N-doped Cu2O with the tunable Cu0 and Cu+ sites for selective CO2 electrochemical reduction to ethylene.

The electrochemical carbon dioxide reduction reaction (CO2RR) to high value-added fuels or chemicals driven by the renewable energy is promising to alleviate global warming. However, the selective CO2 reduction to C2 products remains challenge. Cu-based catalyst with the specific Cu0 and Cu+ sites is important to generate C2 products. This work used nitrogen (N) to tune amounts of Cu0 and Cu+ sites in Cu2O catalysts and improve C2-product conversion. The controllable Cu0/Cu+ ratio of Cu2O catalyst from 0.16 to 15.19 was achieved by adjusting the N doping amount using NH3/Ar plasma treatment. The major theme of this work was clarifying a volcano curve of the ethylene Faraday efficiency as a function of the Cu0/Cu+ ratio. The optimal Cu0/Cu+ ratio was determined as 0.43 for selective electroreduction CO2 to ethylene. X-ray spectroscopy and density functional theory (DFT) calculations were employed to elucidate that the strong interaction between N and Cu increased the binding energy of NCu bond and stabilize Cu+, resulting in a 92.3% reduction in the potential energy change for *CO-*CO dimerization. This study is inspiring in designing high performance electrocatalysts for CO2 conversion.

Role of urea in the retention of DON in soil by clay minerals: Analysis based upon molecular weight.

As a widely used fertilizer, urea significantly promotes the leaching of dissolved organic nitrogen (DON) in soils and aggravates nitrogen contamination in groundwater. Clay minerals are considered the most important factor in retaining DON. However, the effect of urea on the retention of DON with different molecular weights by clay minerals is unknown. In this study, the retention of both low-molecular weight DON (LMWD) and high-molecular weight DON (HMWD) by clay minerals in the presence of urea was investigated. For this purpose, batch adsorption and soil column leaching experiments, characterization analysis (Fourier transform infrared spectroscopy X-ray diffraction, and X-ray photoelectron spectroscopy), and molecular dynamics simulations were carried out. Urea had a positive effect on the adsorption of LMWD, whereas a competitive effect existed for the adsorption of HMWD. The dominant interactions among DON, urea, and clay minerals included H-bonding, ligand exchange, and cation exchange. The urea was preferentially adsorbed on clay minerals and formed a complex, which provided more adsorption sites to LMWD and only a few to HMWD. The presence of urea increased the retention of LMWD and decreased the retention of HMWD in clay minerals. The retention capacity of LMWD increased by 6.9%-12.8%, while that of HMWD decreased by 6.7%-53.1%. These findings suggest that LMWD tended to be trapped in soils, while HMWD was prone to be leached into groundwater, which can be used to evaluate the leaching of DON from soil to groundwater.

Optimization of nitrogen-doped sludge char preparation and mechanism study for catalytic oxidation of NO at room temperature.

Catalytic oxidation of NO at room temperature was carried out over nitrogen (N)-doped sludge char (SC) prepared from pyrolysis of municipal sewage sludge, and urea was adopted as nitrogen source. The effects of different N-doping methods (one-step and two-step method), dried sludge (DS)/urea mass ratios (5:1, 4:1, 3:1, 2:1, and 1:1), SC preparation procedures (pyrolysis only, pyrolysis with acid washing, and pyrolysis with KOH activation and acid washing), and different pyrolysis temperatures (500, 600, 700, and 800°C) on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation. The results indicated that N-doping could obviously promote the catalytic performance of SC. The one-step method with simultaneous sludge pyrolysis (at 700°C), KOH activation, and N-doping (DS/urea of 3:1) was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%, whereas the optimal NO conversion rate of SC without N-doping was only 47.3%. Urea worked both as carbon and nitrogen source, which could increase about 2.9%-16.5% of carbon and 24.8%-42.7% of nitrogen content in SC pyrolyzed at 700°C. N-doping significantly promoted microporosity of SC. The optimal N-doped SC showed specific surface areas of 571.38 m2/g, much higher than 374.34 m2/g of the optimal SC without N-doping. In addition, N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups. Finally, three reaction paths, i.e. microporous reactor, active sites, and basic site control path, were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.

Fluorescent probes based on N-CQDs: For direct detection of food additives STPP and Al3.

Sodium tripolyphosphate (STPP), as one of the many food additives, can cause gastrointestinal discomfort and a variety of adverse reactions when ingested by the human body, which is a great potential threat to human health. Therefore, it is necessary to develop a fast, sensitive and simple method to detect STPP in food. In this study, we synthesized a kind of nitrogen-doped carbon quantum dots (N-CQDs), and were surprised to find that the addition of STPP led to the gradual enhancement of the emission peaks of the N-CQDs, with a good linearity in the range of 0.067-1.96 µM and a low detection limit as low as 0.024 µM. Up to now, there is no report on the use of carbon quantum dots for the direct detection of STPP. Meanwhile, we found that the addition of Al3+ effectively bursts the fluorescence intensity of N-CQDs@STPP solution and has a good linear relationship in the range of 0.33-6.25 µM with a lower detection limit of 0.24 µM. To this end, we developed a fluorescent probe to detect STPP and Al3+. In addition, the probe was successfully applied to the detection of bread samples, which has great potential for practical application.

Construction of a one-stop N-doped negatively charged carbon dot nanoplatform with antibacterial and anti-inflammatory dual activities for wound infection based on biocompatibility.

The development of bacterial resistance significantly contributes to the persistence of infections. Although previous studies have highlighted the benefits of metal-doped positive carbon nanodots in managing bacterial wound infections, their mechanism of action is relatively simple and they may pose potential hazards to human cells. Therefore, it is essential to develop a one-stop carbon dot nanoplatform that offers high biocompatibility, antibacterial properties, and anti-inflammatory activities for wound infection management. This study explores the antibacterial efficacy, without detectable resistance, and wound-healing potential of nitrogen-doped (N-doped) negatively charged carbon dots (TPP-CDs). These carbon dots are synthesized using tannic acid (TA), polyethylene polyamine, and polyethylene glycol (PEG) as precursors, with a focus on their biocompatibility. Numerous systematic studies have shown that TPP-CDs can effectively destroy bacterial biofilms and deoxyribonucleic acid (DNA), while also inducing oxidative stress, leading to a potent antimicrobial effect. TPP-CDs also demonstrate the ability to scavenge excess free radicals, promote cellular proliferation, and inhibit inflammatory factors, all of which contribute to improved wound healing. TPP-CDs also demonstrate favorable cell imaging capabilities. These findings suggest that N-doped negatively charged TPP-CDs hold significant potential for treating bacterial infections and offer practical insights for their application in the medical field.

A comparative study on the formation of nitrogen-containing organic compounds in cloud droplets and aerosol particles.

Nitrogen-containing organic compounds (NOCs) may potentially contribute to aqueous secondary organic aerosols, yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear. With the in-situ measurements performed at a mountain site (1690 m a.s.l.) in southern China, we investigated the formation of NOCs in the cloud droplets and the cloud-free particles, based on their mixing state information of NOCs-containing particles by single particle mass spectrometry. The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual (cloud RES) particles. NOCs were highly correlated with carbonyl compounds (including glyoxalate and methylglyoxal) in the cloud-free particles, however, limited correlation was observed for cloud RES particles. Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles, rather than in the cloud RES particles. The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols, rather than cloud droplets. In addition, we have identified the transport of biomass burning particles that facilitate the formation of NOCs, and that the observed NOCs is most likely contributed to the light absorption. These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.

Adsorption of Carbon Dioxide and Nitrogen in Co3(ndc)3(dabco) Metal-Organic Framework.

Metal-organic frameworks (MOFs) are promising materials for processes such as carbon dioxide (CO2) capture or its storage. In this work, the adsorption of CO2 and nitrogen (N2) in Co3(ndc)3(dabco) MOF (ndc: 2,6-naphthalenedicarboxylate; dabco: 1,4-diazabicyclo[2.2.2]octane) is reported for the first time over the temperature range of 273-323 K and up to 35 bar. The adsorption isotherms are successfully described using the Langmuir isotherm model. The heats of adsorption for CO2 and N2, determined through the Clausius-Clapeyron equation, are 20-27 kJ/mol and 10-11 kJ/mol, respectively. The impact of using pressure and/or temperature swings on the CO2 working capacity is evaluated. If a flue gas with 15% CO2 is fed at 6 bar and 303 K and regenerated at 1 bar and 373 K, 1.58 moles of CO2 can be captured per kg of MOF. The analysis of the multicomponent adsorption of typical flue gas streams (15% CO2 balanced with N2), using the ideal adsorbed solution theory (IAST), shows that at 1 bar and 303 K, the CO2/N2 selectivity is 11.5. In summary, this work reports essential data for the design of adsorption-based processes for CO2 capture using a Co3(ndc)3(dabco) MOF, such as pressure swing adsorption (PSA).

Development and CO2 capture of nitrogen-enriched microporous carbon by coupling waste polyamides with lignocellulosic biomass.

Due to the substantial emissions of global CO2, there has been growing interest in nitrogen-enriched porous carbonaceous materials that possess exceptional CO2 capture capabilities. In this study, a novel N-enriched microporous carbon was synthesized by integrating waste polyamides with lignocellulosic biomass, involving carbonization and physicochemical activation. As-synthesized adsorbents demonstrated significant characteristics including a high specific surface area (1710 m2/g) and a large micropore volume (0.497 cm3/g), as well as abundant N- and O-containing functional groups, achieved through activation at 700 °C. They displayed remarkable CO2 capture capability, achieving uptake levels of up to 6.71 mmol/g at 1 bar and 0 °C, primarily due to the filling effect of narrow micropore along with electrostatic interaction. Furthermore, the adsorbent exhibited a rapid capacity for CO2 capture, achieving 94.9% of its saturation capacity within a mere 5 min at 30 °C. This impressive performance was accurately described by the pseudo second-order dynamic model. Additionally, as-synthesized adsorbents displayed a moderate isosteric heat of CO2 adsorption, as well as superior selectivity over N2. Even after undergoing five consecutive cycles, it maintained ∼100% of its initial capacity. Undoubtedly, such findings hold immense significance in the mitigation of global plastic pollution and greenhouse effect.

Microalgae realizes self N-doped biochar for heavy metal polluted sediment remediation.

Heavy metal contamination in sediment has become a significant global environmental challenge. Numerous studies have demonstrated the effectiveness of modified biochar to solve heavy metal contamination in sediment. However, the modification process with complex methods and expensive modifiers prevented its large-scale application. In this study, an N self-doped biochar was obtained by pyrolysis of Spirulina sp. (SBC). Meanwhile, the K2CO3 impregnation method was utilized to prepare Spirulina sp. biochar (KSBC), which demonstrated a higher specific surface area (874 m2/g) and richer O, N functional groups. The adsorption capacity of KSBC550-120 for Cu (Ⅱ), Zn (Ⅱ), and Cd (Ⅱ) was 57.9 ± 0.3 mg/g, 43.6 ± 0.7 mg/g, and 63.9 ± 0.6 mg/g, respectively. The adsorption process is primarily governed by chemical processes, mainly through ion exchange, surface complexation, dissolution-precipitation, electrostatic interactions, adsorption-reduction, and cation-π interactions. Moreover, utilizing KSBC550-120 for mixing or capping effectively reduced heavy metal concentrations in both the overlying and pore water of the sediments. 1.0 wt% KSBC550-120 with capping treatment significantly reduced the release of heavy metals from the sediment by 80.3-91.9%. This study provides effective theoretical support for re-utilizing waste algal residues and remediation of the heavy metal-contaminated river and lake sediments using microalgae biochar.

Copper and nitrogen-doped carbon quantum dots as green nano-probes for fluorimetric determination of delafloxacin; characterization and applications.

BACKGROUND: Carbon quantum dots (CQDs) have gained much interest recently for being efficient probes. Their cost-effectiveness, eco-friendliness, and unique photocatalytic activities made them distinctive alternatives to other luminescent approaches like fluorescent dyes and luminous derivatization. Meanwhile, delafloxacin (DLF) is a recently approved antibacterial medicine. DLF has been authorized for the treatment of soft-tissue and skin infections as well as pneumonia. Therefore, new eco-friendly, cost-effective, and sensitive tools are needed its estimation in different matrices. RESULTS: In the proposed study, green copper and nitrogen carbon dots (Cu-N@CDs) were synthesized from a green source (plum juice with copper sulphate). Cu-N@CQDs were then characterized using multiple tools including X-ray photon spectroscopy (XPS), FTIR and UV-VIS spectroscopy, Zeta potential measurements, High-resolution transmission electron microscopy (HRTEM), and fluorescence spectroscopy. After gradually adding DLF, the developed quantum dots' fluorescence was significantly enhanced within the working range of 0.5-100.0 ng mL-1. The limits of detection and quantification were 0.08 and 0.27 ng mL-1, respectively. The accuracy of the proposed method ranged from 96.00 to 99.12 % in recovery%, when recovered from milk and plasma samples. SIGNIFICANCE: Cu-N@CDs were utilized and validated for selectively determining DLF in several matrices including pharmaceutical forms, human plasma and in milk samples using spectrofluorimetric technique. The bio-analytical method is simple and could be used in content uniformity testing as well as in therapeutic drug monitoring in human plasma.

High speed enrichment of benzoylurea insecticides by hierarchical pore nitrogen doped carbon materials induced with hydrogen-bonded organic frameworks.

The high speed enrichment of benzoylurea insecticides (BUs) in complex matrices is an essential and challenging step. The present study focuses on the synthesis of a hierarchical pore nitrogen-doped carbon material for magnetic solid phase extraction (MSPE) of BUs. This material was prepared through the carbonization of a composite material ZIF-67@MCA which assembly with hydrogen-bonded organic frameworks (melamine-cyanurate, MCA) and zeolitic imidazolate framework (ZIF-67) at room temperature. The optimal adsorption effect is achieved when the mass ratio of ZIF-67 to MCA is 1/3, and the carbonization was performed at 600 °C, the such obtained carbon material was denoted as 1/3ZIF-67@MCA-DCs-600. The material was characterized with various physical methods including X-ray diffractometry (XRD), Fourier transform infrared spectrometry (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM), Brunauer-Emmett-Teller (BET), vibrating sample magnetometer (VSM), water contact angle measurement, Raman spectrometry. 1/3ZIF-67@MCA-DCs-600 exhibits a macro-mesoporous 3D structure with a high degree of nitrogen doping and relatively large specific surface area, making it suitable for magnetic solid phase extraction (MSPE). The adsorption of BUs with concentration of 100 ng mL-1 can reach equilibrium within 5 s. The interaction between BUs and the adsorbent, facilitated by π-π stacking, hydrophobic interactions, hydrogen bonding forces, as well as the material's porosity, enables efficient extraction recoveries ranging from 45 % to 92 %. The enrichment of BUs was achieved through the establishment of an MSPE method under optimized conditions, which was further coupled with high performance liquid chromatography (HPLC) for the determination of the four BUs. The linear range spans from 5 ng ml-1 to 1000 ng ml-1 with the correlation coefficient (R2) of ≥ 0.99, Meanwhile, the detection limit for these four BUs falls within the range of 0.01 to 0.10 ng ml-1. The material exhibits good reusability and can be reused for at least 5 cycles. Inter day and intra-day precision ranges from 2.1-7.9 % and 1.0-5.4 %, respectively. The method demonstrates a high level of reliability in practical applications for the determination of BUs.

Regulation of warming on the mixed decomposition of Artemisia ordosica and Leymus secalinus litter in Mu Us Desert, China is time-dependent.

Warming drives material cycling in terrestrial ecosystems by affecting litter decomposition, as it can alter litter yield, quality and decomposer composition and activity. The effect of warming on the decomposition of mixed litter in arid and semi-arid zones remains unknown. We investigated the mass loss and nutrient release dynamics during 450 days of decomposition of Artemisia ordosica, Leymus secalinus, and their mixture in Mu Us Desert by open-top chambers and litter bags. The results showed interspecific differences in the responses to warming, in that warming promoted mass loss and N and P release from L. secalinus and inhibited mass loss and P but promoting N release from A. ordosica. Mixing of A. ordosica and L. secalinus litter inhibited decomposition. Warming enhanced the antagonistic effects of mixed decomposition. The total mass loss of mixed litter was decreased by 9%, and the release of N and P was decreased by 4.9% and 12.6%, respectively. The antagonistic effects of mixed litter mass loss and P release under the warming treatment gradually strengthened with time, with N release changing from a synergistic to an antagonistic effect at 150 d. The non-additive effects produced by the mixed decomposition of A. ordosica and L. secalinus litter were jointly regulated by temperature and time. Future research on mixed litter decomposition should consider the interaction between temperature and time.

Nitrogen-doped MoS2 QDs as fluorescent probes for sensitive detection of curcumin and cell imaging.

BACKGROUND: Curcumin has been used in traditional medicine because of its pharmacological activity, including antioxidant, antibacterial, anticancer, and anticarcinogenic properties. Therefore, sensitive and selective monitoring of curcumin is highly demand for practical application. RESULTS: In this study, we describe the construction of a fluorescence method for curcumin assay based on nitrogen-doped MoS2 quantum dots (N-MoS2 QDs). The N-MoS2 QDs are constructed by a solvothermal method using sodium molybdate and Cys as precursors. With the addition of curcumin, the bright blue fluorescence of N-MoS2 QDs is quenched by the inner filter effect (IFE). The QDs emitted bright blue fluorescence and could be quenched by the addition of curcumin via IFE. The dynamic range is the range of 0.1-10 µM for curcumin detection, with a detection limit of 59 nM. N-MoS2 QDs were applied for curcumin assay in real samples with good recovery. In addition, the N-MoS2 QDs exhibited relative low cytotoxicity and could be applied for fluorescence-based imaging in biological samples. SIGNIFICANCE: Our study indicates that the sensor possesses good selectivity to monitor curcumin in water samples, human urine samples, ginger powder samples, mustard samples, and curry samples with satisfactory recoveries. The N-MoS2 QDs possess less cytotoxicity with excellent biocompatibility and were applied for in vitro cell imaging.

The Facile Production of p-Chloroaniline Facilitated by an Efficient and Chemoselective Metal-Free N/S Co-Doped Carbon Catalyst.

The catalytic hydrogenation of the toxic and harmful p-chloronitrobenzene to produce the value-added p-chloroaniline is an essential reaction for the sustainable chemical industry. Nevertheless, ensuring satisfactory control of its chemoselectivity is a great challenge. In this work, a N/S co-doped metal-free carbon catalyst has been fabricated by using cysteine as a source of C, N, and S. The presence of calcium citrate (porogen agent) in the mixture subjected to pyrolysis provided the carbon with porosity, which permitted us to overcome the issues associated with the loss of heteroatoms during an otherwise necessary activation thermal treatment. Full characterization was carried out and the catalytic performance of the metal-free carbon material was tested in the hydrogenation reaction of p-chloronitrobenzene to selectively produce p-chloroaniline. Full selectivity was obtained but conversion was highly dependent on the introduction of S due to the synergetic effect of S and N heteroatoms. The N/S co-doped carbon (CYSCIT) exhibits a mesoporous architecture which favors mass transfer and a higher doping level, with more exposed N and S doping atoms which act as catalytic sites for the hydrogenation of p-chloronitrobenzene, resulting in enhanced catalytic performance when compared to the N-doped carbon obtained from melamine and calcium citrate (MELCIT) used as a reference.

Real-Time and Wireless Transmission of a Nitrogen-Doped Ti3C2Tx Wearable Gas Sensor for Efficient Detection of Food Spoilage and Ammonia Leakage.

With the rising popularity of smart homes, there is an urgent need for devices that can perform real-time online detection of ammonia (NH3) concentrations for food quality measurement. In addition, timely warning is crucial to preventing individual deaths from NH3. However, few studies can realize continuous monitoring of NH3 with high stability and subsequent application validation. Herein, we report on an integrated device equipped with a nitrogen-doped Ti3C2Tx gas sensor that shows great potential in detecting food spoilage and NH3 leakage. The nitrogen doping results in the lattice misalignment of Ti3C2Tx, subsequently realizing effective barrier height modulation and enhanced charge transfer efficiency of nitrogen-doped Ti3C2Tx. Density functional theory calculations confirm the greatly enhanced adsorption of NH3 on nitrogen-doped Ti3C2Tx. Our work can inspire the design of efficient gas sensors for real-time and wireless detection of food spoilage and NH3 leakage.

Interaction and band structure-determined inhibition of negative Cr (VI) and positive Fe (III) for antibiotic photodegradation by nitrogen-doped dissolved black carbon.

The influences of the positive Fe3+ and the negative Cr2O72- on the tetracycline (TC) photodegradation by N-doped dissolved black carbon (NDBC) have been investigated in this work. A series of samples (NDBC300, NDBC400 and NDBC500) have been extracted from the corresponding biochar. NDBC400 has the best photodegradation performance (79%) for TC under visible light irradiation. Adding Cr2O72- and Fe3+ can reduces TC photodegradation efficiency into 37% and 53%, respectively. This maybe from that Cr2O72- has stronger interaction with NDBC400 than Fe3+ since it can quench more fluorescence intensity of NDBC400 than Fe3+. Furthermore, Cr2O72- can reduce the steady-state concentration of 3NDBC400*, 1O2 and •OH, whereas Fe3+can just reduce the steady-state concentration of 3NDBC400* and increase the concentration of •OH. This may explain why Cr2O72- has stronger inhibit performance of TC photodegradation by NDBC400 than Fe3+. The band structures of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- are constructed. And the VB of NDBC400-Fe3+ has a stronger ability to produce •OH than NDBC400. In summary, coupling interaction and band structure characterization of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- can explain well why Cr2O72 has stronger inhibition effect than Fe3+ and Fe3+ can increase the concentration of •OH. This work provides a deep insight for the photochemical behavior of dissolved black carbon and the transformation behavior of the co-existed metal ions and antibiotics.

Using ligand regulation, metal replacement, and ligand doping strategies on Zr-FUM to improve methane separation from coalbed gas.

Developing adsorbents suitable for industrial applications that can effectively enhance the separation of methane (CH4) from nitrogen (N2) in coalbed gas is crucial to improve energy recovery and mitigate greenhouse gas emissions. In this study, three modification strategies were implemented on Zr-FUM, including ligand regulation, metal replacement, and ligand doping, to synthesize Zr-FDCA, Al-FUM, and Zr-FUM-FA, with the aim of improving the performance of CH4/N2 separation under humid conditions. The results demonstrated that the promotion of robust orbital overlap and strengthened electrovalent bonding on adsorbents can selectively enhance CH4 adsorption. As a result, Zr-FUM-FA achieved a saturated CH4 adsorption capacity of 1.37 mmol/g, a CH4 working window of 307 s, and a CH4/N2 sorbent selection parameter (Ssp) of 47.31, exceeding the performance of most reported adsorbents. Analyses of the pore structure, surface morphology, and functional groups revealed that the presence of an ultramicropore proximity to CH4, reduced static resistance, and enhanced electrovalent bond were key factors for CH4 separation. Grand Canonical Monte Carlo and Density Functional Theory studies indicated that the introduction of -C-H- in FA played a crucial role in enhancing CH4 adsorption. Optimization of adsorption parameters using the Aspen adsorption package showed that in a dual-adsorbent bed system, the recovery and purity of CH4 in Zr-FUM-FA reach 99.5% and 97.3%, respectively, providing important theoretical support for the improvement of CH4 recovery in the pressure swing adsorption process from coalbed gas.

Sustainable management of medical plastic waste through carbon dioxide-assisted pyrolysis.

To address the challenges associated with medical plastic waste and to characterize its heterogeneity, non-recyclability, and potential biohazard risks, this study explored a carbon dioxide (CO2)-assisted pyrolysis process as a sustainable disposal method. Medical plastic waste typically includes polypropylene, polystyrene, and polyvinyl chloride. To experimentally evaluate the functional reactivity of CO2, we employed three pyrolysis setups (one-stage, two-stage, and catalytic processes). The technical advantages of using CO2 over inert gases such as nitrogen (N2) were demonstrated through pyrolysis tests. The results showed that energy production was enhanced under CO2 conditions, with catalytic pyrolysis generating 146% more flammable gases compared to pyrolysis in an N2 environment. The use of CO2 also led to a reduction in the formation of toxic chemicals due to improved thermal cracking. The CO2-assisted pyrolysis process exhibited net negative CO2 emissions when a catalyst was present, as a substantial amount of CO2 was consumed during the process. In conclusion, CO2-assisted pyrolysis of medical plastic waste offers a sustainable management solution that maximizes the utilization of carbon resources.

Regulating Manganese-Site Electronic Structure via Reconstituting Nitrogen Coordination for Efficient Non-Oxygen-Dependent Sonocatalytic Therapy against Orthotopic Breast Cancer.

Sonocatalytic therapy (SCT) has emerged as a promising noninvasive modality for tumor treatment but is hindered by the insufficient generation of ultrasound-induced reactive oxygen species (ROS) and the hypoxic tumor microenvironments. Herein, we fabricated a carbon nanoframe-confined N-coordinated manganese single-atom sonocatalyst with a five-coordinated structure (MnN5 SA/CNF) using a phthalocyanine-mediated pyrolysis strategy. The precise coordination structure was identified by synchrotron X-ray absorption fine structure analyses. The MnN5 SA/CNF exhibits superior and nonoxygen-dependent sonocatalytic activity owing to the optimized coordination structure and cavitation effect enhanced by defects. Additionally, density functional theory studies reveal that the five-coordination structure downshifts the d-band center of Mn from -0.547 to -0.829 eV and enhances the desorption capacity for oxygen-containing intermediates, thus accelerating the catalytic process. Finally, the as-synthesized MnN5 SA/CNF demonstrates a significantly enhanced antitumor effect through mitochondrial apoptosis in an orthotopic breast cancer mouse model. This work explores the potential of SAzymes-supported biomedical interventions by leveraging enzymatic activity with sonocatalytic properties.