Institute of New Energy Chemistry and Environmental Science, College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, PR China.
ChemSusChem. 2012 Oct;5(10):2000-10. doi: 10.1002/cssc.201200305. Epub 2012 Sep 10.
A solar thermal electrochemical production (STEP) pathway was established to utilize solar energy to drive useful chemical processes. In this paper, we use experimental chemistry for efficient STEP wastewater treatment, and suggest a theory based on the decreasing stability of organic pollutants (hydrocarbon oxidation potentials) with increasing temperature. Exemplified by the solar thermal electrochemical oxidation of phenol, the fundamental model and experimental system components of this process outline a general method for the oxidation of environmentally stable organic pollutants into carbon dioxide, which is easily removed. Using thermodynamic calculations we show a sharply decreasing phenol oxidation potential with increasing temperature. The experimental results demonstrate that this increased temperature can be supplied by solar thermal heating. In combination this drives electrochemical phenol removal with enhanced oxidation efficiency through (i) a thermodynamically driven decrease in the energy needed to fuel the process and (ii) improved kinetics to sustain high rates of phenol oxidation at low electrochemical overpotential. The STEP wastewater treatment process is synergistic in that it is performed with higher efficiency than either electrochemical or photovoltaic conversion process acting alone. STEP is a green, efficient, safe, and sustainable process for organic wastewater treatment driven solely by solar energy.
建立了一种太阳能热电化学生产（STEP）途径，以利用太阳能驱动有用的化学过程。在本文中，我们使用实验化学来有效处理 STEP 废水，并提出了一个基于有机污染物稳定性随温度升高而降低的理论。以苯酚的太阳能热电化学氧化为例，该过程的基本模型和实验系统组件概述了一种将环境稳定的有机污染物氧化成易于去除的二氧化碳的一般方法。通过热力学计算，我们表明苯酚氧化势随温度升高而急剧下降。实验结果表明，这种升高的温度可以通过太阳能热加热来提供。结合起来，这通过（i）热力学驱动的降低过程所需的能量和（ii）提高动力学以在低电化学过电势下维持高苯酚氧化速率，来驱动电化学苯酚去除并提高氧化效率。STEP 废水处理过程具有协同作用，因为它的效率高于单独使用电化学或光伏转换过程。STEP 是一种绿色、高效、安全且可持续的有机废水处理工艺，完全由太阳能驱动。
