This study reexamined the mechanisms for oxidative organic degradation by the binary mixture of periodate and H2O2 (PI/H2O2) that was recently identified as a new advanced oxidation process. Our findings conflicted with the previous claims that (i) hydroxyl radical (•OH) and singlet oxygen (1O2) contributed as the primary oxidants, and (ii) •OH production resulted from H2O2 reduction by superoxide radical anion (O2 •–). PI/H2O2 exhibited substantial oxidizing capacity at pH < 5, decomposing organics predominantly by •OH. The likelihood of a switch in the major oxidant under varying pH conditions was revealed. IO4 – as the major PI form under acidic conditions underwent one-electron reduction by H2O2 to yield radical intermediates, whereas H2I2O10 4– preferentially occurring at pH > 7 caused 1O2 generation through two-electron oxidation of H2O2. PI reduction by O2 •– was suggested to be a key reaction in •OH production, on the basis of the electron paramagnetic resonance detection of methyl radicals in the dimethyl sulfoxide solutions containing PI and KO2, and the absence of deuterated and 18O-labeled hydroxylated intermediates during PI activation using D2O and H2 18O2. Finally, simple oxyanion mixing subsequent to electrochemical PI and H2O2 production achieved organic oxidation, enabling a potential strategy to minimize the use of chemicals.
Boron removal from aqueous solutions has long persisted as a technological challenge, accounting for a disproportionately large fraction of the chemical and energy usage in seawater desalination and other industrial processes like lithium recovery. Here, we introduce a novel electrosorption-based boron removal technology with the capability to overcome the limitations of current state-of-the-art methods. Specifically, we incorporate a bipolar membrane (BPM) between a pair of porous carbon electrodes, demonstrating a synergized BPM–electrosorption process for the first time. The ion transport and charge transfer mechanisms of the BPM–electrosorption system are thoroughly investigated, confirming that water dissociation in the BPM is highly coupled with electrosorption of anions at the anode. We then demonstrate effective boron removal by the BPM–electrosorption system and verify that the mechanism for boron removal is electrosorption, as opposed to adsorption on the carbon electrodes or in the BPM. The effect of applied voltage on the boron removal performance is then evaluated, revealing that applied potentials above ∼1.0 V result in a decline in process efficiency due to the increased prevalence of detrimental Faradaic reactions at the anode. The BPM–electrosorption system is then directly compared with flow-through electrosorption, highlighting key advantages of the process with regard to boron sorption capacity and energy consumption. Overall, the BPM–electrosorption shows promising boron removal capability, with a sorption capacity >4.5 μmol g-C–1 and a corresponding specific energy consumption of <2.5 kWh g-B–1.
A photoelectrochemical (PEC) oxidation and flow-electrode capacitive deionization (FCDI) dual system was explored for the effective treatment of brackish water. Two anodic electrodes with electrochemically self-doped TiO2 arrays (blue-mesh/ blue-plate TiO2 nanotube arrays (BM-TNA & BP-TNA)) were fabricated by annealing at 600 °C, and applied for the treatment of a water system. Specifically, the BM-TNA confirmed lower electrical resistance and superior performance under multiple light source (UV-A, -B, and -C). Furthermore, the system generated powerful oxidizing reactive oxygen species (ROS), which were assessed via degradation of eight organic pollutants: bisphenol-A, 4-chlorophenol, cimetidine, sulfamethoxazole, benzoic acid, phenol, nitrobenzene, and acetaminophen. Decomposition efficiency was stable throughout a wide range of pH, and durability of the BM-TNA electrode was demonstrated through long-term operation. Concurrently, optimization of the FCDI process via key operational parameters (electrode mass loading, and applied voltage) achieved superior desalination performance, and specific energy consumption (SEC). In particular, increased mass loading enhanced charge transportation through the formation of stable charge-percolation pathways, leading to improved solution conductance. Finally, the feasibility of the dual system (PEC-FCDI) was verified through complete degradation of the organic substrates and successful desalination of the brackish water.
In this work, a techno-economic analysis combining process simulation and economic analysis was conducted for a methanol production capacity of 100 metric tons day–1. In particular, different water electrolysis types such as alkaline water electrolysis (AWE), polymer electrolyte/proton exchange membrane water electrolysis (PWE), and solid oxide high-temperature electrolysis (SOE) were considered as green hydrogen production methods for green methanol production. With the validated process model, the reaction temperature and pressure of 483.5 K and 63.03 bar, respectively, were selected as the optimized operating conditions based on reactant flow rates for a MeOH production capacity of 100 metric tons day–1 and energy efficiency. Based on the process simulation results, an economic parity analysis was conducted to find the switching point, which is the time that unit green methanol production cost is equal or less than gray one, by 2050. From the economic parity analysis, the unit MeOH production costs were $0.794–1.146, $0.897–0.958, and $0.697–1.177 kg–1 for green methanol production using AWE, PWE, and SOE, respectively, with solar photovoltaic-based renewable electricity. Moreover, MeOH parity can occur in 2044 for green methanol production using SOE. Therefore, it can be concluded that the possibility of green MeOH production can be confirmed in terms of the economic point of view and the continuous technology development of water electrolysis and low levelized cost of electricity can be necessary for green methanol production to put methanol parity forward.
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