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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
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Journal of Materials Chemistry C · 2018 ·Vol. 6 ·期 46 ·12631-12637 · IF 5.976

Surface state modulation of red emitting carbon dots for white light-emitting diodes

Kang Yuan,Xinghua Zhang,Ruohan Qin,Xuefeng Ji,Yahui Cheng,Lanlan Li,Xiaojing Yang,Zunming Lu,Hui Liu

Controlling surface states using different functional groups is an effective and facile way to modulate the fluorescence of carbon dots (CDs), but the underlying mechanisms are still unclear and urgent to solve. In this work, we synthesized red emitting CDs and achieved multiple emission states (red, green and blue emission) by tailoring the surface states with different amino groups. In particular, the luminescence mechanism and the role of surface states were studied in detail. It is found that the multiple emission states are related to the speciation of nitrogen (pyridinic N, pyrrolic N, graphitic N and amino N) on the surface of CDs, of which the fluorophore formed by the deformation of p-phenylenediamine contributes to the red emission, pyridinic N is responsible for the green emission state, and pyrrolic N enhances the blue emission. A possible energy level diagram was proposed to disclose the electron transition process and relative levels induced by different surface groups on CDs. In addition, the modulated CDs with multiple emission states can be used as single light converters to fabricate a white light-emitting diode, which has white light color coordinates of (0.31, 0.32), a high color rendering index (CRI) of 85, a luminous efficiency of 8.8 lm W−1 and good stability.

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 光学工程
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ENERGY · 2024 · IF 9

Nitrogen species from Spirulina platensis derived bio-oil enhance catalytic activity of cobalt catalysts for hydrogenation

Mengjiao Fan,Xueming Gao,Yuewen Shao,Kai Sun,Yuchen Jiang,Shu Zhang,Yi Wang,Song Hu,Jun Xiang,Xun Hu

High nitrogen content in Spirulina platensis -derived bio-oil is a highly undesirable feature in upgrading of bio-oil to biofuel via hydrodeoxygenation . However, the nitrogen species could be potentially used as dopant for tailoring the catalytic behaviors of metallic sites in heterogeneous catalysts . In this study, the nitrogen species in the bio-oil from hydrothermal carbonization (HTC) of Spirulina platensis was used to modify Co-based catalyst for enhancing their catalytic activity for hydrogenation of o -chloronitrobenzene ( o -CNB). The results showed that the introduction of N species not only promoted dispersion of Co particles via formation of Co–N sites, but also generated extra pores and significantly increased H 2 uptake. The abundant Co–N sites, high dispersion of Co and higher surface area of N-doped catalyst (CoFeAl–N) jointly contributed to the enhanced catalytic activity for hydrogenation of o -CNB, achieving the yield of 90.3% for o -chloroaniline ( o -CA) and lowering the activation energy from 63.0 kJ mol −1 (with N-free CoFeAl catalyst) to 55.1 kJ mol −1 . The effectiveness of introducing nitrogen for enhancing catalytic activity for hydrogenation of o -CNB was also confirmed in the experiments for doping Co/Al 2 O 3 (prepared via impregnation) and CoAl (prepared via co-precipitation) catalysts with the Spirulina platensis derived bio-oil.

CAS / MDL: 95-51-2
研究领域: 生物化学 · 催化化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2025 · IF 7.7

A novel fluorescent sensing strategy for point-of-care monitoring of Hg2 +-induced oxidative stress in HeLa cells, zebrafish and mice models

Meiqing Zhu,Manjie Chen,Xinfu Zhu,Xingyu Zhu,Rimao Hua,Xiaofan Yang,Saraschandra Naraginti,Yi Wang

Hg 2+ -induced oxidative stress is an important pathway mediating biotoxicity, and the dynamics of reactive oxygen/nitrogen species (ROS/RNS) is a key indicator for quantitatively assessing the level of oxidative stress. Herein, a novel “targeted dual recognition” NIR fluorescent chemosensor (DDPT) was constructed for the specific recognition of Hg 2+ and ONOO - . The DDPT activated by Hg 2+ for the detection of ONOO - exhibited rapid response (<50 s), high sensitivity (16.8 nM) and excellent selectivity. The P = S bond in DDPT is oxidized to P = O by Hg 2+ , followed by ONOO - the specific attack on the P-O bond to break it, releasing the DDPT-OH to generate a significant fluorescence enhancement (with a Stokes shift up to 188 nm). The response mechanism of DDPT was systematically verified by 1 HNMR, HRMS and DFT theoretical calculations. Furthermore, DDPT was successfully evaluated for imaging Hg 2+ -induced ONOO - dynamics in cellular, zebrafish and mouse models due to its advantages of low cytotoxicity, high tissue permeability and biocompatibility. The results reveal that Hg 2+ induces oxidative stress and increases ONOO - concentration to destroy the antioxidant defense system of organisms, thus triggering the toxic pathway of oxidative stress. The development of DDPT provides a basis for analyzing pollutant-oxidative stress interactions, assessing health risks, and developing targeted intervention strategies.

研究领域: 生物化学 · 毒理学 · 医学影像
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Asia-Pacific Journal of Chemical Engineering · 2012 ·Vol. 8 ·期 4 ·567-577 · IF 0.758

The effect of Ca on distribution of nitrogen species during coal pyrolysis in N2, CO2 and Ar atmospheres

Ying Gu,Xiaowei Liu,Bo Zhao,Wenqiang Liu,Minghou Xu

Nitrogen species distribution during coal pyrolysis with Ca addition in N 2 , CO 2 and Ar was studied at 1000 °C using a horizontal tube furnace. In particular, the effect of Ca on the distribution of nitrogen species in N 2 and CO 2 atmospheres, which were closer to pyrolysis processes of conversional air and oxy-fuel combustion in comparison with inert Ar environment, was investigated for the first time in this work. It was found that Ca has a great effect on nitrogen species distribution during both coal and demineralized coal pyrolysis; on the other hand, CO 2 causes the formation of NO. Demineralization increases the formation of HCN and char nitrogen, but there is little effect on NH 3 formation during pyrolysis in N 2 , in contrast to pyrolysis in Ar atmosphere, which decreases NH 3 formation. A significant reduction in char yield was found after char gasification in CO 2 at 1000 °C. With two different Ca-based additives, i.e., (CH 3 COO) 2 Ca and Ca(OH) 2 , char yield decreases with the increasing amount of Ca additives in both cases. The effect of Ca on HCN and NH 3 formation during pyrolysis depends on both the form of Ca and the amount of addition. In most cases, HCN and NH 3 formation decreases with Ca addition in Ar, but increases in N 2 . Ca addition slightly promotes HCN formation during pyrolysis in CO 2 . There is no NH 3 detected during pyrolysis in CO 2 because of the reaction of NH 3 and CO 2 in the background. In addition, NO concentration decreases sharply with increasing the amount of Ca addition in the atmosphere of CO 2 , which means that Ca has an effect not only on pyrolysis, but also on gasification of char in CO 2 . In most cases, char nitrogen increases with Ca addition in N 2 or Ar. © 2012 Curtin University of Technology and John Wiley & Sons, Ltd.

CAS / MDL: 1305-62-0
研究领域: 能源科学 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Toxic effects and metabolic fate of carbamazepine in diatom Navicula sp. as influenced by humic acid and nitrogen species

Tengda Ding,Kunde Lin,Bo Yang,Menting Yang,Juying Li

Carbamazepine (CAB) is a commonly detected pharmaceutical in the surface waters. In the present study, we evaluated the effect of humic acid (HA) and nitrogen species on the toxicity of CAB in a typical diatom Navicula sp., and its metabolic fate. The Navicula sp. showed a high sensitivity to CAB (72 h EC 50 = 0.179 mg L −1 ). The addition of HA (< 30 mg L −1 ) and ammonium could promote the growth of Navicula sp. during 6 d of exposure to CAB. CAB underwent rapid dissipation in the algal culture. The degradation of CAB in Navicula sp. cultures was significantly increased by the addition of HA and higher HA contents caused more degradation of CAB. Degradation and accumulation of CAB in Navicula sp. were significantly inhibited by ammonium. Five metabolites were found and possible degradation pathways of CAB in the algal cell were proposed. Methoxylation, demethylation, glucuronidation and hydroxylation contributed to CAB transformation in the algal cell.

CAS / MDL: 7647-01-0
研究领域: 环境科学 · 毒理学 · 药理学
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

CdMn Bimetallic Complex-Derived Manganese–Nitrogen Species as Electrocatalysts for an Oxygen Reduction Reaction

Heng Liu,Qiulin Li,Bing-Huan Zhang,Long-Cheng Zhang,Guo-Rong Hou,Maowen Xu,Shu-Juan Bao

Fe–N–C catalysts exhibit promising activity toward the catalytic oxygen reduction reaction (ORR). However, applicability of such catalysts is limited by serious oxidative corrosion via the Fenton reaction. In this feature work, we prepared manganese–nitrogen species by pyrolyzing a bimetal CdMn and P-phenylenediamine organic complex (CdMn–PPD) under different atmospheres for the first time. The experimental results suggest that the carbonized atmosphere deeply affects the graphitization degree, pore structure of carbon, and the formation of Mn–N active sites. Of the three prepared catalysts, Mn@NPC–NH3 exhibited the greatest Mn–N and pyridinic N content and delivered excellent ORR activity (Eonset: 0.95 V, E1/2: 0.83 V). Even more impressive, the Fenton reaction was substantially restrained by this catalyst. Overall, the Mn@NPC–NH3 offers superior stability to that of Fe–N–C catalysts, providing new insight for further explorations of excellent non-noble metal ORR catalysts.

研究领域: 材料科学 · 电化学
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INORGANIC CHEMISTRY · 2021 · IF 5.165

B,N-Codoped Porous C with Controllable N Species as an Electrode Material for Supercapacitors

Zhenyu Zhao,Zuoyi Xiao,Yaru Xi,Guoxiang Wang,Youchen Zhang,Jiajun Li,Li Wei

Manufacturing heteroatom-doped porous C with controllable N species is an important issue for supercapacitors. Herein, we report a low-cost and simplified strategy for synthesizing B,N-codoped porous C (BNPC) by a freeze-drying chitosan–boric acid aerogel beads and subsequent carbonization treatment. The BNPC samples were studied using various characterization technologies. The introduction of boric acid to chitosan successfully induced the formation of B,N-codoped C with a well-developed 3D interconnected porous structure. The B doping had a significant impact on the distribution of N species in the samples. Moreover, the good wettability of the sample resulting from B doping is favorable for electrolyte diffusion and ion transport. As a consequence, the optimal BNPC sample showed an excellent specific capacitance of 240 F g–1 at 0.5 A g–1 and an outstanding capacitance retention of 95.1% after 10000 cycles at 5 A g–1. An assembled symmetrical supercapacitor displayed an energy density of 11.4 Wh kg–1 at a power density of 250 W kg–1. The proposed work provides a simple and effective method to obtain B,N-codoped C-based materials with high electrochemical performance.

CAS / MDL: 9012-76-4
研究领域: 材料科学 · 能源存储
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Science China-Chemistry · 2022 ·Vol. 65 ·期 12 ·2476-2486 · IF 10.138

Sulfur-induced dynamic reconstruction of iron-nitrogen species for highly active neutral oxygen reduction reactions

Wang Wenjie,Zhou Tianpei,Zhang Kai,Wang Chun,Shi Xiang,Wang Lin,Liu Qinghua,Wang Yang,Jiao Qiyang,Ma Guixin,Ye Chen,Xie Yi,Wu Xiaojun,Chu Wangsheng,Wu Changzheng

The neutral oxygen reduction reaction (ORR) has attracted tremendous attention for its broad prospects in next-generation power storage systems. However, the extremely sluggish cathodic reaction process and the limited cognition of the reaction mechanism greatly hinder its practical application. Here, we demonstrate a dynamic reconstruction behavior induced by sulfur of the iron-nitrogen (Fe-N x ) species in neutral solution. Our developed FeS 1 N 3 -OH configuration effectively optimizes the reaction kinetics by regulating the adsorption energy of oxygen intermediates for central catalytic sites. Consequently, this structure exhibits over 363% enhancement in ORR mass activity compared to the pristine FeN 4 sites under neutral electrolyte. Moreover, a neutral zinc-air battery assembled with this electrocatalyst reached an ultrahigh peak power density (81.2 mW cm −2 ), robust stability (more than 100 h) as well as superior tolerance to extreme environments (operating between −20 °C and 60 °C), representing a critical breakthrough for neutral ORR exploration and application.

CAS / MDL: 16009-13-5 62-56-6
研究领域: 材料科学 · 电化学 · 能源技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Reactive oxygen/nitrogen species scavenging and inflammatory regulation by renal-targeted bio-inspired rhodium nanozymes for acute kidney injury theranostics

Yue Zheng,Huixi Yi,Zhixiong Zhan,Shan-Shan Xue,Guosheng Tang,Xiyong Yu,Dong-Yang Zhang

Acute kidney injury (AKI) results from the rapid deterioration of renal function, which is mainly treated by transplantation and dialysis, and has a high mortality rate. Inflammation induced by excess reactive oxygen/nitrogen species (RONS) plays a crucial role in AKI. Although small molecule antioxidants have been utilized to alleviate AKI, low bioavailability and side-effect of these drugs tremendously limit their clinical use. Hence, we successfully construct ultra-small (2–4 nm) rhodium nanoparticles modified with l -serine (denoted as Rh-Ser). Our results show that Rh-Ser with multiple enzyme-mimicking activities, allows remove various RONS to protect damaged kidney cells. Additionally, the ultrasmall size of Rh-Ser is conducive to enrichment in the renal tubules, and the modification of l -serine enables Rh-Ser to bind to kidney injury molecule-1, which is highly expressed on the surface of damaged renal cells, thereby targeting the damaged kidney and increasing the retention time. Moreover, Rh-Ser allows the production of oxygen at the inflammatory site, thus further improving hypoxia and inhibiting pro-inflammatory macrophages to relieve inflammation, and increasing the survival rate of AKI mice from 0 to 80%, which exhibits a better therapeutic effect than that of small molecule drug. Photoacoustic and fluorescence imaging can effectively monitor and evaluate the enrichment and therapeutic effect of Rh-Ser. Our study provides a promising strategy for the targeted treatment of AKI via RONS scavenging and inflammatory regulation.

研究领域: 医学 · 生物材料学 · 纳米医学
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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
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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
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