CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhiwei Zhao,Yu Li,Fei Wang,Zhitao Xu,Sai Zhang,Li Li,Junyu Fan,Jie Liu
Monitoring and regulating the formation of toxic byproducts in advanced oxidation processes (AOPs) is of great significance for their practical application in water treatment. In this work, we found that dichloroacetonitrile (DCAN), a common N-containing byproduct in chloramination disinfection, can be formed with the co-presence of g-C 3 N 4 and chloride in a peroxymonosulfate (PMS) system. The measured value was 12.01 μM within 12 h under the given conditions. Structure analysis of raw and used g-C 3 N 4 demonstrated that g-C 3 N 4 decomposition indeed occurred, and C = N bonds acted as primary active sites, releasing N resources for subsequent DCAN formation. Additionally, multiple parameters, including the reactant (i.e., g-C 3 N 4 , PMS, Cl - , phenol) dose and solution pH, were observed to remarkably affect the yield of DCAN. Phenol was identified as the organic precursor of DCAN and may cooperate with inorganic chloramine to promote DCAN formation via the decarboxylation pathway. This study highlights the generation of DCAN in N-involved catalyst-based AOPs and improves understanding of the DCAN formation mechanism.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Weihao Cong,Lin Zang,Mengting Pan,Liyuan Zhang,Yan Zhao,Weiheng Kong
Singlet oxygen ( 1 O 2 ), a highly reactive oxygen species, possesses significant utility in the domains of chemistry and materials science, with applications encompassing wastewater treatment, advanced battery fabrication and the degradation of organic pollutants. The generation of 1 O 2 is typically facilitated through specific processes such as photocatalytic reactions involving photosensitizers, electron transfer reactions, or enzymatic catalysis. The production of 1 O 2 is challenging and its reactivity is constrained, thereby limiting its generation and applications. This study aims to surmount these limitations by investigating the exceptional capacity of a nanomorphic copper phosphate (Cu 3 (PO 4 ) 2 ) to generate 1 O 2 in no need of light activation. A comprehensive characterization of the micromorphology, physical, and chemical properties of Cu 3 (PO 4 ) 2 was conducted to analyze and evaluate its structural and intrinsic characteristics. Systematic research on the kinetic simulation properties of Cu 3 (PO 4 ) 2 was undertaken to acquire experimental data pertaining to the efficiency and mechanism of the catalytic process, providing a scientific foundation for further optimizing its performance as a catalyst for 1 O 2 generation. This research may pave the way for the development of novel and efficient systems for the generation of effective 1 O 2 .
研究领域:
化学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
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IF 5.723
Yitao Zhao,Junjun Cheng,Peng Zhang,Xinhui Liu,Jianguo Zhuang,Yijun Yu,Qichao Zhao,Yuchen Wang,Xuedong Zhu,Fan Yang
Alkylation of benzene with carbon dioxide (CO 2 ) is significant for converting greenhouse gas and surplus benzene into value-added toluene and xylene. Herein, a bifunctional catalyst comprising Zn/Ga oxides and HZSM-5 zeolite was developed to efficiently promote the methylation of benzene with CO 2 and H 2 . This catalytic system exhibited excellent performance at 425 ℃ and 3.0 MPa, through which benzene conversion of 39.1% and total xylene/toluene selectivity of 92.7% have been achieved. Furthermore, the catalysts are carefully characterized; compositions of Zn/Ga oxides and Si/Al ratios of HZSM-5 zeolite are recognized as decisive factors for reaction activity and selectivity respectively. Additionally, primary reaction pathways are explored and testified to provide detailed understanding for the establishment of reaction networks, especially for mechanisms of ethylbenzene evolution. These findings are able to provide more deep insights into the process of benzene alkylation, which further facilitates the emergence of effective catalysts with potential industrial applications.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
RENEWABLE ENERGY
·
2023
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IF 8.7
Jinrui Guo,Fashe Li,Huicong Zhang,Yaozong Duan,Shuang Wang,Fangguan Tan,Yong Chen,Fengju Lu,Linglin Luo
The effect of fuel components and combustion parameters on the emission characteristics of aldehydes from biodiesel combustion is investigated, and the formation mechanism of aldehydes is revealed. The results show that CH 2 O and CH 3 CHO are the main aldehydes produced during biodiesel combustion. The rise in initial temperature and pressure reduces the formation of aldehydes, which accelerates the generation of reactive radicals to promote the oxidation of aldehydes. As the equivalence ratio decreases from 2.0 to 0.5, the concentrations of formaldehyde and acetaldehyde decrease from 444.58 to 438.19 μg/m 3 to 164.72 and 6.71 μg/m 3 , respectively, due to the oxidation and dilution effect of air on aldehydes. In addition, when the number of C C bonds in biodiesel is increased from 0 to 1, the concentrations of formaldehyde and acetaldehyde are enhanced by 117.89 % and 12.74 %, respectively, because of the reduction in the content of reactive radical H. The main formation pathway of aldehydes is as follows: Biodiesel is initially consumed via H-abstraction reactions by reactive radicals (OH, H, etc.) to produce primary fuel radicals, which mainly undergo β-decomposition to form key oxidation intermediates (C 4 H 6 , C 2 H 4 , C 2 H 3 , etc.). Consequently, these small molecular intermediates will be converted to aldehydes by oxidation and dehydrogenation reactions.
研究领域:
能源科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Shuchang Liu,Xi Yuan,Zhewen Shao,Kexin Xiang,Wenfang Huang,Hailin Tian,Feng Hong,Yingping Huang
Presently, the hydroxyl radical oxidation mechanism is widely acknowledged for the degradation of organic pollutants based on hydrodynamic cavitation technology. The presence and production mechanism of other potential reactive oxygen species (ROS) in the cavitation systems are still unclear. In this paper, singlet oxygen ( 1 O 2 ) and superoxide radical (·O 2 − ) were selected as the target ROS, and their generation rules and mechanism in vortex-based hydrodynamic cavitation (VBHC) were analyzed. Computational fluid dynamics (CFD) were used to simulate and analyze the intensity characteristics of VBHC, and the relationship between the generation of ROS and cavitation intensity was thoroughly revealed. The results show that the operating conditions of the device have a significant and complicated influence on the generation of 1 O 2 and ·O 2 − . When the inlet pressure reaches to 4.5 bar, it is more favorable for the generation of 1 O 2 and ·O 2 − comparing with those lower pressure. However, higher temperature (45 °C) and aeration rate (15 (L/min)/L) do not always have positive effect on the 1 O 2 and ·O 2 − productions, and their optimal parameters need to be analyzed in combination with the inlet pressure. Through quenching experiments, it is found that 1 O 2 is completely transformed from ·O 2 − , and ·O 2 − comes from the transformation of hydroxyl radicals and dissolved oxygen. Higher cavitation intensity is captured and shown more disperse in the vortex cavitation region, which is consistent with the larger production and stronger diffusion of 1 O 2 and ·O 2 − . This paper shed light to the generation mechanism of 1 O 2 and ·O 2 − in VBHC reactors and the relationship with cavitation intensity. The conclusion provides new ideas for the research of effective ROS in hydrodynamic cavitation process.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
COMBUSTION AND FLAME
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2023
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IF 4.4
Jinglan Wang,Dandan Xu,Xuezhi Gao,Qiang Xu,Zhandong Wang,Jiuzhong Yang,Lili Xing,Junyu Tao,Beibei Yan,Guanyi Chen,Zhanjun Cheng
N-methyl pyrrole (NMP) is an important nitrogenous heterocyclic compound in bio-oils produced from biomass conversion . NMP can be used as surrogate model compound to clarify the combustion chemistry of nitrogenous fuels and NO X formation mechanism. The low- to moderate-temperature oxidation experiments of NMP are carried out in atmospheric pressure jet-stirred reactor for 0.5% NMP/oxygen/Argon mixtures at different equivalence ratios (0.5, 1.0, and 2.0) over the temperature range of 760 – 1030 K. More than twenty species, including reactants, nitrogen-containing species, and oxygenated products, are measured using synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). A detailed and comprehensive kinetic model for NMP oxidation is developed for the first time based on the pyrrole oxidation model developed by Pelucchi et al. and Chen et al.. Simulated results show that the present model can reasonably reproduce the experimental results. Rate of production analysis indicates that the H-abstraction reactions on the methyl group dominate in NMP oxidation at all equivalence ratios. NMP oxidation produces C4 and C5 nitrogen-containing compounds including pyridine and pyrrole. These species are found to be products of the primary reactions of NMP, and their formation pathways can be explained satisfactorily by the present model. The present work provides a basis to further understand the oxidation characteristics of nitrogen-containing heterocyclic fuels.
研究领域:
能源化学
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燃烧科学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2019
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IF 0
Wangwei Chen,Juanjuan Qi,Chao Dong,Junwei Chen,Zhitao Shen,Yonglin He,Shangfeng Yang,Tao Chen,Chong Chen,Yunliang Li,Ming-De Li,Mingtai Wang
A facile solution-processing method featuring the applications of a stable molecular precursor solution and the repetition of spin-coating and annealing for film growth is reported for the in situ growth of CuInS2 nanoparticle films on TiO2/CdS film to provide TiO2/CdS/CuInS2 ternary superstrate heterojunction films for efficient solar cells. The novel and stable planar solar cells are fabricated using Spiro-OMeTAD as hole transporting material (HTM) and achieved a peak power conversion efficiency of 6.31% under AM 1.5 illumination at the optimized CuInS2 thickness of 200 nm and annealing temperature of 270 °C for CuInS2 formation. The efficiency is the highest among the CuInS2-based planar solar cells derived from molecular precursor methods; in particular, adopting HTM results in the open-circuit voltage up to 0.78 V, much higher than that of the similar devices without HTM. Our results demonstrate a dual nature of excitonic and nonexcitonic charge generation mechanisms in such solar cells. A depletion-field-assisted homojunction-interfacial charge transfer model is proposed to explain the generation and transfer of free charge carriers in the CuInS2 nanoparticle films, and the total charge generation in the TiO2/CdS/CuInS2 solar cells gets well elucidated from the model in combination with excitonic feature. Moreover, the CdS layer is found to act as an effective interfacial spacer to prevent the charge carriers generated upon CuInS2 absorption from recombination.
研究领域:
材料科学
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能源技术
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光电子学
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产品关联
DOI
JOURNAL OF HAZARDOUS MATERIALS
·
2020
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IF 9.038
Yingshi Zhu,Fengxia Deng,Shan Qiu,Fang Ma,Yanshi Zheng,Ruqian Lian
Facing low reactivity/selectivity of oxygen reduction reaction (ORR) in electro-Fenton (EF), N, S atoms were introduced into carbon-based cathode. “End-on” O 2 adsorption was achieved by adjusting electronic nature via N doping, while *OOH binding capability was tuned by spin density variation via S doping. Results showed the optimized N, S co-doped cathode presented a 42.47% improvement of H 2 O 2 accumulation (7.95 ± 0.02 mg L −1 cm −2 ). According to density functional theory (DFT), N, S co-doped structure favored the “end-on” O 2 adsorption as adsorption energy dropped to − 2.24 eV. Moreover, O-O/C-O bond lengths variation proved a possibility for *OOH desorption. The elaborated cathode was used in EF for sulfonamides (SAs) decay. A 100% removal rate of sulfadiazine (SDZ), sulfathiazole (STZ) and sulfadimethoxine (SDM) was achieved within 60 min, among which SDZ tended to be degraded easily. Because the absolute hardness ( η ) of those pollutants is ranked as follows: η SDM > η STZ > η SDZ . Degradation pathways were proposed based on the detected byproducts, along with toxicity was evaluated by ecological structure-activity relationship (ECOSAR) program. Results showed that toxic intermediates generated were reduced or even disappeared. EF with N, S co-doped cathode provides a promising process for antibiotics wastewater treatment .
研究领域:
环境科学
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化学工程
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污染控制
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2018
·Vol. 18
·期 4
·2379-2386
·
IF 1.354
Gong Xiaojin,Zhao Qian,Song Mu,Xue Feng
In our study, we report on the design and characterization of a combined angiogenesis therapy for breast cancer based on well-formed amine-functionalized silica nanoparticles (SLNs). The aminefunctionalized SLNs was employed to simultaneously deliver angiostatin (ANG) plasmid and candesartan
(CD) to the same cancer cell. The well-formed ANG/CD/SLNs exhibited small particle size, reasonable positive charges, excellent loading of drug and gene in vitro. Moreover, aminefunctionalized SLNs were almost no cytotoxicity. ANG/CD/SLNs resulted in enhanced gene transfection compared
to naked plasmid. More importantly, ANG/CD/SLNs as a co-delivery system achieved a stronger inhibitory effect on angiogenesis in vitro, possibly resulting from significant downregulation of vascular endothelial growth factor (VEGF) expression via different pathways. In particular, in
vivo investigation on nude mice bearing MCF-7 xenografts confirmed that ANG/CD/SLNs codelivery system exerted strong anti-tumor efficacy by synergistic antiangiogenic mechanism.
研究领域:
纳米技术
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癌症治疗
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分子生物学
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药剂学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）