Dissecting the Photochemical Reactivity of Metal Ions during Atmospheric Nitrate Transformations on Photoactive Mineral Dust.

Dissecting the photochemical reactivity of metal ions is a significant contribution to understanding secondary pollutant formation, as they have a role to be reckoned with atmospheric chemistry. However, their photochemical reactivity has received limited attention within the active nitrogen cycle, particularly at the gas-solid interface. In this study, we delve into the contribution of magnesium ion (Mg2+) and ferric ion (Fe3+) to nitrate decomposition on the surface of photoactive mineral dust. Under simulated sunlight irradiation, the observed NOX production rate differs by an order of magnitude in the presence of Mg2+ (6.02 × 10-10 mol s-1) and Fe3+ (2.07 × 10-11 mol s-1). The markedly decreased fluorescence lifetime induced by Mg2+ and the change in the valence of Fe3+ revealed that Mg2+ and Fe3+ significantly affect the concentration of nitrate decomposition products by distinct photochemical reactivity with photogenerated electrons. Mg2+ promotes NOX production by accelerating charge transfer, while Fe3+ hinders nitrate decomposition by engaging in a redox cyclic reaction with Fe2+ to consume photogenerated carriers continuously. Furthermore, when Fe3+ coexists with other metal ions (e.g., Mg2+, Ca2+, Na+, and K+) and surpasses a proportion of approximately 12%, the photochemical reactivity of Fe3+ tends to be dominant in depleting photogenerated electrons and suppressing nitrate decomposition. Conversely, below this threshold, the released NOX concentration increases sharply as the proportion of Fe3+ decreases. This research offers valuable insights into the role of metal ions in nitrate transformation and the generation of reactive nitrogen species, contributing to a deep understanding of atmospheric photochemical reactions.

Machine learning and deep learning approaches for enhanced prediction of hERG blockade: a comprehensive QSAR modeling study.

BACKGROUND: Cardiotoxicity is a major cause of drug withdrawal. The hERG channel, regulating ion flow, is pivotal for heart and nervous system function. Its blockade is a concern in drug development. Predicting hERG blockade is essential for identifying cardiac safety issues. Various QSAR models exist, but their performance varies. Ongoing improvements show promise, necessitating continued efforts to enhance accuracy using emerging deep learning algorithms in predicting potential hERG blockade. STUDY DESIGN AND METHOD: Using a large training dataset, six individual QSAR models were developed. Additionally, three ensemble models were constructed. All models were evaluated using 10-fold cross-validations and two external datasets. RESULTS: The 10-fold cross-validations resulted in Mathews correlation coefficient (MCC) values from 0.682 to 0.730, surpassing the best-reported model on the same dataset (0.689). External validations yielded MCC values from 0.520 to 0.715 for the first dataset, exceeding those of previously reported models (0 - 0.599). For the second dataset, MCC values fell between 0.025 and 0.215, aligning with those of reported models (0.112 - 0.220). CONCLUSIONS: The developed models can assist the pharmaceutical industry and regulatory agencies in predicting hERG blockage activity, thereby enhancing safety assessments and reducing the risk of adverse cardiac events associated with new drug candidates.

Photocatalytic Formamide Synthesis via Coupling of Electrophilic and Nucleophilic Radicals over Atomically Dispersed Bi Sites.

Formamide (HCONH2) plays a pivotal role in the manufacture of a diverse array of chemicals, fertilizers, and pharmaceuticals. Photocatalysis holds great promise for green fabrication of carbon-nitrogen (C-N) compounds owing to its environmental friendliness and mild redox capability. However, the selective formation of the C-N bond presents a significant challenge in the photocatalytic synthesis of C-N compounds. This work developed a photocatalytic radical coupling method for the formamide synthesis from co-oxidation of ammonia (NH3) and methanol (CH3OH). An exceptional formamide yield rate of 5.47 ± 0.03 mmol·gcat-1·h-1 (911.87 ± 0.05 mmol·gBi-1·h-1) was achieved over atomically dispersed Bi sites (BiSAs) on TiO2. An accumulation of 45.0 mmol·gcat-1 (0.2 g·gcat-1) of formamide was achieved after long-term illumination, representing the highest level of photocatalytic C-N compounds synthesis. The critical C-N coupling for formamide formation originated from the "σ-σ" interaction between electrophilic ●CH2OH with nucleophilic ●NH2 radical. The  BiSAs sites facilitated the electron transfer between reactants and photocatalysts and enhanced the nucleophilic attack of â—NH2 radical at the â—CH2OH radical, thereby advancing the selective C-N bond formation. This work deepens the understanding of the C-N coupling mechanism and offers an alternative and intriguing photocatalytic approach for the efficient and sustainable production of C-N compounds.

In situ fabrication of atomically adjacent dual-vacancy sites for nearly 100% selective CH4 production.

The photocatalytic CO2-to-CH4 conversion involves multiple consecutive proton-electron coupling transfer processes. Achieving high CH4 selectivity with satisfactory conversion efficiency remains challenging since the inefficient proton and electron delivery path results in sluggish proton-electron transfer kinetics. Herein, we propose the fabrication of atomically adjacent anion-cation vacancy as paired redox active sites that could maximally promote the proton- and electron-donating efficiency to simultaneously enhance the oxidation and reduction half-reactions, achieving higher photocatalytic CO2 reduction activity and CH4 selectivity. Taking TiO2 as a photocatalyst prototype, the operando electron paramagnetic resonance spectra, quasi in situ X-ray photoelectron spectroscopy measurements, and high-angle annular dark-field-scanning transmission electron microscopy image analysis prove that the VTi on TiO2 as initial sites can induce electron redistribution and facilitate the escape of the adjacent oxygen atom, thereby triggering the dynamic creation of atomically adjacent dual-vacancy sites during photocatalytic reactions. The dual-vacancy sites not only promote the proton- and electron-donating efficiency for CO2 activation and protonation but also modulate the coordination modes of surface-bound intermediate species, thus converting the endoergic protonation step to an exoergic reaction process and steering the CO2 reduction pathway toward CH4 production. As a result, these in situ created dual active sites enable nearly 100% CH4 selectivity and evolution rate of 19.4 µmol g-1 h-1, about 80 times higher than that of pristine TiO2. Thus, these insights into vacancy dynamics and structure-function relationship are valuable to atomic understanding and catalyst design for achieving highly selective catalysis.

The relationship between innate/adaptive immunity and gastrointestinal cancer : a multi-omics Mendelian randomization study.

BACKGROUND: Innate/adaptive immunity is the key to anti-tumor therapy. However, its causal relationship to Gastrointestinal (GI) cancer remains unclear. METHODS: Immunity genes were extracted from the MSigDB database. The Genome-wide association studies (GWAS) summary data of GI cancer were integrated with expression quantitative trait loci (eQTL) and DNA methylation quantitative trait loci (mQTL) associated with genes. Summary-data-based Mendelian randomization (SMR) and co-localization analysis were used to reveal causal relationships between genes and GI cancer. Two-sample MR analysis was used for sensitivity analysis. Single cell analysis clarified the enrichment of genes. RESULTS: Three-step SMR analysis showed that a putative mechanism, cg17294865 CpG site regulating HLA-DRA expression was negatively associated with gastric cancer risk. HLA-DRA was significantly differentially expressed in monocyte/macrophage and myeloid cells in gastric cancer. CONCLUSION: This study provides evidence that upregulating the expression level of HLA-DRA can reduce the risk of gastric cancer.

Decoding the κ Opioid Receptor (KOR): Advancements in Structural Understanding and Implications for Opioid Analgesic Development.

The opioid crisis in the United States is a significant public health issue, with a nearly threefold increase in opioid-related fatalities between 1999 and 2014. In response to this crisis, society has made numerous efforts to mitigate its impact. Recent advancements in understanding the structural intricacies of the κ opioid receptor (KOR) have improved our knowledge of how opioids interact with their receptors, triggering downstream signaling pathways that lead to pain relief. This review concentrates on the KOR, offering crucial structural insights into the binding mechanisms of both agonists and antagonists to the receptor. Through comparative analysis of the atomic details of the binding site, distinct interactions specific to agonists and antagonists have been identified. These insights not only enhance our understanding of ligand binding mechanisms but also shed light on potential pathways for developing new opioid analgesics with an improved risk-benefit profile.

Characterization of phosphate modified red mud-based composite materials and study on heavy metal adsorption.

In this paper, Bayer red mud (RM) and lotus leaf powder (LL) were used as the main materials, and KH2PO4 was added to modify the material. Under the condition of high-temperature carbonization, RMLL was prepared and phosphate modified red mud matrix composite (PRMLL) was prepared based on KH2PO4 modification, which can effectively remove Pb2+ from water. The optimum preparation and application conditions were determined through orthogonal experiment: dosage 0.1g, ratio 1:1, and temperature 600 °C. The effects of pH, dosage, and initial concentration on the adsorption of Pb2+ were studied. The pseudo-first-order, pseudo-second-order, and Elovich kinetic models were fitted to the experimental data. It was found that RMLL and PRMLL were more consistent with the pseudo-second-order kinetic model and chemisorption. Langmuir, Freundlich, Timkin, and Dubinin-Radushkevich isothermal adsorption models were used to fit the experimental data. It was found that RMLL and PRMLL were more consistent with Langmuir model. In addition, the maximum adsorption capacity of RMLL and PRMLL was 188.1 mg/g and 213.4 mg/g, respectively. It is larger than the adsorption capacity of their monomers. Therefore, the use of RMLL and PRMLL as the removal of Pb2+ from water is a potential application material.

Steering Photooxidation of Methane to Formic Acid over A Priori Screened Supported Catalysts.

Efficient methane photooxidation to formic acid (HCOOH) has emerged as a sustainable approach to simultaneously generate value-added chemicals and harness renewable energy. However, the persistent challenge lies in achieving a high yield and selectivity for HCOOH formation, primarily due to the complexities associated with modulating intermediate conversion and desorption after methane activation. In this study, we employ first-principles calculations as a comprehensive guiding tool and discover that by precisely controlling the O2 activation process on noble metal cocatalysts and the adsorption strength of carbon-containing intermediates on metal oxide supports, one can finely tune the selectivity of methane photooxidation products. Specifically, a bifunctional catalyst comprising Pd nanoparticles and monoclinic WO3 (Pd/WO3) would possess optimal O2 activation kinetics and an intermediate oxidation/desorption barrier, thereby promoting HCOOH formation. As evidenced by experiments, the Pd/WO3 catalyst achieves an exceptional HCOOH yield of 4.67 mmol gcat-1 h-1 with a high selectivity of 62% under full-spectrum light irradiation at room temperature using molecular O2. Notably, these results significantly outperform the state-of-the-art photocatalytic systems operated under identical condition.

Photocatalytic NO x removal and recovery: progress, challenges and future perspectives.

The excessive production of nitrogen oxides (NO x ) from energy production, agricultural activities, transportation, and other human activities remains a pressing issue in atmospheric environment management. NO x serves both as a significant pollutant and a potential feedstock for energy carriers. Photocatalytic technology for NO x removal and recovery has received widespread attention and has experienced rapid development in recent years owing to its environmental friendliness, mild reaction conditions, and high efficiency. This review systematically summarizes the recent advances in photocatalytic removal, encompassing NO x oxidation removal (including single and synergistic removal and NO3 - decomposition), NO x reduction to N2, and the emergent NO x upcycling into green ammonia. Special focus is given to the molecular understanding of the interfacial nitrogen-associated reaction mechanisms and their regulation pathways. Finally, the status and the challenges of photocatalytic NO x removal and recovery are critically discussed and future outlooks are proposed for their potential practical application.

Efficient and Durable Oxidation Removal of Formaldehyde over Layered Double Hydroxide Catalysts at Room Temperature.

Room temperature catalytic oxidation (RTCO) using non-noble metals has emerged as a highly promising technique for removal of formaldehyde (HCHO) under ambient conditions; however, non-noble catalysts still face the challenges related to poor water resistance and low stability under harsh conditions. In this study, we synthesized a series of layered double hydroxides (LDHs) incorporating various dual metals (MgAl, ZnAl, NiAl, NiFe, and NiTi) for formaldehyde oxidation at ambient temperature. Among the synthesized catalysts, the NiTi-LDH catalyst showed an HCHO removal efficiency and CO2 yield close to 100.0%, and exceptional water resistance and chemical stability on running 1300 min. The abundant hydroxyl groups in LDHs directly bonded with HCHO, leading to the production of CO2 and H2O, thus inhibiting the formation of CO, even in the absence of O2 and H2O. The coexistence of O2 effectively reduced the reaction barrier for H2O molecule dissociation, facilitating the formation of hydroxyl groups and their subsequent backfill on the catalyst surface. The mechanisms underlying the involvement and regeneration of hydroxyl groups in room temperature oxidation of formaldehyde were elucidated with the combined in situ DRIFTS, HCHO-TPD-MS, and DFT calculations. This work not only demonstrates the potential of LDH catalysts in environmental applications but also advances the understanding of the fundamental processes involved in room temperature oxidation of formaldehyde.

S-Scheme heterojunction of Cs2SnBr6/C3N4 with interfacial electron exchange toward efficient photocatalytic NO abatement.

Photocatalytic technology is of great significance in environmental purification due to its eco-friendly and cost-effective operations. However, low charge-transfer efficiency restricts the photocatalytic activity of the catalyst. Herein, we report Cs2SnBr6/C3N4 composite catalysts that exhibit a robust interfacial electron exchange thereby enhancing photocatalytic nitric oxide (NO) oxidation. A comprehensive study has demonstrated the S-scheme electron transfer mechanism. Benefiting from the interfacial internal electric field, the C-Br bond serves as a direct electron transfer channel, resulting in enhanced charge separation. Furthermore, the S-scheme heterojunction effectively traps high redox potential electrons and holes, leading to the production of abundant reactive oxygen radicals that enhance photocatalytic NO abatement. The NO removal rate of the Cs2SnBr6/C3N4 heterogeneous system can reach 86.8 %, which is approximately 3-fold and 18-fold that of pristine C3N4 and Cs2SnBr6, respectively. The comprehensive understanding of the electron transfer between heterojunction atomic interfaces will provide a novel perspective on efficient environmental photocatalysis.

The impact of frailty on clinical outcomes of older patients undergoing enhanced recovery after lumbar fusion surgery: A prospective cohort study.

BACKGROUND: Frailty is recognized as a surrogate for physiological age and has been established as a valid and independent predictor of postoperative morbidity, mortality, and complications. ERAS can enhance surgical safety by minimizing stress responses in frail patients, enabling surgeons to discharge patients earlier. However, the question of whether and to what extent the frailty impacts the post-ERAS outcomes in older patients remains. MATERIALS AND METHODS: An evidence-based ERAS program was implemented in our center from January 2019. This is a prospective cohort study of patients aged ≥75 years who underwent open transforaminal lumbar interbody fusion (TLIF) for degenerative spine disease from April 2019 to October 2021. Frailty was assessed with the Fried frailty scale (FP scale), and patients were categorized as non/prefrail (FP 0-2) or frail (FP ≥ 3). The preoperative variables, operative data, postoperative outcomes and follow-up information were compared between the two groups. Univariate and multivariate logistic regression analyses were used to identify risk factors for 90-day major complications and prolonged length of hospital stay (LOS) after surgery. RESULTS: A total of 245 patients (age of 79.8 ± 3.4 yr) who had a preoperative FP score recorded and underwent scheduled TLIF surgery were included in the final analysis. Comparisons between non-frail and prefrail/frail patients revealed no significant difference in age, sex, and surgery-related variables. Even after adjusting for multiple comparisons, the association between Fried frailty and ADL-dependency, IADL-dependency, and malnutrition remained significant. Preoperative frailty was associated with increased rates of postoperative adverse events. A higher CCI grade was an independent predictor for 90-day major complications, while Fried frailty and MNA-SF scores <12 were predictive of poor postoperative recovery. CONCLUSION: Frail older patients had more adverse post-ERAS outcomes after TLIF compared to non/prefrail older patients. Continued research and multidisciplinary collaboration will be essential to refine and optimize protocols for surgical care in frail older adults.

Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide at Industrial-Level Current Densities Promoted by Alkali Metal Cations.

Acidic H2O2 synthesis through electrocatalytic 2e- oxygen reduction presents a sustainable alternative to the energy-intensive anthraquinone oxidation technology. Nevertheless, acidic H2O2 electrosynthesis suffers from low H2O2 Faradaic efficiencies primarily due to the competing reactions of 4e- oxygen reduction to H2O and hydrogen evolution in environments with high H+ concentrations. Here, we demonstrate the significant effect of alkali metal cations, acting as competing ions with H+, in promoting acidic H2O2 electrosynthesis at industrial-level currents, resulting in an effective current densities of 50-421 mA cm-2 with 84-100 % Faradaic efficiency and a production rate of 856-7842 µmol cm-2 h-1 that far exceeds the performance observed in pure acidic electrolytes or low-current electrolysis. Finite-element simulations indicate that high interfacial pH near the electrode surface formed at high currents is crucial for activating the promotional effect of K+. In situ attenuated total reflection Fourier transform infrared spectroscopy and ab initio molecular dynamics simulations reveal the central role of alkali metal cations in stabilizing the key *OOH intermediate to suppress 4e- oxygen reduction through interacting with coordinated H2O.

BERT-based language model for accurate drug adverse event extraction from social media: implementation, evaluation, and contributions to pharmacovigilance practices.

Introduction: Social media platforms serve as a valuable resource for users to share health-related information, aiding in the monitoring of adverse events linked to medications and treatments in drug safety surveillance. However, extracting drug-related adverse events accurately and efficiently from social media poses challenges in both natural language processing research and the pharmacovigilance domain. Method: Recognizing the lack of detailed implementation and evaluation of Bidirectional Encoder Representations from Transformers (BERT)-based models for drug adverse event extraction on social media, we developed a BERT-based language model tailored to identifying drug adverse events in this context. Our model utilized publicly available labeled adverse event data from the ADE-Corpus-V2. Constructing the BERT-based model involved optimizing key hyperparameters, such as the number of training epochs, batch size, and learning rate. Through ten hold-out evaluations on ADE-Corpus-V2 data and external social media datasets, our model consistently demonstrated high accuracy in drug adverse event detection. Result: The hold-out evaluations resulted in average F1 scores of 0.8575, 0.9049, and 0.9813 for detecting words of adverse events, words in adverse events, and words not in adverse events, respectively. External validation using human-labeled adverse event tweets data from SMM4H further substantiated the effectiveness of our model, yielding F1 scores 0.8127, 0.8068, and 0.9790 for detecting words of adverse events, words in adverse events, and words not in adverse events, respectively. Discussion: This study not only showcases the effectiveness of BERT-based language models in accurately identifying drug-related adverse events in the dynamic landscape of social media data, but also addresses the need for the implementation of a comprehensive study design and evaluation. By doing so, we contribute to the advancement of pharmacovigilance practices and methodologies in the context of emerging information sources like social media.

Designing Surface and Interface Structures of Copper-Based Catalysts for Enhanced Electrochemical Reduction of CO2 to Alcohols.

Electrochemical CO2 reduction (ECR) has emerged as a promising solution to address both the greenhouse effect caused by CO2 emissions and the energy shortage resulting from the depletion of nonrenewable fossil fuels. The production of multicarbon (C2+) products via ECR, especially high-energy-density alcohols, is highly desirable for industrial applications. Copper (Cu) is the only metal that produces alcohols with appreciable efficiency and kinetic viability in aqueous solutions. However, poor product selectivity is the main technical problem for applying the ECR technology in alcohol production. Extensive research has resulted in the rational design of electrocatalyst architectures using various strategies. This design significantly affects the adsorption energetics of intermediates and the reaction pathways for alcohol production. In this review, we focus on the design of effective catalysts for ECR to alcohols, discussing fundamental principles, innovative strategies, and mechanism understanding. Furthermore, the challenges and prospects in utilizing Cu-based materials for alcohol production via ECR are discussed.

Mechanism of Interfacial Molecular Interactions Reveals the Intrinsic Factors for the Highly Enhanced Sensing Performance of Ag-Loaded Co3O4.

The noble metal-loaded strategy can effectively improve the gas-sensing performances of metal oxide sensors. However, the gas-solid interfacial interactions between noble metal-loaded sensing materials and gaseous species remain unclear, posing a significant challenge in correlating the physical and chemical processes during gas sensing. In this study, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and in situ Raman spectroscopy were conducted to collaboratively investigate the interfacial interactions involved in the ethanol gas-sensing processes over Co3O4 and Ag-loaded Co3O4 sensors. In situ DRIFTS revealed differences in the compositions and quantities of sensing reaction products, as well as in the adsorption-desorption interactions of surface species, among Co3O4 and Ag-loaded Co3O4 materials. In parallel, in situ Raman spectroscopy demonstrated that the ethanol atmosphere can modulate the electron scattering of Ag-loaded Co3O4 materials but not of raw Co3O4. In situ experimental results revealed the intrinsic reason for the highly enhanced sensing performances of the Ag-loaded Co3O4 sensors toward ethanol gas, including a decreased optimal working temperature (from 250 to 150 °C), an improved gas response level (from 24 to 257), and accelerated gas recovery dynamics. This work provides an effective platform to investigate the interfacial interactions of sensing processes at the molecular level and further advances the development of high-performance gas sensors.

Impaired meningeal lymphatic drainage in Listeria monocytogenes infection.

Previous studies have demonstrated an association between lymphatic vessels and diseases caused by bacterial infections. Listeria monocytogenes (LM) bacterial infection can affect multiple organs, including the intestine, brain, liver and spleen, which can be fatal. However, the impacts of LM infection on morphological and functional changes of lymphatic vessels remain unexplored. In this study, we found that LM infection not only induces meningeal and mesenteric lymphangiogenesis in mice, but also impairs meningeal lymphatic vessels (MLVs)-mediated macromolecules drainage. Interestingly, we found that the genes associated with lymphatic vessel development and function, such as Gata2 and Foxc2, were downregulated, suggesting that LM infection may affect cellular polarization and valve development. On the other hand, photodynamic ablation of MLVs exacerbated inflammation and bacterial load in the brain of mice with LM infection. Overall, our findings indicate that LM infection induces lymphangiogenesis and may affect cell polarization, cavity formation, and valve development during lymphangiogenesis, ultimately impairing MLVs drainage.

Mechanically treated Mn2O3 triggers peracetic acid activation for superior non-radical oxidation of micropollutants: Identification of reactive complexes.

This study used a simple mechanical ball milling strategy to significantly improve the ability of Mn2O3 to activate peracetic acid (PAA) for sustainable and efficient degradation of organic micropollutant (like bisphenol A, BPA). BPA was successfully removed and detoxified via PAA activation by the bm-Mn2O3 within 30 min under neutral environment, with the BPA degradation kinetic rate improved by 3.4 times. Satisfactory BPA removal efficiency can still be achieved over a wide pH range, in actual water and after reuse of bm-Mn2O3 for four cycles. The change in hydrophilicity of Mn2O3 after ball milling evidently elevated the affinity of Mn2O3 for binding to PAA, while the reduction in particle size exposed more active sites contributing partially to catalytic oxidation. Further analysis revealed that BPA oxidation in the ball mill-treated Mn2O3 (bm-Mn2O3)/PAA process mainly depends on the bm-Mn2O3-PAA complex (i.e., Mn(III)-OO(O)CCH3) mediated non-radical pathway rather than R-O• and Mn(IV). Especially, the existence of the Mn(III)-PAA complex was definitely verified by in situ Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Simultaneously, density functional theory calculations determined that PAA adsorbs readily on manganese sites thereby favoring the formation of Mn(III)-OO(O)CCH3 complexes. This study advances an in-depth understanding of the underlying mechanisms involved in the manganese oxide-catalyzed activation of PAA for superior non-radical oxidation of micropollutants.

Regulating the Selectivity of Nitrate Photoreduction for Purification or Ammonia Production by Cooperating Oxidative Half-Reactions.

The removal and conversion of nitrate (NO3-) from wastewater has become an important environmental and health topic. The NO3- can be reduced to nontoxic nitrogen (N2) for environmental remediation or ammonia (NH3) for recovery, in which the tailoring of the selectivity is greatly challenging. Here, by construction of the CuOx@TiO2 photocatalyst, the NO3- conversion efficiency is enhanced to ∼100%. Moreover, the precise regulation of selectivity to NH3 (∼100%) or N2 (92.67%) is accomplished by the synergy of cooperative redox reactions. It is identified that the selectivity of the NO3- photoreduction is determined by the combination of different oxidative reactions. The key roles of intermediates and reactive radicals are revealed by comprehensive in situ characterizations, providing direct evidence for the regulated selectivity of the NO3- photoreduction. Different active radicals are produced by the interaction of oxidative reactants and light-generated holes. Specifically, the introduction of CH3CHO as the oxidative reactant results in the generation of formate radicals, which drives selective NO3- reduction into N2 for its remediation. The alkyl radicals, contributed to by the (CH2OH)2 oxidation, facilitate the deep reduction of NO3- to NH3 for its upcycling. This work provides a technological basis for radical-directed NO3- reduction for its purification and resource recovery.