Efficient Electroreduction of Low Nitrate Concentration via Nitrate Self-Enrichment and Active Hydrogen Inducement on the Ce(IV)-Co3O4 Cathode.

Low concentrations of nitrate (NO3-) widely exist in wastewater, post-treated wastewater, and natural environments; its further disposal is a challenge but meaningful for its discharge goals. Electroreduction of NO3- is a promising method that allows to eliminate NO3- and even generate higher-value NH3. However, the massive side reaction of hydrogen evolution has raised great obstacles in the electroreduction of low concentrations of NO3-. Herein, we present an efficient electroreduction method for low or even ultralow concentrations of NO3- via NO3- self-enrichment and active hydrogen (H*) inducement on the Ce(IV)-Co3O4 cathode. The key mechanism is that the strong oxytropism of Ce(IV) in Co3O4 resulted in two changes in structures, including loose nanoporous structures with copious dual adsorption sites of Ce-Co showing strong self-enrichment of NO3- and abundant oxygen vacancies (Ovs) inducing substantial H*. Ultimately, the bifunctional role synergistically promoted the selective conversion of NH3 rather than H2. As a result, Ce(IV)-Co3O4 demonstrated a NO3- self-enrichment with a 4.3-fold up-adsorption, a 7.5-fold enhancement of NH3 Faradic efficiency, and a 93.1% diminution of energy consumption when compared to Co3O4, substantially exceeding other reported electroreduction cathodes for NO3- concentrations lower than 100 mg·L-1. This work provides an effective treatment method for low or even ultralow concentrations of NO3-.

Merits and Limitations of Radical vs. Nonradical Pathways in Persulfate-Based Advanced Oxidation Processes.

Urbanization and industrialization have exerted significant adverse effects on water quality, resulting in a growing need for reliable and eco-friendly treatment technologies. Persulfate (PS)-based advanced oxidation processes (AOPs) are emerging as viable technologies to treat challenging industrial wastewaters or remediate groundwater impacted by hazardous wastes. While the generated reactive species can degrade a variety of priority organic contaminants through radical and nonradical pathways, there is a lack of systematic and in-depth comparison of these pathways for practical implementation in different treatment scenarios. Our comparative analysis of reaction rate constants for radical vs. nonradical species indicates that radical-based AOPs may achieve high removal efficiency of organic contaminants with relatively short contact time. Nonradical AOPs feature advantages with minimal water matrix interference for complex wastewater treatments. Nonradical species (e.g., singlet oxygen, high-valent metals, and surface activated PS) preferentially react with contaminants bearing electron-donating groups, allowing enhancement of degradation efficiency of known target contaminants. For byproduct formation, analytical limitations and computational chemistry applications are also considered. Finally, we propose a holistically estimated electrical energy per order of reaction (EE/O) parameter and show significantly higher energy requirements for the nonradical pathways. Overall, these critical comparisons help prioritize basic research on PS-based AOPs and inform the merits and limitations of system-specific applications.

Rapid Simulation of Decade-Scale Charcoal Aging in Soil: Changes in Physicochemical Properties and Their Environmental Implications.

In situ aging can change biochar properties, influencing their ecosystem benefits or risks over time. However, there is a lack of field verification of laboratory methods that attempt simulation of long-term natural aging of biochar. We exploited a decade-scale natural charcoal (a proxy for biochar) aging event to determine which lab-aging methods best mimicked field aging. We oxidized charcoal by ultraviolet A radiation (UVA), H2O2, or monochloramine (NH2Cl), and compared it to 10-year field-aged charcoal. We considered seven selected charcoal properties related to surface chemistry and organic matter release, and found that oxidation with 30% H2O2 most representatively simulated 10-year field aging for six out of seven properties. UVA aging failed to approximate oxidation levels while showing a distinctive dissolved organic carbon (DOC) release pattern. NH2Cl-aged charcoal was the most different, showing an increased persistent free radical (PFR) concentration and lower hydrophilicity. All lab oxidation techniques overpredicted polycyclic aromatic hydrocarbon release. The O/C ratio was well-correlated with DOC release, PFR concentration, surface charge, and charcoal pH, indicating the possibility to accurately predict biochar aging with a reduced suite of physicochemical properties. Overall, our rapid and verified lab-aging methods facilitate research toward derisking and enhancing long-term benefits of biochar application.

Single-Atom MnN5 Catalytic Sites Enable Efficient Peroxymonosulfate Activation by Forming Highly Reactive Mn(IV)-Oxo Species.

Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites in peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four are rarely explored, which represents a fundamental missed opportunity for coordination chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally and theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) sites more effectively activate PMS than MnN4 sites, by facilitating the cleavage of the O-O bond into high-valent Mn(IV)-oxo species with nearly 100% selectivity. The high activity of MnN5 was discerned to be due to the formation of higher-spin-state N5Mn(IV)═O species, which enable efficient two-electron transfer from organics to Mn sites through a lower-energy-barrier pathway. Overall, this work demonstrates the importance of high coordination numbers in SACs for efficient PMS activation and informs the design of next-generation environmental catalysts.

CoN1 O2 Single-Atom Catalyst for Efficient Peroxymonosulfate Activation and Selective Cobalt(IV)=O Generation.

High-valent metal-oxo (HVMO) species are powerful non-radical reactive species that enhance advanced oxidation processes (AOPs) due to their long half-lives and high selectivity towards recalcitrant water pollutants with electron-donating groups. However, high-valent cobalt-oxo (CoIV =O) generation is challenging in peroxymonosulfate (PMS)-based AOPs because the high 3d-orbital occupancy of cobalt would disfavor its binding with a terminal oxygen ligand. Herein, we propose a strategy to construct isolated Co sites with unique N1 O2 coordination on the Mn3 O4 surface. The asymmetric N1 O2 configuration is able to accept electrons from the Co 3d-orbital, resulting in significant electronic delocalization at Co sites for promoted PMS adsorption, dissociation and subsequent generation of CoIV =O species. CoN1 O2 /Mn3 O4 exhibits high intrinsic activity in PMS activation and sulfamethoxazole (SMX) degradation, highly outperforming its counterpart with a CoO3 configuration, carbon-based single-atom catalysts with CoN4 configuration, and commercial cobalt oxides. CoIV =O species effectively oxidize the target contaminants via oxygen atom transfer to produce low-toxicity intermediates. These findings could advance the mechanistic understanding of PMS activation at the molecular level and guide the rational design of efficient environmental catalysts.

Rapid Conversion of Co2+ to Co3+ by Introducing Oxygen Vacancies in Co3O4 Nanowire Anodes for Nitrogen Removal with Highly Efficient H2 Recovery in Urine Treatment.

Urine is a nitrogenous waste biomass but can be used as an appealing alternative substrate for H2 recovery. However, urine electrolysis suffers from sluggish kinetics and requires alkaline condition. Herein, we report a novel system to decompose urine to H2 and N2 under neutral conditions mediated by Cl• using oxygen-vacancy-rich Co3O4 nanowire (Ov-Co3O4) anodes and CuO nanowire cathodes. The Co2+/Co3+ cycle in Co3O4 activates Cl- in urine to Cl•, which rapidly and selectively converts urea into N2. Thus, electron transfer is boosted for H2 production, eliminating the kinetic limitations. The shuttle of Co2+ to Co3+ is the key step for Cl• yield, which is accelerated due to the introduction of Ov. Electrochemical analysis shows that Ov induces positive charge on the Co center; therefore, Co2+ loses electrons more efficiently to form Co3+. H2 production in this system reaches 716 µmol h-1, which is 320% that of non-radical-mediated urine electrolysis. The utilization of Ov-Co3O4 further enhances H2 generation, which is 490 and 210% those of noble Pt and RuO2, respectively. Moreover, urine is effectively degraded in 90 min with the total nitrogen removal of 95.4%, and N2 is the final product. This work provides new insights for efficient and low-cost recovery of H2 and urine remediation.

Ultrahigh Peroxymonosulfate Utilization Efficiency over CuO Nanosheets via Heterogeneous Cu(III) Formation and Preferential Electron Transfer during Degradation of Phenols.

In persulfate activation by copper-based catalysts, high-valent copper (Cu(III)) is an overlooked reactive intermediate that contributes to efficient persulfate utilization and organic pollutant removal. However, the mechanisms underlying heterogeneous activation and enhanced persulfate utilization are not fully understood. Here, copper oxide (CuO) nanosheets (synthesized with a facile precipitation method) exhibited high catalytic activity for peroxymonosulfate (PMS) activation with 100% 4-chlorophenol (4-CP) degradation within 3 min. Evidence for the critical role of surface-associated Cu(III) on PMS activation and 4-CP degradation over a wide pH range (pH 3-10) was obtained using in situ Raman spectroscopy, electron paramagnetic resonance, and quenching tests. Cu(III) directly oxidized 4-CP and other phenolic pollutants, with rate constants inversely proportional to their ionization potentials. Cu(III) preferentially oxidizes 4-CP rather than react with two PMS molecules to generate one molecule of 1O2, thus minimizing this less efficient PMS utilization pathway. Accordingly, a much higher PMS utilization efficiency (77% of electrons accepted by PMS ascribed to 4-CP mineralization) was obtained with CuO/PMS than with a radical pathway-dominated Co3O4/PMS system (27%) or with the 1O2 pathway-dominated α-MnO2/PMS system (26%). Overall, these results highlight the potential benefits of PMS activation via heterogeneous high-valent copper oxidation and offer mechanistic insight into ultrahigh PMS utilization efficiency for organic pollutant removal.

Quantitative structure-activity relationship for the oxidation of organic contaminants by peracetic acid using GA-MLR method.

Peracetic acid (PAA) is considered as an effective and powerful oxidant for eliminating organic contaminants in wastewater treatment. The second-order rate constant (kapp) for the reaction of PAA with organic contaminants is practically important for evaluating their removal efficiency in wastewater treatment, but only limited numbers of kapp values are available. In this study, 70 organic compounds with various structures were selected, and the kapp of PAA with each organic compound was used to develop two quantitative structure-activity relationship (QSAR) models based on three kinds of descriptors including constitutional, quantum chemical, and the PaDEL descriptors. The genetic algorithm (GA) was applied to select the molecular descriptors, then the models developed by multiple linear regression (MLR). The most important descriptors that explain the reactivity of organic compounds with PAA are the EHOMO for the model with the constitutional and quantum chemical descriptors. The maxHdsCH and minHdCH2 are two most important descriptors for the model with only PaDEL descriptors. The developed models can be used to predict kapp for a wide range of organic contaminants. The accuracy of the developed models was proved by the internal, external validation and the Y-scrambling technique. The developed QSAR models using the GA-MLR method can be used as a screening tool for predicting the elimination of organic contaminants by PAA and increasing the understanding of chemical pollutant fate.

Systematic evaluation of activated carbon-Fe3O4 composites for removing and degrading emerging organic pollutants.

In this study, a comparative activity assessment of several activated carbon (AC) and AC-Fe3O4 composites was performed to evaluate their efficiency and versatility as Fenton-like catalysts. Although many studies have demonstrated the advantages of AC-based materials as Fenton-like catalysts, most have been developed using only one oxidant and/or one pollutant. Here, untreated (AC0) and acid-treated AC (ACA) iron-oxide composites were synthesized, characterized, and compared in terms of activity to bare AC using several oxidants and pollutants, the activation efficiency of hydrogen peroxide (H2O2) and ammonium persulfate ((NH4)2S2O8), and the subsequent oxidation extent and kinetics of bisphenol-A, atrazine, and carbamazepine by the AC-based materials were studied in depth. The persulfate-based systems showed considerably higher pollutant removal in the presence of the catalysts, despite lower persulfate decomposition rates: atrazine and carbamazepine were partially degraded, mainly through a radical-dependent pathway; the highest removal of atrazine was achieved with the ACA-iron composite, whereas carbamazepine was best removed by the AC0-iron composite. In contrast, bisphenol A was completely mineralized, probably via a non-radical pathway, in the presence of all AC-based composites, even at very low persulfate concentrations. Furthermore, bisphenol A removal remained high for several consecutive cycles, with the most efficient removal and stability observed in the presence of ACA. These findings reveal the high complexity of AC-based systems, with multiple binding sites and degradation pathways unique to each combination of pollutants, catalysts, and oxidants. In general, the composition of the waste stream governs the applicability of these materials. Thus, the structure-function correlations and degradation mechanisms revealed here are crucial for improving sorbent-catalyst design and accelerating the implementation of low-cost remediation and in situ regeneration technologies.

2D N-Doped Porous Carbon Derived from Polydopamine-Coated Graphitic Carbon Nitride for Efficient Nonradical Activation of Peroxymonosulfate.

Nitrogen-doped carbon materials attract broad interest as catalysts for peroxymonosulfate (PMS) activation toward an efficient, nonradical advanced oxidation process. However, synthesis of N-rich carbocatalysts is challenging because of the thermal instability of desirable nitrogenous species (pyrrolic, pyridinic, and graphitic N). Furthermore, the relative importance of different nitrogenous configurations (and associated activation mechanisms) are unclear. Herein, we report a "coating-pyrolysis" method to synthesize porous 2D N-rich nanocarbon materials (PCN-x) derived from dopamine and g-C3N4 in different weight proportions. PCN-0.5 calcined at 800 °C had the highest surface area (759 m2/g) and unprecedentedly high N content (18.5 at%), and displayed the highest efficiency for 4-chlorophenol (4-CP) degradation via PMS activation. A positive correlation was observed between 4-CP oxidation rates and the total pyridinic and pyrrolic N content. These N dopants serve as Lewis basic sites to facilitate 4-CP adsorption on the PCN surface and subsequent electron-transfer from 4-CP to PMS, mediated by surface-bound complexes (PMS-PCN-0.5). The main degradation products were chlorinated oligomers (mostly dimeric biphenolic compounds), which adsorbed to and deteriorated the carbocatalyst. Overall, this study offers new insights for rational design of nitrogen-enriched carbocatalysts, and advances mechanistic understanding of the critical role of N species during nonradical PMS activation.

Efficient SO2 Removal and Highly Synergistic H2O2 Production Based on a Novel Dual-Function Photoelectrocatalytic System.

The direct conversion of SO2 to SO3 is rather difficult for flue gas desulfurization due to its inert dynamic with high reaction activation energy, and the absorption by wet limestone-gypsum also needs the forced oxidation of O2 to oxidize sulfite to sulfate, which is necessary for additional aeration. Here, we propose a method to remove SO2 with highly synergistic H2O2 production based on a novel dual-function photoelectrocatalytic (PEC) system in which the jointed spontaneous reaction of desulfurization and H2O2 production was integrated instead of nonspontaneous reaction of O2 to H2O2. SO2 was absorbed by alkali liquor then oxidized quickly into SO42- by a nanorod α-Fe2O3 photoanode, which possessed high alkali corrosion resistance and electron transport properties. H2O2 was produced simultaneously in the cathode chamber on a gas diffusion electrode and was remarkably boosted by the conversion reaction of SO32- to SO42- in the anode chamber in which the released chemical energy was effectively used to increase H2O2. The photocurrent density increased by 40% up to 1.2 mA·cm-2, and the H2O2 evolution rate achieved 58.8 µmol·L-1·h-1·cm-2 with the synergistic treatment of SO2, which is about five times than that without SO2. This proposed PEC cell system offers a cost-effective and environmental-benign approach for dual purpose of flue gas desulfurization and simultaneous high-valued H2O2 production.

Sunlight-Mediated Lead and Chromium Release from Commercial Lead Chromate Pigments in Aqueous Phase.

Lead chromate pigments are included in a group of the most widely used pigments, which account for 3% of worldwide lead consumption. This study reports the photoactivity of commercial lead chromate pigment (i.e., chrome yellow) under simulated sunlight. It underwent photodissolution in the presence of organic acid and dissolved organic matter in the aqueous phase, releasing Pb(II) and Cr(III). Pb(II) was released more readily than Cr(III) which mainly formed hydroxides and oxides. The photodissolution can be activated by light with a wavelength <514 nm. The reaction is mediated by the reduction of Cr(VI) in the pigment by self-generated electrons. The kinetics were mainly affected by the electron-hole separation efficiency which can be enhanced by electron donors. The reaction rate decreases with increasing solution pH as the photodissolution process consumes protons. The photodissolution of the chrome yellow pigment was further confirmed in a river water sample under natural sunlight, with 11.28% of lead and 2.56% of chromium released in 7 h. This study highlights the importance of considering photochemical processes in risk assessments and regulations of commercial semiconductor pigments, which are currently based on their solubility.

Selenium and nitrogen co-doped carbon quantum dots as a fluorescent probe for perfluorooctanoic acid.

Highly fluorescent carbon quantum dots co-doped with selenium and nitrogen  (SeN-CQDs) were fabricated via a one-pot hydrothermal route using selenomethionine as the sole precursor. The SeN-CQDs aggregates have sizes between 30 and 45 nm and display blue fluorescence with a quantum yield of 8% at excitation/emission wavelengths of 350/445 nm. The fluorescence is pH dependent and decreases under acidic conditions. The doping of the CQDs with selenium and nitrogen was proven by X-ray photoelectron spectroscopy (XPS). Fluorescence is selectively quenched by perfluorooctanoic acid (PFOA), and this is accompanied by a decreased fluorescence lifetime. Quenching is not due to aggregation in view of the unaltered sizes of nanoparticles as revealed by TEM and DLS analyses. UV-vis absorption titration suggested the formation of an excited state complex between SeN-CQDs and PFOA, and quenching originates from the internal electron transfer in the excited state complex. The method was used to detect PFOA quantitatively in the linear range of 10-70 µM with a 1.8 µM detection limit. The nanoprobe has a high selectivity for PFOA over potentially interfering molecules. The practicability of the method was ascertained by accurate detection of PFOA in real samples by the standard addition method. The method may be further improved by tuning the interaction between PFOA and SeN-CQDs through optimizing the doping and the surface composition of the SeN-CQDs. Graphical abstract Schematic presentation of a fluorometric method for perfluorooctanoic acid detection by using a selenium and nitrogen co-doped carbon quantum dots as the fluorescent probe.

Novel Composite Electrodes for Selective Removal of Sulfate by the Capacitive Deionization Process.

Capacitive deionization (CDI) can remove ionic contaminants from water. However, concentrations of background ions in water are usually much higher than target contaminants, and existing CDI electrodes have no designed selectivity toward specific contaminants. In this study, we demonstrate a selective CDI process tailored for removal of SO42- using activated carbon electrodes modified with a thin, quaternary amine functionalized poly(vinyl alcohol) (QPVA) coating containing submicron sized sulfate selective ion exchange resin particles. The resin/QPVA coating exhibited strong selectivity for SO42- at Cl-: SO42- concentration ratios up to 20:1 by enabling preferential transport of SO42- through the coating, but had no negative impact on the electrosorption kinetics when the coating thickness was small. The cationic nature of the coating also significantly improved the charge efficiency and consequently the total salt adsorption capacity of the electrode by 42%. The resin/QPVA coated CDI system was stable, showing highly reproducible performance in more than 50 adsorption and desorption cycles. This work suggests that addition of selective ion exchange resins on the surface of a carbon electrode could be a generally applicable approach to achieve selective removal of target ions in a CDI process.

Phosphate Changes Effect of Humic Acids on TiO2 Photocatalysis: From Inhibition to Mitigation of Electron-Hole Recombination.

A major challenge for photocatalytic water purification with TiO2 is the strong inhibitory effect of natural organic matter (NOM), which can scavenge photogenerated holes and radicals and occlude ROS generation sites upon adsorption. This study shows that phosphate counteracts the inhibitory effect of humic acids (HA) by decreasing HA adsorption and mitigating electron-hole recombination. As a measure of the inhibitory effect of HA, the ratios of first-order reaction rate constants between photocatalytic phenol degradation in the absence versus presence of HA were calculated. This ratio was very high, up to 5.72 at 30 mg/L HA and pH 4.8 without phosphate, but was decreased to 0.76 (5 mg/L HA, pH 8.4) with 2 mM phosphate. The latter ratio indicates a surprising favorable effect of HA on TiO2 photocatalysis. FTIR analyses suggest that this favorable effect is likely due to a change in the conformation of adsorbed HA, from a multiligand exchange arrangement to a complexation predominantly between COOH groups in HA and the TiO2 surface in the presence of phosphate. This configuration can reduce hole consumption and facilitate electron transfer to O2 by the adsorbed HA (indicated by linear sweep voltammetry), which mitigates electron-hole recombination and enhances contaminant degradation. A decrease in HA surface adsorption and hole scavenging (the predominant inhibitory mechanisms of HA) by phosphate (2 mM) was indicated by a 50% decrease in the photocatalytic degradation rate of HA and 80% decrease in the decay rate coefficient of interfacial-related photooxidation in photocurrent transients. These results, which were validated with other compounds (FFA and cimetidine), indicate that anchoring phosphate - or anions that exert similar effects on the TiO2 surface - might be a feasible strategy to counteract the inhibitory effect of NOM during photocatalytic water treatment.

Selective Degradation of Organic Pollutants Using an Efficient Metal-Free Catalyst Derived from Carbonized Polypyrrole via Peroxymonosulfate Activation.

Metal-free carbonaceous materials, including nitrogen-doped graphene and carbon nanotubes, are emerging as alternative catalysts for peroxymonosulfate (PMS) activation to avoid drawbacks of conventional transition metal-containing catalysts, such as the leaching of toxic metal ions. However, these novel carbocatalysts face relatively high cost and complex syntheses, and their activation mechanisms have not been well-understood. Herein, we developed a novel nitrogen-doped carbonaceous nanosphere catalyst by carbonization of polypyrrole, which was prepared through a scalable chemical oxidative polymerization. The defective degree of carbon substrate and amount of nitrogen dopants (i.e., graphitic nitrogen) were modulated by the calcination temperature. The product carbonized at 800 °C (CPPy-F-8) exhibited the best catalytic performance for PMS activation, with 97% phenol degradation efficiency in 120 min. The catalytic system was efficient over a wide pH range (2-9), and the reaction of phenol degradation had a relatively low activation energy (18.4 ± 2.7 kJ mol-1). The nitrogen-doped carbocatalyst activated PMS through a nonradical pathway. A two-step catalytic mechanism was extrapolated: the catalyst transfers electrons to PMS through active nitrogen species and becomes a metastable state of the catalyst (State I); next, organic substrates are oxidized and degraded by serving as electron donors to reduce State I. The catalytic process was selective toward degradation of various aromatic compounds with different substituents, probably depending on the oxidation state of State I and the ionization potential (IP) of the organics; that is, only those organics with an IP value lower than ca. 9.0 eV can be oxidized in the CPPy-F-8/PMS system.

Sunlight Promotes Fast Release of Hazardous Cadmium from Widely-Used Commercial Cadmium Pigment.

Cadmium pigments are widely used in the polymer and ceramic industry. Their potential environmental risk is under debate, being the major barrier for appropriate regulation. We show that 83.0 ± 0.2% of hazardous cadmium ion (Cd2+) was released from the commercial cadmium sulfoselenide pigment (i.e., cadmium red) in aqueous suspension within 24 h under simulated sunlit conditions. This photodissolution process also generated sub-20 nm pigment nanoparticles. Cd2+ release is attributed to the reactions between photogenerated holes and the pigment lattices. The photodissolution process can be activated by both ultraviolet and visible light in the solar spectrum. Irradiation under alkaline conditions or in the presence of phosphate and carbonate species resulted in reduced charge carrier energy or the formation of insoluble and photostable cadmium precipitates on pigment surfaces, mitigating photodissolution. Tannic acid inhibited the photodissolution process by light screening and scavenging photogenerated holes. The fast release of Cd2+ from the pigment was further confirmed in river water under natural sunlight, with 38.6 ± 0.1% of the cadmium released within 4 h. Overall, this study underscores the importance to account for photochemical effects to inform risk assessments and regulations of cadmium pigments which are currently based on their low solubility.

Turn-on fluorometric and colorimetric probe for hydrogen peroxide based on the in-situ formation of silver ions from a composite made from N-doped carbon quantum dots and silver nanoparticles.

The authors describe a fluorometric and colorimetric nanoprobe for H2O2. The detection scheme is based on the in-situ formation of silver(I) ions from a composite consisting of nitrogen-doped carbon quantum dots (N-CQDs) and silver nanoparticles (AgNPs). A drastic change occurs both in fluorescence and color of the solution of the N-CQD/AgNPs composite. The fluorescence of composite (with excitation/emission peaking at 320/384 nm) is enhanced on increasing the concentration of H2O2 due to the oxidation of silver metal in the N-CQD/AgNPs to form Ag(I) ions. The latter undergo strong coordination with the nitrogen atoms of the N-CQDs. In-situ formation of Ag(I) ions further results in a change in color of the solution from pale yellow (with a peak at 408 nm) to colorless. Under optimized conditions, the probe gives a fluorometric and colorimetric response in the 10 to 50 µM H2O2 concentration range with a 4.7 µM limit of detection. The probe is highly selective over several potentially interfering ions and agents. It was successfully applied to the determination of H2O2 in spiked samples without prior treatment. Graphical abstract Graphical presentation for specific detection of H2O2 based on the in-situ formation of Ag(I) ions from a composite consisting of silver nanoparticles and nitrogen-doped carbon quantum dots.