Performance enhancement and mechanism of electroenhanced peroxymonosulfate activation by single-atom Fe catalyst modified electrodes.

Peroxymonosulfate-based electrochemical advanced oxidation processes (PMS-EAOPs) have great potential for sustainable water purification, so an in-depth understanding of its catalytic mechanism is imperative to facilitate its practical application. Herein, the performance enhancement and mechanism of electroenhanced PMS activation by single-atom Fe catalyst modified carbon felt was investigated. Compared with the anode, the cathode exhibited faster bisphenol A degradation (kcathode = 0.073 vs. kanode = 0.015 min-1), increased PMS consumption (98.8 vs. 10.3%), and an order of magnitude reduction of Fe dissolution (0.068 vs. 0.787 mg L-1). Mass transfer is a key factor limiting PMS activation, while the electrostriction of water in the hydrophobic region caused by cathode electric field (CEF) significantly increased mass transfer coefficient (km, cathode = 1.49 × 10-4 vs. km, anode = 2.68 × 10-5 m s-1). The enhanced activation of PMS is a synergistic result between electroactivation and catalyst-activation, which is controlled by the applied current density. 1O2 and direct electron transfer are the main active species and activation pathway, which achieve high degradation efficiency over pH 3 to 10. Density functional theory calculations prove CEF increases the adsorption energy, lengthens the O-O bond in PMS, and promotes charge transfer. A flow-through convection unit achieves sustainable operation with high removal efficiency (99.5% to 97.5%), low electrical energy consumption (0.15 kWh log-1 m-3), and low Fe leaching (0.81% of the total single atom Fe). This work reveals the critical role of electric fields in modulating Fenton-like catalytic activity, which may advance the development of advanced oxidation processes and other electrocatalytic applications.

Regulating the electronic structure by P-doping cobalt-based catalyst for atomic hydrogen mediated electrocatalytic dechlorination.

Electrocatalytic dechlorination by atomic hydrogen (H*) is efficient, but limited by the low efficiency of H* production. Herein, a phosphorus-doped cobalt nitrogen carbon catalyst (Co-NP/C) was prepared, which had high catalytic activity in a wide pH range (3-11). The turnover frequency of Co-NP/C (3.54 min-1) was 1.21-59000 times superior to that of current Pd-based and non-noble metal catalysts (0.00006-2.92 min-1). Co-NP/C significantly enhanced H* generation, which was 1.52, 2.44, and 3.77 times stronger than that of Co-N/C, NP/C, and N/C, respectively, since the introduction of phosphorus was found enhanced the electron density of cobalt and regulated the electron transfer. Co-NP/C showed outstanding catalytic performance after ten cycles and could achieve nearly complete chloramphenicol removal. This regulation method was verified to be effective for other non-noble metal (Fe, Mn, Cu, Ni) phosphorus doped catalysts, proposing a general class for efficient electrochemical dechlorination, which would be of great significance for the elimination of chlorinated organic pollutants.

A pilot scale of electrochemical integrated treatment technology and equipment driven by solar energy for decentralized domestic sewage treatment.

Based on the natural air diffusion electrode (NADE) cathode, a solar-driven electrochemical integrated sewage treatment technology and equipment in a pilot scale was developed to treat dispersed rural wastewater. The non-aeration NADE had efficient and stable H2O2 production performance, maintaining the H2O2 output between 1474 and 1535 mg h-1 within 50 h with the current efficiency of 77.4%-80.6%. This electrochemical integrated wastewater treatment system was coupled with technologies such as dual-cathode electro-Fenton, peroxi-coagulation and photoelectro-Fenton, which effectively improved the conversion and utilization efficiency of H2O2. It integrated Fenton-like oxidation, electro-oxidation and UV/H2O2, as well as Fe(OH)3-dominated flocculation, which could effectively remove various pollutants in wastewater. The integrated sewage treatment equipment (500 L d-1) realized the effective treatment of a rural decentralized domestic sewage, achieving simultaneous removal of chemical oxygen demand (COD), NH3-N, total phosphorus (TP) and bacteria. Driven by solar energy, its application feasibility, superiority and stability have been proved, providing theoretical and technical support for the efficient and low-consumption treatment of dispersed organic wastewater.

B-doping mediated formation of oxygen vacancies in Bi2Sn2O7 quantum dots with a unique electronic structure for efficient and stable photoelectrocatalytic sulfamethazine degradation.

This study devised a straightforward one-step approach that enabled simultaneous boron (B) doping and oxygen vacancies (OVs) production on Bi2Sn2O7 (BSO) (B-BSO-OV) quantum dots (QDs), optimizing the electrical structure of the photoelectrodes. Under light-emitting diode (LED) illumination and a low potential of 1.15 V, B-BSO-OV demonstrated effective and stable photoelectrocatalytic (PEC) degradation of sulfamethazine (SMT), achieving the first-order kinetic rate constant of 0.158 min-1. The surface electronic structure, the different factors influencing the PEC degradation of SMT, and the degradation mechanism were studied. Experimental studies have shown that B-BSO-OV exhibits strong visible light trapping ability, high electron transport ability, and superior PEC performance. DFT calculations show that the presence of OVs on BSO successfully reduces the band gap, controls the electrical structure, and accelerates charge transfer. This work sheds light on the synergistic effects of the electronic structure of B-doping and OVs in heterobimetallic oxide BSO under the PEC process and offers a promising approach for the design of photoelectrodes.