Journal of Water Process Engineering
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2024
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IF 6.3
Xu-Dong Miao,Rui-Xiang Zhang,Wen-Tao Li,Qian Wang,Yu-Han Cai,Yong Guo,Ai-Min Li
The increasing environmental risks associated with tetracycline (TC) have been of widespread interest in the development of adsorbents for the efficient treatment of TC. This work synthesized a high-performance boron carbonitride (BCN v O) with nitrogen-vacancies (N v ) and oxygen-doping (O d ) via a hydrogen peroxide mediated strategy. The adsorption capacity of BCN v O-1 for TC (202.85 mg/g) is 1.79 times higher than that of BCN (113.08 mg/g). The adsorption process is well described by the pseudo-second-order kinetic and controlled by surface and intra-pore diffusion. Langmuir can well characterize isothermal adsorption with the fitted maximum adsorption up to 440.53 mg/g. Thermodynamics indicates a spontaneous and endothermic progress in BCN v O-1 adsorption. The abundant pore structures promote pore filling of TC by BCN v O-1. N v and O d enhance BCN v O-1 proton capture, and the captured protons strengthen hydrogen bonding and electrostatic interactions during adsorption. The functional groups, aromatic regions, and B N rings on BCN v O-1 are involved in hydrogen bonding and π-π stacking to TC. BCN v O-1 has high adsorption performance, great environmental appropriateness and thermal regeneration performance, suggesting good prospects for its potential application in environmental wastewater treatment.
研究领域:
环境科学
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材料科学
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高影响因子
Journal of Physical Chemistry C
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2021
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IF 4.126
Jing Wang,Sisi Fan,Hongmin Duan,Jinming Xu,Yanqiang Huang
Carbon spheres with hierarchical pore structure were successfully synthesized by using strongly basic anion exchange resins exchanged with silicate, followed by pyrolysis in an inert atmosphere and etching silica. As a result of the quaternary ammonium group in the anion exchange resin structure, these carbon spheres were doped with nitrogen. The performance of these carbon spheres in the catalytic dehydrochlorination of 1,2-dichloroethane (EDC) was improved with the increase of calcination temperature, and the carbon sphere 900-900-RC showed the highest conversion rate (96.7%) and a selectivity to vinyl chloride above 99%. The structural and surface properties of N-doped carbon spheres were characterized by scanning electron microscopy, nitrogen sorption, and Raman and X-ray photoelectron spectroscopy. The result of these characterizations further verified that the quaternary nitrogen species are as effective as pyridine nitrogen species in this catalyst.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Junyu Fan,Meimei Zuo,Zhaoxia Ding,Zhiwei Zhao,Jie Liu,Bo Sun
A promising and practicable catalyst is the key challenge for industrial perspective to promote photocatalytic nitrogen fixation. In this study, a new 0D /2D heterojunction, oxygen vacancy-induced In(OH) 3 /carbon nitride (OV-In(OH) 3 /CN), was synthesized by generating In(OH) 3 nanoparticles on g-C 3 N 4 nanosheets in the presence of glyoxal through a facile and readily precipitation growth method at 60℃and under atmospheric pressure. The existence of oxygen vacancies, structure, morphology and optical-electronic properties of the composite were characterized by HRTEM, XPS and EPR analysis and other measurements. The OV-In(OH) 3 /CN heterojunction exhibited excellent photocatalytic activity for nitrogen fixation with a good chemical stability. The OV-In/CN-3 sample reached the maximum NH 3 generation rate to be 3.81 mM*h −1 *g −1 , which was about 10 times as that of pure g-C 3 N 4 and was also higher than that of other catalysts reported. Though the In(OH) 3 in heterojunction was demonstrated incapable of producing photogenerated electrons under vis-light irradiation, its oxygen vacancy was found to “receive” and “trap” some excited electrons from g-C 3 N 4 , promoting electron-hole pairs separation efficiency and prolonging the lifetime of carriers. And it also can introduce many chemisorption sites for N 2 . Those are the two key reasons for its high photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
RSC Advances
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2020
·Vol. 11
·期 2
·700-710
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IF 3.119
Shurong Gao,Jiaxin Jin,Masroor Abro,Ruozhen Song,Miao He,Xiaochun Chen
Extractive denitrification (EDN) of shale oil using ionic liquids (ILs) as the extracting agent has good industrial prospects. In such processes, ILs with higher selectivity to N-compounds and lower solubility in shale oil are desired to improve the EDN efficiency, and reduce the loss of ILs and the contamination of shale oil. In the present study, we employed COSMO-RS to calculate the selectivity of 70 ILs to the typical N-compounds (pyridine, quinoline and indole). The influence of the IL structural characteristics, composition of shale oil and properties of N-compounds are investigated from a micro-level view with the σ-surface and σ-profile. The selectivity strongly depends on anionic species and it is greatly influenced by hydrogen bonding (HB) and π–π interaction between N-compounds and ILs. ILs composed of [H2PO4]− and [MeSO3]− with larger HB donor energy show higher selectivity to the basic N-compounds, while ILs composed of [Ac]− with larger π-electron cloud density show higher selectivity to the non-basic N-compounds. Anions with stronger polarity have lower solubility in shale oil. Moreover, experimental determinations of EDN indicated that [C4py][H2PO4]/[C4mim][H2PO4] and [C2mim][Ac]/[C2py][Ac] have good EDN performance for quinoline/pyridine with efficiency of 100% and for indole with efficiency of 91%, respectively. This work presents a theoretical basis to design and select ILs having higher selectivity for N-compounds and lower solubility in shale oil for use in denitrification.
研究领域:
化学工程
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材料科学
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PubMed
高影响因子
Insects
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2021
·Vol. 12
·期 6
·507
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IF 2.769
Yan Lu,Shouyu Zhang,Shibo Sun,Minghuo Wu,Yongming Bao,Huiyan Tong,Miaomiao Ren,Ning Jin,Jianqiang Xu,Hao Zhou,Weiping Xu
Simple SummaryBlack soldier fly larvae (BSFL) have received global research interest and industrial application due to their high performance on the organic waste treatment. However, the substrate C/N property, which may affect larvae development and the waste bioconversion process greatly, is significantly less studied. The current study focused on the food waste treatment by BSFL, compared the nitrogen supplying effects of 9 nitrogen species (i.e., NH4Cl, NaNO3, urea, uric acid, Gly, L-Glu, L-Glu:L-Asp (1:1,w/w), soybean flour, and fish meal), and further examined the C/N effects on the larval development and bioconversion process. We found that NH4Cl and NaNO3led to poor larval growth and survival, while 7 organic nitrogen species exerted no harm to the larvae. Urea was further chosen to adjust the C/Ns. Results showed that lowering the C/N from the initial 21:1 to 18:1–14:1 improved the waste reduction and larvae production performance, and C/N of 18:1–16:1 was further beneficial for the larval protein and lipid bioconversion, whereas C/N of 12:1–10:1 resulted in a significant performance decline. Therefore, the C/N range of 18:1–16:1 is likely the optimal condition for food waste treatment by BSFL and adjusting food waste C/N with urea could be a practical method for the performance improvement.AbstractBiowaste treatment by black soldier fly larvae (BSFL,Hermetia illucens) has received global research interest and growing industrial application. Larvae farming conditions, such as temperature, pH, and moisture, have been critically examined. However, the substrate carbon to nitrogen ratio (C/N), one of the key parameters that may affect larval survival and bioconversion efficiency, is significantly less studied. The current study aimed to compare the nitrogen supplying effects of 9 nitrogen species (i.e., NH4Cl, NaNO3, urea, uric acid, Gly, L-Glu, L-Glu:L-Asp (1:1,w/w), soybean flour, and fish meal) during food waste larval treatment, and further examine the C/N effects on the larval development and bioconversion process, using the C/N adjustment with urea from the initial 21:1 to 18:1, 16:1, 14:1, 12:1, and 10:1, respectively. The food wastes were supplied with the same amount of nitrogen element (1 g N/100 g dry wt) in the nitrogen source trial and different amount of urea in the C/N adjustment trial following larvae treatment. The results showed that NH4Cl and NaNO3caused significant harmful impacts on the larval survival and bioconversion process, while the 7 organic nitrogen species resulted in no significant negative effect. Further adjustment of C/N with urea showed that the C/N range between 18:1 and 14:1 was optimal for a high waste reduction performance (73.5–84.8%,p< 0.001) and a high larvae yield (25.3–26.6%,p= 0.015), while the C/N range of 18:1 to 16:1 was further optimal for an efficient larval protein yield (10.1–11.1%,p= 0.003) and lipid yield (7.6–8.1%,p= 0.002). The adjustment of C/N influenced the activity of antioxidant enzymes, such as superoxide dismutase (SOD,p= 0.015), whereas exerted no obvious impact on the larval amino acid composition. Altogether, organic nitrogen is more suitable than NH4Cl and NaNO3as the nitrogen amendment during larval food waste treatment, addition of small amounts of urea, targeting C/N of 18:1–14:1, would improve the waste reduction performance, and application of C/N at 18:1–16:1 would facilitate the larval protein and lipid bioconversion process.Keywords:nitrogen source;carbon to nitrogen ratio;food waste;urea;black soldier fly larvae;Hermetia illucens
研究领域:
环境科学
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昆虫学
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废弃物处理
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Jing Ding,Wei Xu,Hui Wan,Dashui Yuan,Chong Chen,Lei Wang,Guofeng Guan,Wei-Lin Dai
Vacancy defect in the semiconductors plays an important role in the improvement of the electronic structure and the increase of specific reaction sites for reactant molecules, and consequently enhancing the photocatalytic activity of semiconductor photocatalysts. Through high-temperature thermal condensation of a nitric acid-pretreated melamine precursor, nitrogen vacancies were successfully introduced in the framework of g-C 3 N 4 . The nitrogen vacancies located at the uncondensed terminal NH x lattice sites were conducive to the enhancement of optical absorption, the improvement of the separation efficiency of the photogenerated charge carrier and the increase of surface area, which was beneficial to the photocatalytic oxidation process. More significantly, the novel CNNA(X) were used as efficient photocatalysts in the green process of aromatic aldehydes from the photocatalytic selective oxidation of aromatic alcohols and the photocatalytic degradation of organic pollutants. CNNA(X) samples exhibited enhanced photocatalytic activity and excellent recyclability and stability. The 68.3% benzyl alcohol conversion and almost 100% selectivity was observed for the CNNA (0.9) photocatalyst, higher than that of pure g-C 3 N 4 . Meanwhile, CNNA (0.9) showed superior photocatalytic degradation performance of organic dyes (RhB and MO). Furthermore, the underlying photocatalytic oxidation mechanism was proposed by the controlled experiments using radical scavengers.
研究领域:
材料科学
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环境科学
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化学工程
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高影响因子
Nanoscale
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2017
·Vol. 9
·期 44
·17593-17600
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IF 7.367
Min Wang,Xiangqian Fan,Lingxia Zhang,Jianjun Liu,Beizhou Wang,Ruolin Cheng,Mengli Li,Jianjian Tian,Jianlin Shi
Porous activated carbons (PACs) are promising candidates to capture CO2 through physical adsorption because of their chemical stability, easy-synthesis, cost-effectiveness and good recyclability. However, their low CO2 adsorption capacity, especially low CO2/N2 selectivity, has limited their practical applications. In this work, an optimized PAC with a large specific surface area, a small micropore size, and a large micropore volume has been synthesized by one-step carbonization/activation of casein using K2CO3 as a mild activation agent. It showed a remarkably enhanced CO2 adsorption capacity as high as 5.78 mmol g−1 and an excellent CO2/N2 selectivity of 144 (25 °C, 1 bar). Based on DFT calculations and experimental results, the coexistence of adjacent pyridinic N and –OH/–NH2 species was proposed for the first time to make an important contribution to the ultra-high CO2 adsorption performance, especially CO2/N2 selectivity. This work provides effective guidance to design PAC adsorbents with high CO2 adsorption performance. The content of pyridine N combined with –OH/–NH2 was further elevated by additional nitrogen introduction, resulting in a further enhanced CO2 adsorption capacity up to 5.96 mmol g−1 (25 °C, 1 bar). All these results suggest that, in addition to the well-defined pore structure, pyridinic N with neighboring OH or NH2 species played an important role in enhancing the CO2 adsorption performance of PACs, thus providing effective guidance for the rational design of CO2 adsorbents.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2019
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IF 5.383
Haoqing Ji,Mengfan Wang,Sisi Liu,He Sun,Jie Liu,Tao Qian,Chenglin Yan
Pyridinic and graphitic nitrogen are recognized as the most promising dopants for promoting oxygen reactions since they are beneficial to the formation of corresponding C–N bonds as efficient active sites. However, complete control of such efficient nitrogen-doping sites in carbon materials is difficult to realize in practice in a pyrolysis process . Here, we present maximized pyridinic and graphitic nitrogen-doped oxygen electrode via the precise use of nitrogen-containing precursors and carbonization temperature. The critical roles of pyridinic and graphitic nitrogen dopants in enhancing oxygen reaction activity are unraveled and this highly active material exhibits a remarkable half-wave potential of 0.89 V versus the reversible hydrogen electrode (vs. RHE) for oxygen reduction reaction (ORR) and a small potential gap of 0.78 V between ORR and oxygen evolution reaction (OER) in 0.1 M KOH, which is one of the best to date among metal-free bifunctional electrocatalysts . Both zinc-air batteries using liquid electrolytes and the all-solid-state batteries assembled with such air cathodes exhibit excellent cycle performance and reversibility, which can be expressly observed by in-situ X-ray diffraction (XRD) characterization. This nitrogen dopants engineering strategy gives an effective methodology to make full use of nanocarbon materials for their practical applications in next-generation powerful and durable energy devices.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CARBON
·
2022
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IF 11.307
Jun Wan,Guoqun Zhang,Hongrun Jin,Jiabin Wu,Nian Zhang,Bin Yao,Kaisi Liu,Meilin Liu,Tonghuan Liu,Liang Huang
While nitrogen (N)-doped carbon can facilitate the four-electron transfer in oxygen reduction reaction (ORR), its effect on the two-electron path is yet to be investigated. To date, the random N-C bond configurations in N-doped carbons make it difficult to identify the active sites for electrochemical reactions . Here, we report a preparation of well-controlled N-C configurations with high centrality as model catalysts for identification of active sites for two-electron transfer ORR. Specifically, the synthesized Pyrrolic-N doped single-wall carbon nanotube and graphene utilizing a microwave-assisted pulse heating method, exhibit excellent activity for two-electron path (H 2 O 2 selectivity of 93.5% and 98.35%). X-ray adsorption near-edge structure spectroscopy measurements indicate that carbon atoms adjacent to Pyrrolic-N are the active sites for two-electron transfer. This work provides a viable way for the fabrication of tailored N configurations in carbon materials and significantly advances our understanding of the N moieties for the electrochemical H 2 O 2 generation.
研究领域:
材料科学
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电化学
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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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
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化学工程
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
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2021
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IF 8.071
Na Liu,Qing Hu,Chao Wang,Lizhi Tong,Chih-Huang Weng,Longzhen Ding
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The k obs values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid . Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
研究领域:
环境科学
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催化化学
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DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2023
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IF 3.7
Song Chen,Yulong He,Siyu Ding,Jintao Zhang
To address the low capacity and poor stability of aqueous zinc–iodine batteries owing to the insulating nature of iodine and the shuttle effect of polyiodide, herein, tungsten nitride-modified porous carbon polyhedron (W2N/N-C) was prepared via the pyrolysis of ZIF-8 injected with phosphotungstic acid (PTA@ZIF-8). During the thermal treatment process, the self-nitridation enabled the in situ formation of tungsten nitride nanoparticles in hierarchical porous carbon with nitrogen doping for favorable loading of iodine. When used as the electrode material, the zinc–iodine battery exhibited the low polarization during the charge/discharge process with improved reversibility and good cycling stability for 2000 cycles. The improved electrochemical performance would be attributed to the confinement effect of W2N/N-C for the reversible conversion between iodine and polyiodide, thus enhancing the redox reversibility and utilization of active materials. The present work demonstrates an efficient strategy to prepare porous carbon with metal nitrides via the combination of carbonization and self-nitridation process for high-performing zinc–iodine battery.
研究领域:
材料科学
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电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）