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A light-addressable potentiometric sensor (LAPS) is a semiconductor-based sensor platform for sensing and imaging of various chemical species. Being a potentiometric sensor, no faradaic current flows through its sensing surface, and no electrochemical reaction takes place in the course of LAPS measurement. In this study, a four-electrode system is proposed, in which a LAPS is combined with the conventional three-electrode electrochemical system. A LAPS is included as the fourth electrode for potentiometric sensing and imaging of the target analyte in the course of an electrochemical reaction taking place on the surface of the working electrode. The integrated system will be useful for analyzing dynamic processes, where both the electrochemical process on the electrode surface and the ion distribution in the solution need to be simultaneously investigated. Different grounding modes of control circuits that can simultaneously conduct potentiostatic/galvanostatic polarization and LAPS measurement are designed, and their functionalities are tested. The interference between polarization and LAPS measurement will also be discussed.

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Organic pollutants can alter the physicochemical properties and microbial communities of water bodies. In water contaminated with organic pollutants, the unique extracellular electron transfer mechanisms that promote sulfamethoxazole (SMX) degradation in tri-electrode microbial electrochemical systems (TE-MES) may be impacted. To simulate biodegradable organic matter contamination, glucose (GLU) was added. Metagenomics and metabolomics were used to analyze changes in microbial community structure, metabolism, and function on the electrodes. GLU addition accelerated water quality deterioration, and enhanced SMX degradation. Microbial taxa on the electrodes experienced selective enrichment. Notably, methanogens and SMX-degrading bacteria were enriched, while denitrifying bacteria and antibiotic-resistant bacteria were suppressed. Enriched metabolites were linked to 15 metabolic pathways and other functions like microbial signaling and genetics. Non-redundant genes also clustered in metabolic pathways, aligning with metabolite enrichment results. Additional pathways involved life cycle processes and protein interactions. Enzymes related to carbon metabolism, particularly glycoside hydrolases, increased significantly, indicating a shift in carbon metabolism on microbial electrodes after GLU addition. The abundance of intracellular electron transfer enzymes rose, while outer membrane proteins decreased. This contrasts with the typical TE-MES mechanism where outer membrane proteins facilitate SMX degradation. The presence of organic pollution may shift SMX degradation from an extracellular electrochemical process to an intracellular metabolic process, possibly involving co-metabolism with simple organic compounds. This study provides mechanistic insights and theoretical guidance for using TE-MES with embedded microbial electrodes to treat antibiotic-contaminated water affected by organic pollution.

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BACKGROUND: Pseudomonas putida KT2440 has emerged as a promising host for industrial bioproduction. However, its strictly aerobic nature limits the scope of applications. Remarkably, this microbe exhibits high bioconversion efficiency when cultured in an anoxic bio-electrochemical system (BES), where the anode serves as the terminal electron acceptor instead of oxygen. This environment facilitates the synthesis of commercially attractive chemicals, including 2-ketogluconate (2KG). To better understand this interesting electrogenic phenotype, we studied the BES-cultured strain on a systems level through multi-omics analysis. Inspired by our findings, we constructed novel mutants aimed at improving 2KG production. RESULTS: When incubated on glucose, P. putida KT2440 did not grow but produced significant amounts of 2KG, along with minor amounts of gluconate, acetate, pyruvate, succinate, and lactate. 13C tracer studies demonstrated that these products are partially derived from biomass carbon, involving proteins and lipids. Over time, the cells exhibited global changes on both the transcriptomic and proteomic levels, including the shutdown of translation and cell motility, likely to conserve energy. These adaptations enabled the cells to maintain significant metabolic activity for several weeks. Acetate formation was shown to contribute to energy supply. Mutants deficient in acetate production demonstrated superior 2KG production in terms of titer, yield, and productivity. The ∆aldBI ∆aldBII double deletion mutant performed best, accumulating 2KG at twice the rate of the wild type and with an increased yield (0.96 mol/mol). CONCLUSIONS: By integrating transcriptomic, proteomic, and metabolomic analyses, this work provides the first systems biology insight into the electrogenic phenotype of P. putida KT2440. Adaptation to anoxic-electrogenic conditions involved coordinated changes in energy metabolism, enabling cells to sustain metabolic activity for extended periods. The metabolically engineered mutants are promising for enhanced 2KG production under these conditions. The attenuation of acetate synthesis represents the first systems biology-informed metabolic engineering strategy for enhanced 2KG production in P. putida. This non-growth anoxic-electrogenic mode expands our understanding of the interplay between growth, glucose phosphorylation, and glucose oxidation into gluconate and 2KG in P. putida.

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Additive abuse in fishery, such as tricaine methanesulfonate (MS222), ciprofloxacin (CPFX), and malachite green (MG), threatens public human health and interferes with the ecological equilibrium of water resources. However, the majority of the present detection methods suffer from high costs, complex operations, and poor portability. Therefore, real-time and rapid detection of the above additive by mobile devices is becoming increasingly important. Here we report the fabrication and performance of an entirely electrochemical system with USB-stick size for simultaneous detection of MS222, CPFX, and MG, as well as pH and permittivity. The limits of detections are 0.17, 0.67, and 0.28 µg/mL, while the resolution ratios are 10 %, 10 %, and 5 % for MS222, MG, and CPFX, respectively. For both pH and permittivity, they have linear regressions measured by brightness and capacitance of the sample respectively, at the range of 1.5-9 (pH) and 10-20 (permittivity). The interference experiments, using target analytes (40 µg/mL) and 15 interfering analytes (80 µg/mL), demonstrated the anti-interference performance of the sensor patches. The field studies on carps, catfishes, and chubs indicated that the developed integrated portable system could be used for real sample analysis with high performance.

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This study is the first to explore the performance and mechanism of biochar-impacted sediment microbial fuel cell for removing antibiotic resistance genes (ARGs), and examines the effects of different biochar contents. The addition of 5% biochar produced the highest output voltage and power density, which increased by 100% and 219%, respectively, while simultaneously reducing the abundance and risk of ARGs. Comparatively, the addition of moderate amount of biochar (1-5%) promoted the removal of ARGs, while the opposite was true for excessive (10%) biochar. Biochar affected ARGs through prophages, insertion sequence, and transposons. Biological factors and voltage jointly influenced ARGs variation, with the former accounting for 56%. Further analysis of functional genes indicated that biochar controlled ARGs by regulating the synthesis of genetic material and amino acids to influence metabolism. Overall, findings of this study shed light on the potential removal of ARGs in microbial electrochemical systems.

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Although dissolved oxygen plays an important role in electro-Fenton-like processes, few investigations have revealed its underlying effects in such processes. Herein, the effect of dissolved oxygen on peroxide activation in an electro-Fenton-like system comprising electrochemical cells and peroxymonosulfate (PMS) was investigated. Cobalt phosphide-modified carbon aerogel (Co/P/CA) was used as the cathode material owing to the high conductivity and catalytic activity of Co/P/CA. Several free radicals and their effects on organic pollutant removal were observed using electron paramagnetic resonance spectrometry and quenching experiments, respectively. The observations revealed that in the presence of O2, hydroxyl radical (·OH), superoxide (O2-·), and singlet oxygen (1O2) served as the primary active species in the PMS activation process, while in the presence of N2, ·OH and sulfate radical (SO4-·) served as the dominant active species in this process. The factor responsible for the difference in the PMS activation pathways available under O2 and N2 conditions was investigated using rotating disk electrode tests and free energy calculations. The tests indicated that O2 facilitates PMS activation to form ·OH instead of SO4-·. The dissolved oxygen subsequently underwent a single-electron-reduction reaction and was converted into O2-·, which could serve as a source of 1O2. When N2 was introduced, Co species, particularly Co(II), played a key role in activating PMS. The free radicals ·OH and SO4-· were generated during the PMS activation process. This study clearly demonstrates the mediating catalysis role of dissolved oxygen in electro-Fenton-like system through experimental data and theoretical calculations, thereby positively contributing to future studies regarding the continuous activation of peroxides in composite systems and improvement of the efficiency of waterbody remediation.

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This study investigated the effects of different external circuit loading mode on pollutants removal and power generation in microbial fuel cells (MFC). The results indicated that MFC exhibited distinct characteristics of higher maximum power density (Pmax) (named MFC-HP) and lower Pmax (named MFC-LP). And the capacitive properties of bioanodes may affect anodic electrochemistry. Reducing external load to align with the internal resistance increased Pmax of MFC-LP by 54.47 %, without no obvious effect on MFC-HP. However, intermittent external resistance loading (IER) mitigated the biotoxic effects of sulfamethoxazole (SMX) (a persistent organic pollutant) on chemical oxygen demand (COD) and NH4+-N removal and maintained high Pmax (424.33 mW/m2) in MFC-HP. Meanwhile, IER mode enriched electrochemically active bacteria (EAB) and environmental adaptive bacteria Advenella, which may reduce antibiotic resistance genes (ARGs) accumulation. This study suggested that the external circuit control can be effective means to regulate electrochemical characteristics and pollutants removal performance of MFC.

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With the rapid development of modern industry, it is urgently needed to measure the biotoxicity of complex chemicals. Microbial electrochemical biotoxicity sensors are an attractive technology; however, their application is usually limited by their stability and reusability after measurements. Here, we improve their performance by encapsulating the electroactive biofilm with polydopamine (PDA), and we evaluate the improvement by different concentrations of heavy metal ions (Cu2+, Ag+, and Fe3+) in terms of inhibition ratio (IR) and durability. Results indicate that the PDA-encapsulated sensor exhibits a more significant detection concentration than the control group, with a 3-fold increase for Cu2+ and a 1.5-fold increase for Ag+. Moreover, it achieves 15 more continuous toxicity tests than the control group, maintaining high electrochemical activity even after continuous toxicity impacts. Images from a confocal laser scanning microscope reveal that the PDA encapsulation protects the activity of the electroactive biofilm. The study, thus, demonstrates that PDA encapsulation is efficacious in improving the performance of microbial electrochemical biotoxicity sensors, which can extend its application to more complex media.

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The constructed wetland coupled with a microbial fuel cell (CW-MFC) is a wastewater treatment process that combines contaminant removal with electricity production, making it an environmentally friendly option. This hybrid system primarily relies on anaerobic bioprocesses for wastewater treatment, although other processes such as aerobic bioprocesses, plant uptake, and chemical oxidation also contribute to the removal of organic matter and nutrients. CW-MFCs have been successfully used to treat various types of wastewater, including urban, pharmaceutical, paper and pulp industry, metal-contaminated, and swine wastewater. In CW-MFC, macrophytes such as rice plants, Spartina angalica, Canna indica, and Phragmites australis are used. The treatment process can achieve a chemical oxygen demand removal rate of between 80 and 100%. Initially, research focused on enhancing power generation from CW-MFC, but recent studies have shifted towards resource recovery from wastewater. This review paper provides an overview of the development of constructed wetland microbial fuel cell technology, from its early stages to its current applications. The paper also highlights research gaps and potential directions for future research.

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Microbial electrochemical systems (MESs) rely on the microbes' ability to transfer charges from their anaerobic respiratory processes to electrodes through extracellular electron transfer (EET). To increase the generally low output signal in devices, advanced bioelectrical interfaces tend to augment this problem by attaching conducting nanoparticles, such as positively charged multiwalled carbon nanotubes (CNTs), to the base carbon electrode to electrostatically attract the negatively charged bacterial cell membrane. On the other hand, some reports point to the importance of the magnitude of the surface charge of functionalized single-walled CNTs (SWCNTs) as well as the size of functional groups for interaction with the cell membrane, rather than their polarity. To shed light on these phenomena, in this study, we prepared and characterized well-solubilized aqueous dispersions of SWCNTs functionalized by either positively or negatively charged cellulose-derivative polymers, as well as with positively charged or neutral small molecular surfactants, and tested the electrochemical performance of Shewanella oneidensis MR-1 in MESs in the presence of these functionalized SWCNTs. By simple injection into the MESs, the positively charged polymeric SWCNTs attached to the base carbon felt (CF) electrode, and as fluorescence microscopy revealed, allowed bacteria to attach to these structures. As a result, EET currents continuously increased over several days of monitoring, without bacterial growth in the electrolyte. Negatively charged polymeric SWCNTs also resulted in continuously increasing EET currents and a large number of bacteria on CF, although SWCNTs did not attach to CF. In contrast, SWCNTs functionalized by small-sized surfactants led to a decrease in both currents and the amount of bacteria in the solution, presumably due to the detachment of surfactants from SWCNTs and their detrimental interaction with cells. We expect our results will help researchers in designing materials for smart bioelectrical interfaces for low-scale microbial energy harvesting, sensing, and energy conversion applications.

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In this work, a series of 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) radicals bearing different functional groups were exploited as a simple catalyst to promote electrochemiluminescence (ECL) generation in luminol/H2O2 system. These TEMPO radicals were found to facilitate the electrochemical oxidation of H2O2 and luminol through different catalytic mechanisms, as well as the subsequent ECL generation of luminol/H2O2 system. The electrochemical oxidation and luminol ECL generation could be tuned by the functional group on the para-position of TEMPO, for which the structure/activity relationship was revealed. Finally, with the combination of enzymatic system, luminol ECL enhancement up to 9.6-fold was obtained through the catalysis of 4-hydroxyl-TEMPO. The enhanced luminol ECL allows acquiring brighter ECL images in a single-electrochemical system (SEES) for multiplex detection of cholesterol, H2O2 and glucose.

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Previous research has established a MES embedding a microbial electrode to facilitate the degradation of antibiotics in water. We modified microbial electrodes in the MES with PEDOT and rGO to enhance electron utilization on electrodes and to further promote antibiotic degradation. Density functional theory calculations on the SMX molecule indicated that the C4-S8 and S8-N27 bonds are the most susceptible to electron attack. The introduction of various functional groups and multivalent elements enhanced the electrodes' capacitance and electron mediation capabilities. This led to enhance both electron utilization on the electrodes and the removal efficiency of SMX. After 120 h, the degradation efficiency of SMX by PEDOT and rGO-modified electrodes increased by 45.47 % and 25.19 %, respectively, compared to unmodified electrodes. The relative abundance of sulfate-reducing and denitrifying bacteria significantly increased in PEDOT and rGO-modified electrodes, while the abundance of nitrifying bacteria and potential antibiotic resistance gene host microbes significantly decreased. The impact of PEDOT modification positively influenced microbial Cellular Processes, including cell growth, death, and motility. This study provides insights into the mechanisms of direct electron involvement in antibiotic degradation steps in microbial electrochemistry, and provides a possible path for improved strategies in antibiotic degradation and sustainable environmental remediation.

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To enhance the removal efficiencies of polycyclic aromatic hydrocarbons (PAHs) in sediments and to elucidate the mechanisms by which microbial electrochemical action aids in the degradation of PAHs, humic acid was used as an electron mediator in the microbial electrochemical system in this study. The results revealed that the addition of humic acids led to increases in the removal efficiencies of naphthalene, phenanthrene, and pyrene by 45.91%, 97.83%, and 85.56%, respectively, in areas remote from the anode, when compared to the control group. The investigation into the microbial community structure and functional attributes showed that the presence of humic acid did not significantly modify the microbial community composition or its functional expression at the anode. However, an examination of humic acid transformations demonstrated that humic acid extended the electron transfer range in sediment via the redox reactions of quinone and semiquinone groups, thereby facilitating the PAHs degradation within the sediment.

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Recovering ammonia nitrogen from wastewater is a sustainable strategy that simultaneously addresses both nitrogen removal and fertilizer production. Membrane electrochemical system (MES), which utilizes electrochemical redox reactions to transport ammonium ions through cation exchange membranes, has been considered as an effective technology for ammonia recovery from wastewater. In this study, we develop a mathematical model to systematically investigate the impact of co-existing ions on the transport of ammonium (NH4+) ions in MES. Our analysis elucidates the importance of pH values on both the NH4+ transport and inert ion (Na+) transport. We further comprehensively assess the system performance by varying the concentration of Na+ in the system. We find that while the inert cation in the initial anode compartment competes with NH4+ transport, NH4+ dominates the cation transport in most cases. The transport number of Na+ surpasses NH4+ only if the fraction of Na+ to total cation is extremely high (>88.5%). Importantly, introducing Na+ ions into the cathode compartment significantly enhances the ammonia transport due to the Donnan dialysis. The analysis of selective ion transport provides valuable insights into optimizing both selectivity and efficiency in ammonia recovery from wastewater.

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Recent attention on the detrimental effects of pharmaceutically active compounds (PhACs) in natural water has spurred researchers to develop advanced wastewater treatment methods. Carbamazepine (CBZ), a widely recognized anticonvulsant, has often been a primary focus in numerous studies due to its prevalence and resistance to breaking down. This study aims to explore the effectiveness of a bio-electrochemical system in breaking down CBZ in polluted water and to assess the potential harmful effects of the treated wastewater. The results revealed bio-electro degradation process demonstrated a collaborative effect, achieving the highest CBZ degradation compared to electrodegradation and biodegradation techniques. Notably, a maximum CBZ degradation efficiency of 92.01% was attained using the bio-electrochemical system under specific conditions: Initial CBZ concentration of 60 mg/L, pH level at 7, 0.5% (v/v) inoculum dose, and an applied potential of 10 mV. The degradation pathway established by identifying intermediate products via High-Performance Liquid Chromatography-Mass Spectrometry, revealed the complete breakdown of CBZ without any toxic intermediates or end products. This finding was further validated through in vitro and in vivo toxicity assays, confirming the absence of harmful remnants after the degradation process.

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A portable and integrated electrochemical detection system has been constructed for on-site and real-time detection of chemical oxygen demand (COD). The system mainly consists of four parts: (i) sensing electrode with a copper-cobalt bimetallic oxide (CuCoOx)-modified screen-printed electrode; (ii) an integrated electrochemical detector for the conversion, amplification, and transmission of weak signals; (iii) a smartphone installed with a self-developed Android application (APP) for issuing commands, receiving, and displaying detection results; and (iv) a 3D-printed microfluidic cell for the continuous input of water samples. Benefiting from the superior catalytic capability of CuCoOx, the developed system shows a high detection sensitivity with 0.335 µA/(mg/L) and a low detection limit of 5.957 mg/L for COD determination and possessing high anti-interference ability to chloride ions. Moreover, this system presents good consistency with the traditional dichromate method in COD detection of actual water samples. Due to the advantages of cost effectiveness, portability, and point-of-care testing, the system shows great potential for water quality monitoring, especially in resource-limited remote areas.

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The enhancing effects of anodes on the degradation of the organochlorine pesticide atrazine (ATR) in soil within microbial electrochemical systems (MES) have been extensively researched. However, the impact and underlying mechanisms of soil microbial electrochemical systems (MES) on ATR degradation, particularly under conditions involving the addition of humic acids (HAs), remain elusive. In this investigation, a soil MES supplemented with humic acids (HAs) was established to assess the promotional effects and mechanisms of HAs on ATR degradation, utilizing EEM-PARAFAC and SEM analyses. Results revealed that the maximum power density of the MES in soil increased by 150%, and the degradation efficiency of ATR improved by over 50% following the addition of HAs. Furthermore, HAs were found to facilitate efficient ATR degradation in the far-anode region by mediating extracellular electron transfer. The components identified as critical in promoting ATR degradation were Like-Protein and Like-Humic acid substances. Analysis of the microbial community structure indicated that the addition of HAs favored the evolution of the soil MES microbial community and the enrichment of electroactive microorganisms. In the ATR degradation process, the swift accumulation of Hydrocarbyl ATR (HYA) was identified as the primary cause for the rapid degradation of ATR in electron-rich conditions. Essentially, HA facilitates the reduction of ATR to HYA through mediated bonded electron transfer, thereby markedly enhancing the efficiency of ATR degradation.

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Seeking low-cost and eco-friendly electrode catalyst of microbial fuel cell (MFC) reactor has received extensive attention in recent decades. In this study, a sludge MFC was coupled with biochar-modified-anode (BC-300, BC-400, and BC-500) for actual brewery wastewater treatment. The physicochemical properties of biochar largely depended on the pyrolysis temperature, further affecting the removal efficiency of wastewater indicators. BC-400 MFC proved to be efficient for TN and NH4+-N removal, while the maximum removal efficiencies of COD and TP were achieved by BC-500 MFC, reaching respectively 97.14 % and 89.67 %. Biochar could promote the degradation of dissolved organic matter (DOM) in wastewater by increasing the electrochemical performances of MFC. The maximum output voltage of BC-400 MFC reached 410.24 mV, and the maximum electricity generation of 108.05 mW/m2 was also obtained, surpassing the pristine MFC (BCC-MFC) by 4.67 times. High-throughput sequencing results illustrated that the enrichment of electrochemically active bacteria (EAB) and functional bacteria (Longilinea, Denitratisoma, and Pseudomonas) in BC-MFCs, contributed to pollutants degradation and electron transfer. Furthermore, biochar affected directly the electrical conductivity of wastewater, simultaneously changing microbial community composition of MFC anode. Considering both enhanced removal efficiency of pollutants and increased power generation, the results of this study would offer technical reference for the application of biochar as MFC catalyst for brewery wastewater treatment.

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Humus substances (HSs) participate in extracellular electron transfer (EET), which is unclear in heterogeneous soil. Here, a microbial electrochemical system (MES) was constructed to determine the effect of HSs, including humic acid, humin and fulvic acid, on soil electron transfer. The results showed that fulvic acid led to the optimal electron transfer efficiency in soil, as evidenced by the highest accumulated charges and removal of total petroleum hydrocarbons after 140 days, with increases of 161% and 30%, respectively, compared with those of the control. However, the performance of MES with the addition of humic acid and humin was comparable to that of the control. Fulvic acid amendment enhanced the carboxyl content and oxidative state of dissolved organic matter, endowing a better electron transfer capacity. Additionally, the presence of fulvic acid induced an increase in the abundance of electroactive bacteria and organic degraders, extracellular polymeric substances and functional enzymes such as cytochrome c and NADH synthesis, and the expression of m tr C gene, which is responsible for EET enhancement in soil. Overall, this study reveals the mechanism by which HSs stimulate soil electron transfer at the physicochemical and biological levels and provides basic support for the application of bioelectrochemical technology in soil.

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Reducing energy consumption in conventional nitrogen removal processes is a crucial and urgent requirement. This study proposes an efficient electrode-dependent bio-electrochemical anaerobic ammonium (NH4+-N) oxidation (BE-ANAMMOX) process, employing a carbon brush as the electron acceptor and voltage of 0.8 V. The applied voltage facilitated the removal of NH4+-N with a maximum removal efficiency of 41% and a Coulombic efficiency of 40.92%, without the addition of nitrite (NO2--N). Furthermore, the NH4+-N removal efficiency demonstrated an increase corresponding to the increase in the anodic surface area. The bio-electrochemical NH4+-N removal achieved remarkable reductions, eliminating the need for O2 and NO2--N by 100%, lowering energy consumption by 67%, and reducing CO2 emissions by 66% when treating 1 kg of NH4+-N. An analysis of the microbial community revealed an increase in nitrifiers and denitrifiers, including Exiguobacterium aestuarii, Alishewanella aestuarii, Comamonas granuli, and Acinetobacter baumannii. This intricate process involved the direct conversion of NH4+-N to N2 by ANAMMOX bacteria through extracellular electron transfer, all without NO2--N. Thus, bio-electrochemical NH4+-N removal exhibits promising potential for effective nitrogen removal in wastewater treatment facilities.

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