CHEMOSPHERE
·
2023
·
IF 8.8
Le Zhang,Yong Liu,Jianlong Wang
The oxidation of ammonium (NH 4 + ) to dinitrogen (N 2 ) with high selectivity and high efficiency is still a challenge. Herein, a novel sunlight induced persulfate (PS)-based AOPs process (MgO/Na 2 SO 3 /PS/ hv ) was proposed by introducing solid base (MgO) and hydrated electron (e aq − ), to selectively oxidize NH 4 + to N 2 , with high selectivity and high efficiency at a wide range of pH value. The deprotonation of NH 4 + into NH 3 by MgO and the generation of •OH and SO 4 −• by PS activation were responsible for the high efficiency of NH 4 + oxidation. The buffering capacity provided by MgO to proton released from PS activation made the NH 4 + oxidation possible at a wide pH range. The e aq − from the Na 2 SO 3 / hv process was the main active specie to reduce NO 2 − and NO 3 − (NO x − ) into N 2 , responsible for high N 2 selectivity of NH 4 + oxidation. 100% NH 4 + could be oxidized within 30 min, and N 2 selectivity exceeded 96% at the initial pH range of 3–11 and the initial concentration of NH 4 + of 30 mg N/L. This work could offer an efficient AOPs process for selective NH 4 + oxidation, which is promising for the chemical denitrification of wastewater ….
研究领域:
环境科学
·
化学工程
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DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Xinyuan Ma,Haobo Bai,Guoxue Li,Lingling Li,Haofeng Meng,Yan Liu,Jing Yuan
In order to reduce N 2 O emissions during composting, the effects of different nitrification inhibitors (NI), dicyandiamide (DCD) and 3,4-dimethylpyrazole phosphate (DMPP), on compost maturity, N 2 O, and NH 3 emissions were studied under continuous incremental addition. This study used pig manure and corn straw as composting materials, based on the total nitrogen (TN) content of the initial mixture, two treatments were set: DCD (2.5% in the early phase and 5.0% in the maturation phase) and DMPP (0.25% in the early phase and 0.75% in the maturation phase) in a composting experiment. The results showed that adding DCD and DMPP did not affect the compost maturity, with the seed germination index (GI) of final compost reaching 80.76%–97.06%. Before the maturity period of compost, ammonia (NH 3 ) emissions accounted for 98.5%–99.4% of total emissions. Compared with the control group (CK), the addition of DCD and DMPP in the early stage reduced NH 3 emissions by 8.85% and 12.83%, respectively, by decreasing the ammonification rate. During the mature stage of composting, N 2 O emissions account for 95.6%–98.9% of the total emissions. The addition of DCD and DMPP delayed N 2 O emissions by 4 and 6 days, respectively, through nitrification inhibition. The DMPP amendment also reduced cumulative N 2 O emissions by 54.50% and increased the nitrogen content of the final compost. Correlation analysis showed that N 2 O was mainly originated from the denitrification of nitrification substrate (NO 2 − -N and NO 3 − -N). This study provides technical support for low-carbon management of agricultural waste.
研究领域:
环境科学
·
农业生态学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Haohong Xian,Haoran Guo,Jiaojiao Xia,Qiru Chen,Yonglan Luo,Rui Song,Tingshuai Li,Enrico Traversa
Nitrogen can be electrochemically reduced to produce ammonia, which supplies an energy-saving and environmental-benign route at room temperature, but high-efficiency catalysts are sought to reduce the reaction barrier. Here, iron-doped α-MoO3 nanosheets are thus designed and proposed as potential catalysts for fixing N2 to NH3. The α-MoO3 band structure is intentionally modulated by the iron doping, which narrows the band gap of α-MoO3 and turns the semiconductor into a metal-like catalyst. Oxygen vacancies, generated by substituting Mo6+ for Fe3+ anions, are beneficial for nitrogen adsorption at the active sites. In 0.1 M Na2SO4, the Fe-doped MoO3 catalyst reached a high faradaic efficiency of 13.3% and an excellent NH3 yield rate of 28.52 μg h–1 mgcat–1 at −0.7 V versus reversible hydrogen electrode, superior to most of the other metal-based catalysts. Theoretical calculations confirmed that the N2 reduction reaction at the Fe–MoO3 surface followed the distal reaction path.
研究领域:
材料科学
·
环境科学
·
化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yong Liu,Le Zhang,Ting Liu,Jianlong Wang
The selective oxidation of ammonium nitrogen (NH 4 + -N) to dinitrogen (N 2 ) by advanced oxidation processes (AOPs) is of paramount significance, but it is still a great challenge. In this study, a novel composite (FeO x -MgO) was synthesized to activate persulfate (PS) for selective oxidation of ammonium (NH 4 + ) to N 2 under simulated solar-light irradiation ( hv ). The results demonstrated that the conversion of NH 4 + to ammonia (NH 3 ) on the basic sites of FeO x -MgO was a key step for the selective oxidation of NH 4 + . Fe(IV) species formed in FeO x -MgO/PS/ hv system could enhance both the efficiency and N 2 selectivity of the NH 4 + -N oxidation through the oxidation of ammonia hydride to N 2 . The 100 % NH 4 + -N removal and over 95.5 % N 2 selectivity could be achieved after 30 min when initial pH was in range of 2–10, and the initial NH 4 + -N concentration was 30 mg N/L. This study could provide a promising technology for the selective oxidation of NH 4 + -N to N 2 in water and wastewater.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Xinyu Liu,Jianlong Wang
The selective oxidation of ammonia to dinitrogen gas in some special wastewater is of paramount significance, but still a challenge. In this study, chlorine radical (Cl•)-mediated oxidation process was developed to realize the selective oxidation of NH 4 + -N to N 2 , in which Cl• was generated in Co 2+ /peroxymonosulfate (PMS)/chloridion (Cl − ) system. The effect of various operational parameters on the efficiency and selectivity of ammonia oxidation to N 2 was investigated, such as PMS concentration, Co 2+ concentration, Cl − concentration and pH value. The experiment results showed that Cl•-mediated NH 4 + -N oxidation reaction exhibited high NH 4 + -N removal efficiency and considerable selectivity to N 2 in the range of pH from 2.0 to 6.5. The removal efficiency of NH 4 + -N was 90.39%, and the selectivity of NH 4 + -N to N 2 achieved up to 97.16%. The possible mechanism for high efficient and selective oxidation of NH 4 + -N to N 2 was tentatively proposed. The process developed in this study could provide a novel technology for the treatment and selective oxidation of ammonium in some special types of ammonium-containing wastewater.
研究领域:
环境科学
·
化学工程
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chunhong Fu,Song Shu,Lin Hu,Zixun Liu,Zhouyang Yin,Xiaoshu Lv,Sen Zhang,Guangming Jiang
Selective electrocatalytic nitrate reduction reaction (NO 3 RR) to dinitrogen (N 2 ) is essential to nitrogen-cycle management and environmental sustainability. Palladium-based nanomaterials were extensively studied as NO 3 RR catalysts, but only delivered limited N 2 selectivity (<50%, NH 3 dominated the product). Here we report that, by tuning bimetallic composition of CuPd alloy nanowires, the Cu 28 Pd 72 nanowires deliver a near-unit conversion of NO 3 – -N and an unprecedented N 2 product selectivity of 75.9 ± 5.2% in treating 22.5 mg L −1 NO 3 – -N solution at −0.80 V vs. Ag/AgCl. Combining in-situ spectrometric measurements and theoretical calculations, we demonstrate that the contiguous Pd ensemble with a specific size at catalyst surface is essential to the N 2 formation via a kinetically-favored pathway of NO 2 * → NO* → N* → N 2 *. Alloying Pd with Cu is indispensable as Cu contributes to the N*-N* pairing by initiating the NO 3 – –NO 2 * conversion and lowering the H ads coverage on catalyst. This work discloses the key surface atomic structure for N 2 formation, and provides a guideline for the design of efficient NO 3 RR catalyst that enables selective NO 3 – –N 2 conversion.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
MOLECULES
·
2021
·Vol. 26
·期 17
·5209
·
IF 4.412
Li Du,Shaonan Xu,Han Wu,Tengwen Zhao,Xuesheng Wang,Manman Wang
A novel diatomite-supported zeolitic imidazolate framework-8 sorbent (ZIF-8@Dt-COOH) was in situ fabricated and developed for solid-phase extraction of three benzodiazepines (triazolam, midazolam and diazepam) in urine followed by high-performance liquid chromatography. ZIF-8@Dt-COOH was easily prepared by coating ZIF-8 on the surface of Dt-COOH and characterized by Fourier transform infrared spectra, X-ray powder diffractometry and scanning electron microscopy. Compared with bare Dt-COOH, the extraction efficiency of ZIF-8@Dt-COOH for the target was significantly increased from 20.1–39.0% to 100%. Main extraction parameters, including ionic strength and pH of solution, loading volume, washing solution, elution solvent and elution volume, were optimized in detail. Under optimum conditions, the developed method gave linearity of three BZDs in 2–500 ng/mL (r≥ 0.9995). Limits of detection (S/N= 3), and limits of quantification (S/N= 10) were 0.3–0.4 ng/mL and 1.0–1.3 ng/mL, respectively. In addition, the average recoveries at three spiked levels (5, 10 and 20 ng/mL) varied from 80.0% to 98.7%, with the intra-day and inter-day precisions of 1.4–5.2% and 1.5–8.2%, respectively. The proposed method provided an effective purification performance and gave the enrichment factors of 24.0–29.6. The proposed method was successfully employed for the accurate and sensitive determination of benzodiazepines in urine.Keywords:benzodiazepines;diatomite;zeolitic imidazolate framework-8;solid-phase extraction;urine
研究领域:
分析化学
·
医学检测
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PubMed
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 23
·2201-2210
·
IF 2.524
Shiwei Wang,Bo Yan,Juan Chai,Tianhao Li,Hongbo Yu,Tong Li,Peng Cao,Fan Yang,Xuemin Yuan,Hongfeng Yin
Graphical A prominently size-dependent intrinsic catalytic activity or structure-sensitive catalysis in N 2 O decomposition appeared over Rh encapsulated within silicalite-1 (Rh@S-1). The size of metal species plays a pivotal role in governing catalytic performance of supported metal catalysts. In this work, a series of Rh encapsulated within silicalite-1 catalysts with different sizes were prepared by one-pot hydrothermal method and employed to catalyze the decomposition of N 2 O. Detailed structure determinations by HAADF-STEM, XPS and CO-DRIFTS demonstrate that subtle modulation of the encapsulated Rh species were achieved easily from single-atom to nanoclusters and nanoparticles by controlling the loading and reduction conditions of Rh. The turnover frequency (TOF) of N 2 O decomposition showed a typical volcano-type dependence on Rh size. Kinetic studies revealed that this structure-sensitive catalysis was related to the difference in N 2 O and O 2 adsorption/desorption for various Rh species. Furthermore, a Rh@S-1 catalyst with a proper Rh size (ca. 1.6 nm) was identified as the best-performing catalyst with a maximum TOF (ca. 95 h −1 ), showing much superior activity than other reported Rh-based catalysts.
研究领域:
化学
·
材料科学
·
催化反应
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Bo Zhang,Huaihao Xu,Han Zhang,Zhou Chen,Huiqun Shi,Shaohua Chen,Xiaojun Wang
Salinity is considered a major factor influencing nitrous oxide (N 2 O) emissions from biochemical treatment of high-salinity wastewater, but its mechanism has not been thoroughly investigated. In this study, we investigated the effects of salinity on N 2 O emissions under aerobic conditions. As salinity rose from 0.66 % to 3.66 %, N 2 O emission flux first increased and then decreased, while the emission factor (EF) consistently increased, likely due to significant inhibition of nitrification at 3.66 % salinity. Nitrogen‑oxygen dual isotope labeling experiments demonstrated that the dominant N 2 O production pathway shifted with salinity: from nitrifier nitrification (NN, 36.07 %–40.97 %) at low salinity (0.66 %, 1.66 %), to nitrification-coupled denitrification (NCD, 51.67 %) at 2.66 %, and to nitrifier denitrification (ND, up to 80.81 %) at the salinity of 3.66 %. From the changes in bacterial relative abundances and expressions of 4 key functional genes ( amoA , hao , nor , and nosZ ) revealed by metatranscriptomic sequencing, Nitrosomonas , unclassified Rhodospirillales , and Nitrospira were identified as key contributors to NN, NCD, and ND pathways, respectively, as salinity increased. We also found that the differential expressed genes and metabolites involved in energy metabolism, oxidative phosphorylation, and metabolism of amino acids, pyrimidines, and nucleotides may affect N-cycling bacteria, thereby influencing nitrogen conversion and salinity tolerance as well. This study sheds light on nitrification process in response to salinity stress and offers insights for mitigating greenhouse gas emissions from high-salinity wastewater treatment.
研究领域:
环境科学
·
微生物学
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PubMed
高影响因子
Journal of Water Process Engineering
·
2022
·
IF 7.34
Mengyao Han,Luxin Liang,Yazi Wang,Yuwei Deng,Qiuyue Zhang,Yuxuan Ye,Dandan Wang,Qiang Li,Fei Pan,Dongsheng Xia
The effective control of antibiotic pollution in water has become an important issue in the field of environmental protection. In this study, the composite of iron sulfide and melamine sponge (FeS@MS) was successfully synthesized by in-situ synthesis method and applied to the oxidative removal of tetracycline (TC) in the presence of peroxymonosulfate (PMS). Under optimal conditions ([FeS@MS] = 0.1 g/L and [PMS] = 0.2 mM), 95.7% of TC was degraded in 5 min. The presence of NO 3 − , SO 4 2− , and Cl − slightly inhibited TC removal, whereas HPO 4 − had a certain promotion effect in activating PMS to degrade TC. The primary reactive oxygen species (ROS), including SO 4 − , OH , 1 O 2 , and O 2 − were identified through electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments. In addition, Fe 3+ in solution could react with FeS to produce Fe 2+ , which continuously activates PMS to generate radicals for TC degradation. The presence of MS reduced the agglomeration of FeS and played a protective role in the slow release of Fe 2+ . The degradation performance was further validated in real water matrices. This study provided new insight into fabricating functional material for the remediation of antibiotic wastewater.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
FERROELECTRICS
·
2020
·
IF 0.669
Jie Xing,Ming-Hong Wang,Song Wang,Hai-Lin Cong,You-Qing Shen,Bing Yu
In this paper, we report on a successful development and application of diazoresin (DR)/β-Cyclodextrin covalently linked capillary coatings using the layer by layer (LBL) self-assembly technique combined with photochemistry reactions. The modified capillary remarkably suppressed the protein adsorption on the inner surface of silica capillary and successfully separated lysozyme (Lys), myoglobin (Mb), bovine serum albumin (BSA) and ribonuclease A (RNase A). Furthermore, the DR/β-Cyclodextrin covalently linked capillary coatings showed good stability and repeatability. More importantly, this method is more environmentally friendly and simpler than traditional methods for the use of DR instead of highly toxic and moisture-sensitive silane coupling agent.
研究领域:
分析化学
·
生物化学
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产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Weixuan Yao,Zhefeng Fan,Suling Zhang
A poly( N -vinylcarbazole- co -divinylbenzene) (NVC/DVB) monolithic column was successfully prepared in a silanized capillary for microextraction of six benzodiazepines (BZPs) in complex samples. The polymerization was optimized primarily by changing the ratio of porogen content. The optimized polymer monolith had a homogeneous and continuous column bed, good permeability and mechanical stability. Poly(NVC/DVB) had good affinity to BZPs because of its through-pore structure and strong π-π stacking interactions derived from the rich benzene functional groups in the polymer. Potential factors that affect the extraction efficiency were studied in detail. In the optimized method, 3 mL of sample (pH 2) was extracted with the polymer monolithic column and eluted with 80 μL of methanol, and the eluent was analysed with ultra-high-performance liquid chromatography and quadrupole high resolution Orbitrap mass spectrometry (UHPLC/Q-Orbitrap MS). Under these conditions, the developed method gave the linear range of 0.005–0.5 ng/mL for most of the six BZPs, whereas 0.05–0.5 ng/mL for nitrazepam, 0.01–0.5 ng/mL for lorazepam, respectively, with coefficients of determination (R 2 ) ≥ 0.9991. The detection limits (LODs) were 1.08–6.04 ng/L, and the quantification limits (LOQs) were 3.60–20.1 ng/L. The method repeatability was investigated in terms of intra- and inter-day precision, which were indicated by relative standard deviations (RSDs) of ≤8.3% and ≤9.9%, respectively. Finally, the proposed method was successfully applied to detect BZPs in beer and human urine samples. The percentages of extraction recovery were 80.4–94.2% for beer and 79.6–95.2% for urine.
研究领域:
分析化学
·
药物分析
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DOI
PubMed
高影响因子
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