It is a novel and energy-free route for wastewater treatment, accomplished by the synergistic use of solar energy without any other input of energy.
太阳能热电化学过程(STEP)可持续地利用太阳能完全驱动十二烷基苯磺酸钠(SDBS)的太阳能热和电化学氧化,通过热化学和电化学的结合获得高效率和快速速率。在本文中,我们通过热诱导电化学解决了 STEP 降解 SDBS 的深入理解。我们采用了依赖温度的循环伏安法、温度依赖的荧光电化学光谱法和时间依赖的电化学电流光谱法来研究电化学,包括反应、途径和机制。首先,依赖温度的循环伏安光谱表明,SDBS 在氯化钠溶液中通过活性氯引发的间接过程氧化,显著加速和完成氧化过程。其次,温度依赖的荧光电化学光谱通过发现初始脱硫和随后的烷基侧链和苯环断裂,显示了途径和动力学。最后,时间依赖的电化学电流光谱表明,初始脱硫是快速步骤,产生高电流,随后的断裂是缓慢步骤,电流响应低,这与温度依赖的荧光电化学光谱一致。提出并设计了全景视图,以充分理解 STEP 降解 SDBS 的过程和机制。此外,在户外和室内测试中,证明了 STEP 显著提高了 SDBS 降解的效率和效果。这是一种新颖的、无能量输入的废水处理途径,通过协同利用太阳能完成,无需任何其他能量输入。