CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Yang,Shiying Fan,Xinyong Li,Yiyuan Tao,Jingang Wang,Guohua Chen
Electrochemical selective dechlorination of dichloromethane (DCM) to chloromethane is a promising and sustainable strategy of resources. However, the current lack of high-performance electrocatalysts and complicated dechlorination mechanisms pose significant challenges. In this study, we report a series of Cu single-atom catalysts (SACs) supported on Co 3 O 4-β spinel with a tube-in-tube nanofiber structure, denoted as Cu x SACs/Co 3 O 4-β , where x represents the theoretical Cu loading (0.26 wt%, 0.30 wt% and 0.50 wt%). These catalysts effectively dechlorinate DCM, producing high-value hydrocarbons like chloromethane and methane. Notably, Cu 0.30 SACs/Co 3 O 4-β exhibited a high chloromethane production rate (2931 μmol g −1 h −1 ) and selectivity (76%) at −2.98 V vs (Ag/AgCl/Me 4 NCl) due to the synergy of cobaltosic oxide (Co 3 O 4 ) spinel and Cu single atom. X-ray photoelectron spectroscopy and electron paramagnetic resonance experiments confirmed the presence of additional surface oxygen vacancies in Cu 0.30 SACs/Co 3 O 4-β , which improved the electrocatalysis performance for DCM dechlorination. Furthermore, a concerted dechlorination mechanism was suggested based on the transfer coefficient α . This research paves the way for the development of novel spinel electrocatalysts and the advancement of dechlorination reactions.
研究领域:
材料科学
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环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Dongmiao Li,Jinni Shen,Jiangjie Zhang,Yao Chai,Yanyu Xie,Chengwei Qiu,Mengmeng Ni,Yuanhui Zheng,Xuxu Wang,Zizhong Zhang
The development of direct conversion for selective functionalization of inert methane plays an important role in the chemical sciences. Here, we report a photocatalytic approach to successfully convert methane into methyl chloride over NaTaO3 photocatalyst using an alkali chloride solution as the chlorine source under ambient conditions, which can overcome disadvantages of toxicity and corrosiveness in the traditional chlorination of methane. Various noble metals and oxide cocatalysts (Pt, Pd, Au, Ag, and Ag2O) and different chloride ion solutions (NaCl, KCl, LiCl, MgCl2, BaCl2, CaCl2, CuCl2, FeCl3, ZnCl2, etc.) are investigated to optimize the photocatalytic chlorination processes. Ag2O/NaTaO3 is the best photocatalyst, giving the maximum CH3Cl yield of 152 μmol g–1 h–1 in aqueous NaCl solutions and an apparent quantum yield of 7.2% under 254 nm monochromatic light irradiation. The target product CH3Cl is verified to be formed by a direct combination of the photoinduced species •CH3 and •Cl on the Ag2O surface. This work provides a meaningful approach for the conversion of methane into chloromethane under normal conditions.
研究领域:
化学科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Heliyon
·
2023
·
IF 4
Jingqi Zhang,Ying Song,Jingbo Chao,Hai Huang,Dazhi Liu,Frederic Coulon,Xiao Jin Yang
Zero-valent iron (ZVI) has been extensively studied for its efficacy in removing heavy metals, nitrate, and chlorinated organic compounds from contaminated water. However, its limited effectiveness due to rapid passivation and poor selectivity is prompting for alternative solutions, such as the use of aluminium alloys. In this study, the efficacy of five distinct aluminium alloys, namely Al–Mg, Al–Fe, Al–Cu, and Al–Ni, each comprising 50 % Al by mass at a concentration of 10 g/L, was assessed using copper, nitrate and trichloromethane (TCM) as model contaminants. Results show that chemical pollutants reacted immediately with Al–Mg. On the contrary, the remaining three alloys exhibited a delay of 24 h before demonstrating significant reactivity. Remarkably, Al–Mg alloy reduced nitrate exclusively to ammonium, indicating minimal preference for nitrate reduction to N 2 . In contrast, the Al–Cu, Al–Ni, and Al–Fe alloys exhibited N 2 selectivity of 3 %, 5 %, and 19 %, respectively. The removal efficiency of copper, nitrate and TCM reached 99 % within 24 h, 95 % within 48h and 48 % within 48h, respectively. Noteworthy findings included the correlation between Fe concentration within the Al–Fe alloy and an increased N 2 selectivity from 9.3 % to 24.1 %. This resulted in an increase of Fe concentration from 10 % to 58 % albeit with a concurrent reduction in reactivity. Cu 2+ removal by Al–Fe alloy occurred via direct electron transfer, while the removal of nitrate and TCM was facilitated by atomic hydrogen generated by the alloy's hydrolysis. Intriguingly, nitrate and TCM suppressed Cu 2+ reduction, whereas Cu 2+ improved nitrate reduction and TCM degradation. These findings demonstrate the great potential of Al–Mg and Al–Fe alloys as highly efficient agents for water remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Materials Research Express
·
2025
·Vol. 12
·期 1
·015304
·
IF 2.2
Shibo Ren,Jianlin Xu,Lei Niu,Penghui Yang
In this study, the surface flame retardancy of polycarbonate (PC) was improved and the impact of flame retardants on the substrate were minimized by pre-mixing Al2O3 particles with dichloromethane, an infiltration promoter, to form a suspension, and then treating PC with the suspension to form an Al2O3 infiltration layer. For this layer, its structure and composition were characterized, its flame retardancy was evaluated, and its flame retardancy mechanism was investigated. The characterization results confirmed that an Al2O3 infiltration layer was successfully prepared on the PC surface under the aid of dichloromethane and that the involvement of dichloromethane induced certain microscopic pores and voids in the PC, with some dichloromethane remaining within the surface infiltration layer. The surface Al2O3 infiltration layer mainly served as a condensed-phase flame retardant. The infiltration layer prepared using a suspension with a dichloromethane-to-Al2O3 mass ratio of 24:1 not only exhibited a good overall performance but also achieved the best improvement in the PC flame retardancy, such as an increase in the vertical burning rating from HB to V-0, as well as the LOI increased from 24 to 31.3, and a 35% reduction in the peak heat release rate compared to those of pure PC.
研究领域:
材料科学
·
燃烧学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2019
·
IF 4.191
Cai Liang,Li Yang,Yu Shao,Xinyue Zhu,Hongliang Zhao,Biwei Chen,Wen Song,Xiangmin Song,Xiaofan Ding,Ranfeng Sun
The secondary metabolites produced by plants are important sources of fungicides with intriguing bioactivities and environmentally benign attributes (eg. low residual toxicity to mammals and readily biodegradable in soil). In this study, the dichloromethane extract of stems of Waltheria indica L. was found to exhibit broad-spectrum antifungal activity toward eight phytopathogenic fungi, particularly against carbendazim-resistant Sclerotinia sclerotiorum with inhibition rate of 100% at 500 μg/mL. Two quinoline alkaloids, antidesmone and waltherione C, were isolated and identified as fungicidal compounds by bioassay-guided isolation and spectroscopic analyses. Antidesmone displayed superior antifungal activities against eight phytopathogenic fungi to commercial botanical fungicides (osthole, carvacrol, and eugenol). Moreover, antidesmone was found to have significant negative cross-resistance with carbendazim to Sclerotinia sclerotiorum for the first time and exhibited much better antifungal activity (EC 50 = 0.60 μg/mL) against carbendazim-resistant strains than carbendazim-sensitive strain (EC 50 = 9.61 μg/mL) of Sclerotinia sclerotiorum , which was further supported by the molecular modelling result. In addition, the dichloromethane extract of the Waltheria indica stems could effectively control the development of eleven species of phytopathogenic fungi in vivo. These results suggest that Waltheria indica dichloromethane extract and antidesmone can be developed as promising broad-spectrum botanical fungicides.
研究领域:
植物学
·
真菌学
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农药科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 49
·25933-25939
·
IF 3.708
Qingfeng Liu,Yansen Zhang,Zhiguo Zhang,Tongxin Liu,Lei Shi,Guisheng Zhang
This paper describes a highly efficient and facile transformation of substituted oxazolidin-2-ones to methylene-bridged 3,3′-bis(oxazolidin-2-one) derivatives in a mixture solvent of CH2Cl2 (DCM) and N,N-dimethylformamide (DMF) in the presence of NaH at ambient temperature. Isotopic labeling experiments indicated that the C of the bridged methylene group was derived from CH2Cl2 instead of DMF and other unknown substances in the NaH reagent (60% dispersion in mineral oil).
研究领域:
有机化学
·
药物化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 42
·15724-15734
·
IF 8.307
Shaohua Chai,Shuangde Li,Le Zhang,Guijun Fan,Linfeng Nie,Xin Zhou,Wuxinchen Yang,Weiman Li,Yunfa Chen
The regulation of oxygen vacancies and Ru species using metal–organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO2 and Ru/N-TiO2 catalysts were synthesized by the pyrolysis of MIL-125 and NH2-MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at ∼290 °C over Ru/M-TiO2 and Ru/N-TiO2 catalysts, while Ru/N-TiO2 showed quite less monochloromethane (MCM) and higher CO2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO2, compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO2. Additionally, Ru/N-TiO2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Shengyu Wu,Zhongran Wu,Guofeng Li,Yongkai Liao,Shanna Lin,Zhao Liu,Chao Cai
The transport behavior of pollutants under dynamic groundwater conditions has attracted significant attention recently. However, there is limited research on the simultaneous effects of groundwater table fluctuations on the transport of co-existing pollutants, especially combined dense and light non-aqueous phase liquids (DNAPLs and LNAPLs). In this study, column experiments investigated toluene and dichloromethane transport in a controlled water table system with varying fluctuation conditions. Results showed that both dichloromethane and toluene accumulated near the groundwater table under static water table conditions, but the concentration of dichloromethane declined more rapidly than toluene due to differences in their physicochemical properties, such as solubility, density, and hydrophobicity. Groundwater fluctuations facilitated pollutants transportation towards deeper layers, potentially resulting in unforeseen increases in pollutant volatilization and downward fluxes. The interactions between dichloromethane and toluene, including competitive adsorption, enhanced dissolution, and altered kinematic viscosities, resulted in the reduced transport potential of dichloromethane while enhancing that of toluene. Furthermore, compared to dichloromethane, the initial upward fluctuation of the water table had a more pronounced impact on toluene due to its lower solubility and volatility. The downward transport risk index assessment indicated that among various factors considered, groundwater fluctuation amplitude exerted the most significant influence on pollutant migration risk. These new findings will provide important insights into understanding and assessment of the potential transport risk associated with combined LNAPLs and DNAPLs in the natural environment.
研究领域:
环境科学
·
水文学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Yutong Zhang,Yinge Bai,Mengjun Wang,Shaojuan Zeng,Wei Han,Xiangping Zhang
Ionic liquids (ILs) show great potential for the treatment of dichloromethane (DCM)-containing waste gases, but currently there are limited data on the vapor–liquid equilibrium (VLE) of DCM + IL systems. This work uses headspace gas chromatography (HS-GC) to determine the isothermal VLE data of the DCM + [Epy][EtSO4] and DCM + [Emim][EtSO4] systems at 308.15 K, 313.15 K, 318.15 K, 323.15 K, and 328.15 K. The nonrandom two-liquid (NRTL) and universal quasi-chemical correlation activity coefficient (UNIQUAC) models are used to regress the VLE data. The results show that the fitting average relative deviations (ARDs) of the DCM + [Epy][EtSO4] and DCM + [Emim][EtSO4] systems to the NRTL model were 6.97% and 7.95% and the fitting ARDs to the UNIQUAC model were 6.10% and 6.28%, respectively. The fitting effects of the UNIQUAC models for both systems were better than those of the NRTL model. With the models, the calculated activity coefficients of DCM were all less than 1, indicating that the solutions exhibited negative deviations from Raoult’s law, and the nonideality of the solutions increased with increasing IL concentration.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2025
·
IF 0
Liu Pengxiao,Gao Shuai,Li Ying,Hou Bin,Liu Ning,Du Zhen,Lu Jing
This study investigated the aging and pollution behavior of acrylonitrile butadiene styrene (ABS) and polycarbonate (PC) microplastics (MPs) exposed to residual chlorine in tap water distribution systems. The ABS and PC MPs in the aging processes were analyzed using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Results revealed that 0.4 mg/L residual chlorine could induce morphological changes, increase surface oxygen-containing functional groups, and enhance the hydrophilicity of MPs at the CT value of 9216 mg·min/L. Additionally, both ABS and PC MPs released dissolved organic matter (DOM) into water, with higher DOM concentrations observed in the presence of residual chlorine. Besides, this interaction also led to the formation of trichloromethane (TCM). And the TCM production increased with higher MPs concentrations, smaller particle size, and longer chlorine exposure time.
研究领域:
环境科学
·
污染生态学
✓ 已验证
产品关联
DOI
PubMed
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Qiangbing Shi,Kaixuan Wang,Mengjun Wang,Tao Li,Baozeng Ren,Yinge Bai,Xiangping Zhang
Four sulfate-based ILs, 1-butyl-3-ethylimidazolium ethyl sulfate [Beim][EtSO4], 1-ethyl-3-ethylimidazolium ethyl sulfate [Eeim][EtSO4], 1-ethyl-3-methylimidazolium ethyl sulfate [Emim][EtSO4], and 1-ethylpyridinium ethyl sulfate [Epy][EtSO4], were synthesized and used as an absorbent for dichloromethane (DCM). Among them, the maximum DCM absorption capacity of 0.426 g DCM g–1 IL was achieved in [Beim][EtSO4] at 313.15 K and 37.7% DCM concentration, which was 42.2% higher than that of common organic solvent bis(2-ethylhexyl) adipate under the same conditions. The density and viscosity of [Beim][EtSO4] containing different mass fractions of DCM were measured. The density of [Beim][EtSO4] increases with the mass fraction of adsorbed DCM, while the viscosity decreases sharply. The efficient performance of ILs to absorb DCM is mainly due to the hydrogen bonding interaction between the anion and DCM, which was confirmed by spectroscopic measurement and quantum chemical calculations. This work demonstrates the great potential of ILs in separating and recovering DCM from exhaust gas.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Shengyu Wu,Zhongran Wu,Suhang Wang,Youchi Zhang,Yongkai Liao,Chao Cai
The transport behavior of combined organic pollutants in soil and groundwater has attracted significant attention in recent years. Research on the influence of humic acid (HA) on organic pollutant transport behavior mainly focuses on the study of the mobile phase HA, with less research on the adsorbed phase HA, especially regarding its interaction with combined pollutants. To enhance understanding of the regulation of co-transport and retention of combined pollutants by adsorbed phase HA, in this study, tests were conducted to investigate how toluene (TOL) and dichloromethane (DCM) are transported in the presence of adsorbed phase HA at different pH levels and ionic strengths. As the proportions of HA-coated sand increased, so did its adsorption capacity for TOL and DCM, which can be attributed to adsorbed phase HA providing more adsorption sites compared to plain sand, thereby reducing the transport potential of the pollutants. The presence of both TOL and DCM facilitated their mutual transportation due to competitive adsorption controlled by the adsorbed phase HA content in the porous medium. Furthermore, it was observed that pH levels influenced the transport behavior of TOL and DCM when adsorbed phase HA was present since adsorbed phase HA transformation into mobile phase was regulated by pH levels. The transport patterns can be effectively simulated using the chemical nonequilibrium two-site sorption model in HYDRUS-1D, accurately reflecting the retardation coefficients and transport distances based on model parameters. This work sheds new light on the regulatory role of adsorbed phase HA in TOL and DCM transport under diverse hydrochemical conditions, with implications for accurately depicting the behavior of combined pollutants, optimizing the remediation strategies and improving remediation efficiency in contaminated sites.
研究领域:
环境科学
·
土壤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）