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Frontiers in Environmental Science · 2024 · IF 3.3

Enhanced photochemical formation of active nitrogen species from aqueous nitrate in the presence of halide ions

Zhao Yilong,Liu Chengwei,Tu Xiang,Huang Wenkai,Liu Yu,Fu Hongbo

Field observations have confirmed that halide ions are widely distributed among aerosols from the marine boundary layer and on the surfaces of ice and snow in polar regions. Consequently, the coexistence of halide ions may play a more significant role in nitrate photolysis than previously thought. In this study, we simultaneously measured HONO, NO2, and NO2− in situ to gain a deeper understanding of the coexisting system, including the photogenerated nitrogen products and the effects on nitrate photolysis rates due to enhanced aqueous nitrite and HONO transfer rates by halides. The presence of halides significantly increased the photogenerated nitrogen products across various molar ratios ([X–]/[NO3−]) at pH 3.5. By eliminating oxygen flux, the transformation of the primary photogenerated products was affected, resulting in higher concentrations of N(III) as both HONO and NO2−. Experiments involving OH scavengers indicated that the attack from·OH initiated by halides leads to side reactions that enhance nitrate photolysis. Both theoretical calculations and nitrate actinometry were used to determine the photolysis rate of nitrate solutions, which together indicated that the presence of halides enhances nitrate photolysis. A newly developed model was used to determine the HONO transfer rate, finding that the presence of halides ([X–]/[NO3−] = 0.2) enhanced the evaporation of N(III) in solution by factors of 0.68, 0.95, and 1.27 for Cl−, Br−, and I−, respectively. To our knowledge, this is the first determination of halide effects on the mass transfer of HONO. The enhanced nitrate photolysis rate can be attributed to the differential surface effects of halides and parallel reactions initiated via ·OH stemming from nitrate photolysis, with varying rates leading to different quantities of nitrogenous products. Additionally, simultaneous measurements of photoproducts in both gas and condensed phases are recommended to better constrain the rate constants of NO3− photolysis.

研究领域: 环境科学 · 大气化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Photo-anammox by vacuum ultraviolet tandem chlorine

Wenzhe Liu,Baiyang Chen,Yang Yang,Boqiang Li,Huimei Pan,Wang Luo

Excessive ammonia (NH 4 + ) discharge can lead to algal blooms and disrupt water sustainability, so its control is imperative. Although microbiology-triggered anammox process is promising, its application is limited due to time-consuming cultivation of specific microorganisms and need for skilled operation. To bypass these barriers, this study proposed and verified a photo-induced anammox technology that removes NH 4 + and total nitrogen (TN) from water by ultraviolet (UV)/vacuum UV (VUV)/chlorine under anoxic conditions . Under the Cl/N mass ratio of 5:1, the anoxic VUV/UV/chlorine process achieved 66.8% removal of 10 mg-N/L NH 4 + within 10 min along with 57.8% reduction in TN. Besides the evidence from TN loss, this study confirmed nitrogen gas (N 2 ) as the primary degradation product at low dissolved oxygen (DO) concentration of 2.0 mg/L. The selective conversion of NH 4 + into N 2 was mainly attributed to reactive nitrogen species (RNS, 42.5%) and reactive chlorine species (RCS, 57.5%). The TN removal efficiency was insensitive to certain variations of pH (7.0–9.0), NH 4 + concentration (1–30 mg-N/L), chloride (50–125 mg/L), and sulfate (25–100 mg/L), but sensitive to DO and bicarbonate (25–100 mg/L). Given its robustness and high efficiency, the anoxic VUV/UV/chlorine technology may serve as a potentially promising alternative for NH 4 + and TN alleviation in wastewater.

研究领域: 环境科学 · 微生物学
✓ 已验证 DOI PubMed 高影响因子
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CHEMOSPHERE · 2022 · IF 8.943

Influence of nitrate/nitrite on the degradation and transformation of triclosan in the UV based disinfection

Xuguang Liu,Fengqin Chang,Dayu Zhang,Meijie Ren

This study investigated the influence of nitrate/nitrite on the degradation and transformation pathway of triclosan (TCS) in UV, UV/peracetic acid (PAA) and UV/HClO processes. The results indicated that the function of nitrate/nitrite significantly depended on the UV source and wavelength, especially nitrate. Generally, the presence of nitrate decreased the direct photo-degradation of TCS in the UV based disinfection. In the LED-UV and LED-UV/HClO processes, the presence of nitrate improved the radical oxidation, and transformation pathway of TCS was varied accordingly. However, nitrate more played a role of photo-competitor in the UV/PAA process, and the reactive nitrogen species (RNS) was difficult to participant in the degradation of TCS due to low redox potential . Compared to nitrate, the presence of nitrite decreased the degradation of TCS in three different UV based disinfection processes. Under UV irradiation, nitrite primarily acted as an irradiation competitor and radical scavenger. Thus, the indirect photo-degradation of TCS was reduced. Noticeably, nitrate/nitrite were the improtant precersors of nitrogenous products in the UV base disinfection. Many new nitrogenous products were identified. But RNS preferentially reacted with the intermediates by –NO 2 addition compared to directly reacted with TCS.

研究领域: 环境科学 · 化学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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WATER RESEARCH · 2020 · IF 9.13

UV365 induced elimination of contaminants of emerging concern in the presence of residual nitrite: Roles of reactive nitrogen species

Shiqing Zhou,Ling Li,Yangtao Wu,Shumin Zhu,Ningyuan Zhu,Lingjun Bu,Dionysios D. Dionysiou

The presence of nitrite (NO 2 − ) is inevitable with concentrations of several mg L −1 in some typical water bodies. In this study, UV at wavelength of 365 nm was investigated to degrade contaminants of emerging concern (CECs) in the presence of NO 2 − at environmentally relevant concentrations (0.1–5.0 mg L −1 ). Six selected CECs with different structures were efficiently removed because of the generation of reactive nitrogen species (RNS) and hydroxyl radical (HO • ) from photolysis of NO 2 − . Contributions of UV 365 photolysis, RNS, and HO • to CEC degradation in UV 365 /NO 2 − system were calculated, and RNS were found to be the predominant species that are responsible for CEC degradation. The second major contributor is HO • for the degradation of selected CECs except for the case of sulfadiazine. Impacts of water matrix components (including dissolved oxygen, solution pH, and natural organic matter) on CEC degradation in UV 365 /NO 2 − system were evaluated. Furthermore, evolution profiles of CECs and NO 2 − in UV 365 /NO 2 − system were tracked when actual water samples were used as background, and a simultaneous removal of CECs and NO 2 − was observed. Transformation products of bisphenol A and carbamazepine were proposed according to the results of HPLC/MS and quantum chemistry calculations. Nitration induced by RNS and hydroxylation induced by HO • are main reactions occurred during CEC degradation in UV 365 /NO 2 − system. Overall, UV 365 is a potential technology to remove CECs and NO 2 − in aquatic environment when residual NO 2 − is present. Our present study also provides possibility for the application of sunlight to remediate water co-polluted by CECs and NO 2 − .

研究领域: 环境科学 · 化学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Small · 2025 · IF 12.1

Broad-Spectrum ROS/RNS Scavenging Catalase-Loaded Microreactors for Effective Oral Treatment of Inflammatory Bowel Diseases

Xiangyu Zhang,Yujie Zhu,Zijian Xiong,Wenjie Xie,Ming Shao,Zhuang Liu

Inflammatory bowel disease (IBD) such as ulcerative colitis (UC) is an autoimmune disease characterized by persistent inflammation along the gastrointestinal tract with excessive generation of reactive oxygen species (ROS)/reactive nitrogen species (RNS) generation. Here, catalase (CAT)-containing microreactor capsules with long-lasting broad-spectrum ROS/RNS-scavenging capability are developed for the treatment of IBD. In this design, CAT is encapsulated in the dense hydrogel network of calcium alginate (ALG) microspheres, which provides long-term protection of CAT activity in protease-rich intestinal environment. Afterward, the polydopamine (PDA) modification on the surface of CAT@ALG microspheres can provide them bioadhesiveness to achieve prolonged retention in the intestinal tract and broad-spectrum scavenging capability against various types of ROS/RNS beyond hydrogen peroxide. Enteric capsules are further used to protect the CAT@ALG–PDA microspheres from gastric fluid for selective release at the intestinal site. The combined action of PDA and CAT in CAT@ALG–PDA microreactors results in the broad-spectrum scavenging of excess ROS/RNS and regulates redox balance in acute UC rat model, showing satisfactory therapeutic effects superior to the mesalazine and adalimumab at clinically relevant doses without obvious side effects. This work highlights that these CAT@ALG–PDA capsules can act as long-acting broad-spectrum ROS/RNS reactors, promising for IBD treatment.

CAS / MDL: 62-31-7
研究领域: 医学 · 生物材料学 · 药剂学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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WATER RESEARCH · 2020 · IF 9.13

Nitrogen conversion from ammonia to trichloronitromethane: Potential risk during UV/chlorine process

Shiqing Zhou,Yangtao Wu,Shumin Zhu,Julong Sun,Lingjun Bu,Dionysios D. Dionysiou

In this study, the potential formation of trichloronitromethane (TCNM) from model organic compounds in ammonia-containing water treated by UV/chlorine process was evaluated. Monochloramine generated from the reaction of chlorine and ammonia can be photolyzed to produce NO 2 − and reactive nitrogen species (RNS), which play important roles in the formation of TCNM during the subsequent chlorination. The results showed that increase of nitrogen to chlorine molar ratio (from 0 to 1.0) and pH (from 6.5 to 8.0) enhanced the formation of TCNM, mainly due to the increased yield of NO 2 − and RNS from the photolyzed monochloramine. The formation of TCNM was interestingly found to be linearly correlated with Hammett constants of the model precursors, which is theoretically related to the rate constants of RNS with model compounds. Enhanced formation of TCNM was also observed during the treatment of natural organic matter by UV/chlorine process in ammonia-containing water. The toxicity assessment showed that TCNM significantly increased the genotoxicity of formed DBPs . Furthermore, the electrophilic substitution reaction of • NO 2 was proved to more likely occur on the ortho and para position of phenol according to the calculation of Gaussian program, and a possible reaction pathway of phenol and • NO 2 was proposed based on the calculated results.

研究领域: 环境科学 · 毒理学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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MOLECULAR PHARMACEUTICS · 2025 · IF 4.5

Ultrasound-Driven Nitric Oxide Generation for Enhanced Sonodynamic–Photothermal Therapy

Kun Zhang,Weirong Kong,Dewu Lin,Xiaobing Wang,Pan Wang

Recently, green gas therapy based on nitric oxide (NO) has gained considerable attention in cancer treatment. The supplementation of exogenous NO and its controlled release represent promising strategies for adjuvant tumor therapy. In this study, we developed a novel ultrasound (US)-triggered NO generation and release nanoplatform that integrates NO therapy, sonodynamic therapy, and photothermal therapy (PTT) into a collaborative therapeutic modality. An environmentally friendly biomacromolecule, polydopamine, was employed to coload chlorin e6 (Ce6) and NO donor (BNN6), resulting in the nanocomposite PDA-Ce6/BNN6 (PCB). A single US stimulus simultaneously activated Ce6 to produce reactive oxygen species (ROS) and promoted BNN6 to release NO. The dual effects of ultrasonic mechanical action and physiological modulation by NO substantially improved local vascular function and enhanced tumor cell permeability, thereby increasing the targeted accumulation of PCB within tumors. Reactive nitrogen species (RNS) derived from NO and ROS further exacerbated oxidative damage and enhanced the sensitivity of tumor cells to hyperthermia. Both in vitro and in vivo experiments demonstrated that ultrasonic stimulation of NO/ROS/RNS combined with PTT effectively inhibited tumor cell growth and proliferation. The findings suggest that NO gas therapy based on extracorporeal US can significantly amplify the efficacy of PTT and offer new insights for developing other combined strategies aimed at physically regulating deep tumors.

研究领域: 生物医学工程 · 癌症治疗研究 · 纳米医学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Water Resources and Industry · 2023 · IF 5.1

Mechanism, kinetics and DBPs formation of UV/NH2Cl process on sulfathiazole removal in aqueous solution

Jiayu Zhang,Qiongfang Wang,Lei Dong,Pinhua Rao,Xin Zhang,Naiyun Gao,Xiaoying Yin

In this paper, UV/NH 2 Cl process was used to research the degradation of sulfathiazole (STZ) and the formation of disinfection by-products (DBPs) after disinfection were detected. UV and NH 2 Cl process showed a synergistic effect on the removal of STZ. Natural organic matter and CO 3 2− inhibited the STZ degradation, NO 3 − promoted the degradation of STZ, whereas NH 2 Cl concentration, HCO 3 − and Cl − had dual effects on the removal of STZ. The removal of STZ by UV/NH 2 Cl was slightly influenced by pH. The contribution of reactive chlorine species and reactive nitrogen species to STZ degradation was significantly higher than that of HO · . Possible STZ degradation pathways were presented by analyzing intermediate products. In addition, the pretreatment of UV/NH 2 Cl significantly reduced the formation of DBPs during NH 2 Cl or NaClO disinfection. In conclusion, UV/NH 2 Cl process is an effective water treatment technology and can be well applied for practical purposes.

研究领域: 环境科学 · 水处理技术
✓ 已验证 DOI 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

A novel ratiometric electrochemical sensing strategy for monitoring of peroxynitrite anion released from high glucose-induced cells

Li Lin,Liu Qian,Fan Weizhou,Ding Lan,Zhonghua Xue,Liu Xiuhui,Lu Xiaoquan

Monitoring of reactive nitrogen species (RNS) released from cells under high glucose induction is of great importance due to their significant contributions in the occurrence and development of diabetes mellitus (DM). Here, we developed a novel ratiometric electrochemical sensor based on platinum/hollow tubular conjugated organic microporous polymer/chitosan (Pt/HTCMP/CTS) and used for the detection of peroxynitrite anion (ONOO − ), which is the main member of RNS. A "signal on-off" ratiometric dual-signal strategy was designed by using of the redox characteristics of K 3 [Fe(CN) 6 ] ([Fe(CN) 6 ] 4- ) and the analyte (ONOO − ) for the first time. Then, due to the significant enhancement for the ratio of oxidation current value (I ONOO − /I [Fe(CN)6]4- ), the sensor showed excellent analytical performance over a wide range from 3.09 × 10 -10 to 1.20 × 10 -4 M and a detection limit as low as 0.103 nM (S/N = 3). Importantly, in high glucose environment, ONOO − and H 2 O 2 released from cancer cells were monitored directly with the proposed sensor for the first time. Therefore, the study provides an effective method for realizing fast, reliable and ultra-sensitive determination of ONOO-, and exhibits significant application value in biomedical analysis and clinical diagnosis.

CAS / MDL: 9002-93-1
研究领域: 生物医学分析 · 临床诊断 · 材料科学 · 电化学
✓ 已验证 产品关联 DOI 高影响因子
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TEXTILE RESEARCH JOURNAL · 2023 · IF 2.3

Peroxymonosulfate-based catalytic degradation of reactive dyes in real wastewater by Fe/N-codoped carbocatalysts loaded on carbon cloth

Limeng Yang,Wenqiang Yang,Chengyu Fu,Yujuan Li,Pengfei Zhang

This study simulated actual dyeing wastewater in dyeing factories with three types of dyeing wastewaters from laboratory cotton fabric dyeing to investigate the effects of catalyst and oxidant peroxymonosulfate (PMS) concentrations, pH level, and temperature on dye degradation in wastewater and determine the optimal conditions for dyeing wastewater treatment accordingly. The results demonstrated that the optimal conditions varied with the reactive dyes. Specifically, the optimal oxidant PMS concentration for degrading Reactive Yellow and Reactive Blue was 0.6 g/L, and that for degrading Reactive Red was 0.4 g/L. The optimal pH level for degrading Reactive Red and Reactive Blue was around 7.0, and that for degrading Reactive Yellow was about 5.0. The activation energy of the degradation and the mineralization degree of the three dyes were also discussed. Reactive Blue showed greater activation energy (47.0 kJ/mol) and a higher mineralization degree (81% chemical oxygen demand removal) than the other two dyes under optimal disposal conditions. The Fe/N-codoped carbocatalyst loaded on carbon cloth exhibited desirable reusability and good stability for the degradation of the three dyes. Mechanisms involved in their degradation were analyzed through X-ray photoelectron spectroscopy, focusing on N species, Fe-N binding, and C=C and C–N active components in the Fe/N-codoped carbocatalyst. Electron paramagnetic resonance experiments demonstrated that both the radical and non-radical pathways were accountable for the degradation of the three dyes, primarily the non-radical pathway. This study may contribute to the application of activated PMS for practical dyeing wastewater treatment.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Journal of Food Measurement and Characterization · 2024 · IF 2.9

An electrochemical sensor based on full-faradaic-active nitrogen species doped porous carbon materials for highly sensitive nitrite detection

Chen Zhiyan,Ye Xiangzhen,Dhamodharan A.,Zhou Tianhao,Gao Yajun,Xie Mingjiang

Excessive nitrite ( \(\:{\text{NO}}_{\text{2}}^{-}\) ) addition poses a significant threat to food safety. Thus, it is desirable to construct a selective and dependable electrochemical sensor for the quantitative measurement of \(\:{\text{NO}}_{\text{2}}^{-}\) . In this study, an electrochemical sensor using nitrogen-rich porous carbon (NPC) derived from graphitic carbon nitride (g-C 3 N 4 ) was developed for the quantitative detection of \(\:{\text{NO}}_{\text{2}}^{-}\) . The NPC synthesis involved a two-step process, namely polymerization and carbonization. The carefully designed polymerization method and optimal carbonization condition yielded an NPC material with a relatively high surface area of 593.36 m²·g⁻¹. Notably, NPC nanomaterials exhibited a high nitrogen content of 19.8%, comprising various nitrogen species (pyridinic N, pyrrolic N, and oxidized N) that are fully faradaic-active N species, leading to enhanced electrochemical properties and sensitivity. The calibration plot exhibited linearity within the concentration range of 2-3410 µM, LOD of 0.11 µM, a sensitivity of 11.32 µA·µM − 1 cm − 2 and further showed excellent adaptability in real sample analysis. This innovative way of creating electrochemical sensors from nitrogen-rich porous carbon materials broadens the scope of electroanalysis and provides a beneficial means of guaranteeing food safety.

研究领域: 食品科学 · 分析化学 · 材料科学
✓ 已验证 产品关联 DOI 高影响因子
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Journal of Materials Chemistry B · 2017 ·Vol. 5 ·期 46 ·9197-9203 · IF 4.543

Silica nanoparticles based on an AIE-active molecule for ratiometric detection of RNS in vitro

Leijing Liu,Fengli Zhang,Bin Xu,Wenjing Tian

Nitric oxide (NO), known as a reactive nitrogen species (RNS), has been considered to be a significant factor in many cell-related biological processes. There is a great desire to develop fluorescent probes that can highly sensitively and selectively detect NO in living cells. Herein, a fluorescent probe, a tetraphenylethene (TPE) derivative TPE-2NH2, with aggregation induced emission (AIE) properties was designed and synthesized. Then silica nanoparticles based on TPE-2NH2 were fabricated for ratiometric detection of NO in vitro with high sensitivity and selectivity. In the presence of NO, the fluorescence of the silica nanoparticles changes from 519 nm (green) to 655 nm (red) because of the chemical reaction between NO and o-phenylenediamine in TPE-2NH2. The silica nanoparticles exhibited very high sensitivity and selectivity towards NO in aqueous buffer, and the response time was as short as 5 minutes. Moreover, the silica nanoparticles can also highly sensitively and selectively respond to NO produced in living cells. When MCF-7 cancer cells were activated by lipopolysaccharides (LPS), which can effectively induce the production of NO, the red emission signal of the silica nanoparticles obviously increased. This demonstrated that the silica nanoparticles showed fine imaging contrast towards NO in MCF-7 cancer cells, which provides a facile tool to detect intracellular NO.

研究领域: 生物化学 · 分析化学 · 细胞生物学
✓ 已验证 DOI PubMed 高影响因子
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