ABSTRACT
Recovery of ammonium from wastewater represents a sustainable strategy within the context of global resource depletion, environmental pollution and carbon neutralization. The present study developed an advanced self-reporting electroswitchable colorimetric platform (SECP) to realize smart ammonium recovery based on the electrically stimulated transformation of Prussian blue/Prussian white (PB/PW) redox couple. The key to SECP was the selectivity of ammonium adsorption, sensitivity of desorption to electric signals and visualability of color change during switchable adsorption/desorption transformation. The results demonstrated the electrochemical intercalation-induced selective adsorption of NH4+ (selectivity coefficient of 3-19 versus other cations) and deintercalation-induced desorption on the PB-film electrode. At applied voltage of 1.2 V for 20 min, the negatively charged PB-film electrode achieved the maximum adsorption capacity of 3.2 mmol g-1. Reversing voltage to -0.2 V for 20 min resulted in desorption efficiency as high as 99%, indicating high adsorption/desorption reversibility and cyclic stability. The Fe(III)/Fe(II) redox dynamics were responsible for PB/PW transformation during reversible intercalation/deintercalation of NH4+. Based on the blue/transparence color change of PB/PW, the quantitative relationship was established between amounts of NH4+ adsorbed and extracted RGB values by multiple linear regression (R2 = 0.986, RMSE = 0.095). Then, the SECP was created upon the unique capability of real-time monitoring and feedback of color change of electrode to realize the automatic control of NH4+ adsorption/desorption. During five cycles of tests, the adsorption process consistently peaked at an average value of 3.15±0.04 mmol g-1, while desorption reliably approached the near-zero average of 0.06±0.04 mmol g-1. The average time of duration was 19.6±1.67 min for adsorption and 18.8±1.10 min for desorption, respectively. With electroswitchability, selectivity and self-reporting functionalities, the SECP represents a paradigm shift in smart ammonium recovery from wastewater, making wastewater treatment and resource recovery more efficient, more intelligent and more sustainable.
