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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Highly Reversible and Efficient Absorption of Low-Concentration NO by Amino-Acid-Based Ionic Liquids

Ying Sun,Shuhang Ren,Yucui Hou,Kai Zhang,Qi Zhang,Weize Wu

A series of environmentally benign functional ionic liquids (ILs) based on l-proline as the anion to efficiently absorb low-concentration NO have been investigated in this work. The results indicate that the ILs with an l-proline anion have high absorption capacities for 0.16 vol % NO, reaching a maximum absorption capacity of 0.51 mol of NO per mol of IL at 30 °C and ambient pressure for l-proline choline IL ([Ch][l-Pro]). The absorbed NO could be recovered from [Ch][l-Pro], and the regenerated IL had no significant loss of NO absorption capacity for at least 7 recycles. We verified the mechanism through both experimental and theoretical methods. The results indicate that the absorption of NO in [Ch][l-Pro] mainly resulted from a chemical process—NO and the secondary amine group in the anion form a NONOate with a chemical formula [l-Pro]−–(NO)–NO. We believe that this efficient and reversible absorption of low-concentration NO by the ILs has potential as a new NO capture technique.

研究领域: 环境科学 · 化学工程
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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Experimental solubility and thermodynamic modeling of nitric oxide absorption in low-viscosity DBU-based deep eutectic solvents

Wentao Zheng,Guangwen Yu,Guibing Xia,Wanghao Shen,Weizhong Shi,Tengteng Zhou,Xiankun Wu

Developing absorbents with highly efficient nitric oxide (NO) absorption and desorption is very important for flue gas denitrification process. Toward this end, a class of DBU-based deep eutectic solvents (DESs) containing alkanones or azoles as functional HBDs for the capture of NO were synthesized in this work, with viscosities of only 7.71–45.57 mPa·s at 303.2 K. Solubilities of NO in these DESs were determined at temperatures from 303.2 to 333.2 K and pressures from zero to 1 bar. It was found that the absorbing abilities of the DESs increased with the increasing HBDs’ alkalinity. Impressively, these DBU-based DESs had remarkable larger absorption capacities than those reported DESs in the literature. According to the solubility curves of NO, chemical absorption was thought to occur accompanying with the physical one in the systems. Therefore, the reaction equilibrium thermodynamic model (RETM) was applied to model the experimental NO solubilities. The corresponding thermodynamic parameters for each system, such as the reaction equilibrium constant, Henry’s law constant, and the enthalpy change were also obtained to assess the NO absorption process in these DESs.

研究领域: 环境科学 · 化学工程
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TOXICON · 2019 · IF 2.276

Role of divalent metals Cu2+ and Zn2+ in Microcystis aeruginosa proliferation and production of toxic microcystins

Dong Ao,Zhen Lei,Mawuli Dzakpasu,Rong Chen

Cu 2+ and Zn 2+ , two ubiquitous metals in water environments, can widely trigger algae blooms at favourable environmental conditions. This paper elucidates the roles of Cu 2+ and Zn 2+ in the proliferation of Microcystis aeruginosa ( M. aeruginosa ) and synthesis of Microcystins (MCs). Findings indicate significant influences of increasing Cu 2+ and Zn 2+ concentrations on cell proliferation at limited available phosphorus concentrations of less than 0.1 mg/L. By contrast, Cu 2+ and Zn 2+ notably affected MCs production at all the inoculated phosphorus concentrations. The critical concentrations of 1 μg/L and 5 μg/L for Cu 2+ and Zn 2+ , respectively, are determined to trigger rapid cell proliferation and MCs production. Furthermore, the impacts of Cu 2+ and Zn 2+ on nitrogen absorption and, subsequently, on amino acids (AAs) formation in cells, is likely key in MCs synthesis. The two AAs Alanine (Ala) and glutamic acid (Glu) demonstrate the most notable variations with the concentrations of Cu 2+ & Zn 2+ .

研究领域: 环境科学 · 微生物学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2022 · IF 11.357

Mechanism and Kinetic Study of Cyclodextrin Use to Facilitate NO2 Absorption in Sulfite Solutions

Zheng Lian,Guojun Li,Shule Zhang,Weihua Ma,Qin Zhong

An innovative strategy to control nitrogen oxide emission from flue gas was developed using the wet flue gas denitrification technology. The use of cyclodextrin (CD) as an additive facilitated NO2 absorption by the sulfite absorbent. Compared with absorption by a sulfite solution (59.12%), the instantaneous absorption efficiencies employing CD improved to 94.57%. Moreover, 48 h of continuous absorption indicated cyclic utilization of CD. The favorable role of CD was ascribed to facilitating the limiting step for the entire NO2 absorption–dissolution process which included both water solubility and gas–liquid mass transfer. Furthermore, we propose a potential mechanism of CD/sulfite mixed solution absorbing NO2, among which the favorable role of the additive is related to its amphiphilic behavior toward gas and liquid phases. Additionally, a kinetic model describing the rates of gas–liquid transfer and macro absorption was established based on various operating conditions. This model explains the absorption improvement in the kinetic aspect and provides theoretical guidance for practical applications.

研究领域: 环境科学 · 化学工程
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Highly Efficient Absorption of NO by Dual Functional Ionic Liquids with Low Viscosity

Ying Sun,Shuhang Ren,Yucui Hou,Kai Zhang,Weize Wu

In this work, we demonstrate an innovative strategy for efficient and sustainable absorption of NO in a series of ionic liquids (ILs) containing amine groups and azole groups. The results show that the ILs have low viscosities and high performance for NO absorption. For instance, [TEPA][Im] had a high absorption capacity of 6.79 mol NO per mol IL at 30 °C and ambient pressure. The absorbed NO was easily released by heat treatment, and the regenerated IL had significant reversibility. The results of 1H NMR, UV spectra, and FT-IR spectra of ILs before and after NO absorption indicated that the absorption of NO in the [TEPA][Im] mainly resulted from a chemical interaction. NO interacts with not only the secondary amine groups in the cation but also N-imidazole in the anion through the formation of NONOate, indicating [TEPA][Im] is a dual functional IL. By introducing this efficient and reversible absorption of NO by ILs, our work broadens the method of NO capture.

研究领域: 化学工程 · 环境科学
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Highly Efficient and Reversible Absorption and Oxidation of Low-Concentration Nitric Oxide by Functionalized Ionic Liquids

Shenyao Wang,Xiaoyu Lv,Zhenyu Zhao,Yixin Chen,Zhong Chen,Wenjun Lin,Haoran Li,Congmin Wang

A novel method of using anion-functionalized ionic liquids (ILs) with high NO absorption capacity and reversibility for the capture and in situ oxidation of low-concentration NO was established. For the mixed gas containing 0.25% NO, the accumulation rate of nitric acid in these ILs was significantly higher than that in the conventional ILs; after absorption and oxidation reached equilibrium, the molar ratio of HNO3 to [P4446][PhSO3] was 0.86, which was 5 times as high as that of the conventional IL. Therefore, the problems of low efficiency and poor reversibility of traditional ILs in the absorption and oxidation process were solved. Through absorption and oxidation experiments, quantum chemical calculation, NMR, and time-resolved in situ ATR-FTIR spectroscopic investigation, the results demonstrated that such a high accumulation rate of HNO3 originated from high uptake of NO through multiple-site interaction. Moreover, high reversibility is attributed to low volatility of conjugated acid of anions and decreased basicity of O sites on anions. We believe that such highly efficient and reversible conversion of low-concentration NO to HNO3 by ILs provides a new strategy for improving atomic economy of fossil fuel combustion, that is, converting post-combustion pollutants to good valuable chemicals.

研究领域: 环境科学 · 化学工程 · 材料科学
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ENERGY & FUELS · 2019 · IF 3.021

Highly Efficient Absorption of NO by Amine-Based Functional Deep Eutectic Solvents

Ying Sun,Minjie Gao,Shuhang Ren,Qi Zhang,Yucui Hou,Weize Wu

To explore new reversible and environmentally friendly solvents for the capture of nitric oxide (NO), a series of amine-based functional deep eutectic solvents (DESs) were designed via ammonium salts (triethylenetetramine chloride-[TETA]Cl and tetraethylenepentamine chloride-[TEPA]Cl) and polyhydric alcohols (ethylene glycol-EG, 1,3-propanediol-PG, glycerol-Gy, and polyethylene glycol 2000-PEG). All of the DESs prepared showed good absorption capacities for 10 vol % NO. EG-[TEPA]Cl DES (nEG/n[TEPA]Cl = 3:1) had the highest absorption capacity of 10 vol % NO, 0.327 g NO per g DES at 30 °C. Moreover, the EG-[TEPA]Cl DES (nEG/n[TEPA]Cl = 3:1) showed excellent reusability for at least 5 recycles. The comparison of FT-IR and UV–vis spectra of DESs before and after NO absorption was made to study the absorption mechanism. The results indicated that the absorption of NO by the DESs was mainly a chemical process. One mole of amine group in HBA could react with two moles of NO to produce R1R2N–(NO)–NO, where both R1 and R2 belong to alkyl groups. This efficient and reusable absorption of NO in the functional DESs was expected to provide a new idea for the capture of NO.

CAS / MDL: 107-21-1 504-63-2
研究领域: 环境科学 · 化学工程
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

Efficient absorption and thermodynamic modeling of nitric oxide by low viscous DBU-based N-heterocyclic deep eutectic solvents

Wentao Zheng,Guibing Xia,Guangwen Yu,Qian Cai,Xiankun Wu,Weizhong Shi

A series of low viscous deep eutectic solvents composed of 1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU) and N-heterocyclic compounds were designed and synthesized as NO trapping agents. These DESs exhibited low viscosity of 10.02 mPa·s and excellent NO absorption capacity up to ∼ 5.10 mol·kg −1 at 293.2 K and atmospheric pressure. The N-heterocyclic compounds were found to play a dominant role in the absorption, and the absorption behavior could thus be adjusted by the molar ratio of DBU to N-heterocyclic compounds. With the assumption of complex formation between NO and DESs, the reaction equilibrium thermodynamic model (RETM) was developed to correlate the experimental solubilities of NO. The thermodynamic parameters, such as the equilibrium constant K , the Henry’s constant H and the enthalpy change Δ H , were thus calculated to evaluate the absorption process. In addition, through a combination of the experimental absorption capacities, the RETM modeling results and the spectroscopic investigations, it was proposed that the absorption of NO in the DBU-based N-heterocyclic DESs was governed by the chemical interaction between NO and the N atom on the N-heterocyclic compounds with the reaction stoichiometry of 1:1.

研究领域: 化学工程 · 环境科学
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JOURNAL OF ENVIRONMENTAL MANAGEMENT · 2025 · IF 8.4

From glycine peptides uptake to toxin surge: Decoding adaptation mechanisms under organic nitrogen enrichment in Microcystis aeruginosa

Yaxin Guo,Zongcheng Yao,Xiating Zhao,Yuting Wang,Qiming Xian

The structural specificity of organic nitrogen sources in modulating cyanobacterial physiology and toxin production remains poorly understood. This study systematically evaluated the bioavailability of exogenous glycine peptides in Microcystis aeruginosa ( M. aeruginosa ) and their regulatory roles in algal growth and microcystins (MCs) synthesis through an integrated physiological and transcriptomic approach. Glycine peptides demonstrated hierarchical bioavailability: glycine (Gly) > Glycylglycine (Gly2) > Tetraglycylglycine (Gly4) > Hexaglycylglycine (Gly6) > Cycloglycylglycine (CGly2). Gly and Gly2 were rapidly assimilated by M. aeruginosa , supporting robust algal growth comparable to the control group with nitrate as nitrogen source, while CGly2 and Gly6 induced nitrogen stress, damaging biomass and photosynthetic pigments. Notably, M. aeruginosa cultured with Gly4 as sole nitrogen source uniquely enhanced intracellular MCs production, and shifted MCs variants toward the highly toxic MC-LR. The shift in MCs variants ratios (MC-RR/MC-LR) reflected nitrogen availability, demonstrating a trade-off between nitrogen storage and toxin potency. Transcriptomic profiling unveiled nitrogen-centric metabolic rewiring, resulting in enhanced nitrogen assimilation, mcy genes for MCs biosynthesis, photosynthetic efficiency, and resource reallocation. While exogenous glycine peptides represent only a minor component of organic nitrogen in natural systems, these findings provide mechanistic insights into how peptide structure can influence cyanobacterial physiology and toxin profiles, contributing to a more nuanced understanding of organic nitrogen utilization by harmful cyanobacteria.

CAS / MDL: 56-40-6
研究领域: 环境微生物学 · 水生生态学 · 毒理学 · 分子生物学 · 藻类学
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ACS Earth and Space Chemistry · 2021 · IF 3.475

Atmospheric Nitrate Formation through Oxidation by Carbonate Radical

Xiaozhong Fang,Yangyang Liu,Kejian Li,Tao Wang,Yue Deng,Yiqing Feng,Yang Yang,Hanyun Cheng,Jianmin Chen,Liwu Zhang

The carbonate radical (CO3•–) has been proved to be of great significance in the water environment. However, a few studies concerned with its contribution to atmospheric heterogeneous chemistry. Here, we report the pathway for the first time for CO3•– generation by interfacial photogenerated hole/hydroxyl radical (•OH) transfer between the photoactive component and (bi)carbonate (CO32–/HCO3–) of mineral dust under atmospherically relevant actinic irradiation. By combining laboratory simulation, nanosecond transient absorption spectroscopy (NTAS), and field observation, we demonstrate that (bi)carbonate in the atmosphere not only has a pH buffering effect in the uptake of NO2 but more importantly directly participates in the photochemical reactions by generating CO3•– under irradiation. CO3•– can play an important role by facilitating nitrite transformation to nitrate, especially under a lower light intensity (15 mW/cm2) and a higher humidity (60% RH). Diffuse reflectance infrared Fourier transform spectrometry (DRIFTS) was used to detect the surface species generated on simulated mineral dust. Under irradiation, the time-dependent reactive uptake coefficient for the first-order reaction of NO2 uptake on simulated mineral dust was found to be 2.817 × 10–8 × e–t/6559. These results highlight the important role of CO3•– in atmospheric photochemistry, which could act as a reactive radical and influence secondary aerosol formation.

研究领域: 大气化学 · 环境科学 · 光化学
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