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TALANTA · 2024 · IF 5.6

Oxygen-functionalized Fe3O4@o-polypyrrole acting as high-efficiency oxidase mimics and their application in glutathione colorimetric sensing

Jianwen Fei,Wei Yang,Yin Dai,Wei Xu,Huizhu Fan,Yani Zheng,Junli Hong,Jun Zhang,Wanying Zhu,Xuemin Zhou

The enzyme-like properties of nanozymes may be considerably affected by the structure and surface groups, which thus need to be optimized. Here, through a simple NaOH chemical corrosion method, the chemical structure similar to N-Methylpyrrolidone (NMP), which possessed intrinsic oxidase-like activity, was introduced into polypyrrole (PPy), and then this nanomaterial became oxygen-functionalized PPy ( o -PPy) with excellent oxidase-like activity from PPy without this property. Furthermore, after compounding magnetic Fe 3 O 4 , the obtained nanocomposites Fe 3 O 4 @o-PPy nanoparticles (Fe 3 O 4 @o-PPy NPs) showed superiorities in separation during synthesis and real-time control of enzyme catalysis . Studies have found that the enzymatic activity of Fe 3 O 4 @o-PPy NPs depended on the amount of functionalized oxygen and the conjugation extent of o -PPy. Fe 3 O 4 @o-PPy NPs had efficient oxidase-like activity under a wide range of pH and temperature. Based on the oxidase-like activity of Fe 3 O 4 @o-PPy NPs, a colorimetric sensor for glutathione (GSH), which presented rich color changes and satisfactory colorimetric resolution by adding the amaranth , was realized. We believe that the functional modification and structural regulation of PPy can not only realize its wider application but also promote the discovery of novel and efficient nanozymes .

研究领域: 材料科学 · 纳米技术 · 分析化学 · 生物化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2020 · IF 7.864

Phase Splitting Agent Regulated Biphasic Solvent for Efficient CO2 Capture with a Low Heat Duty

Chenkai Jiang,Han Chen,Junliang Wang,Yao Shen,Jiexu Ye,Shihan Zhang,Lidong Wang,Jianmeng Chen

A biphasic solvent features high absorption capacity and low heat duty for CO2 capture. Phase separation behavior is essential to cut down energy penalty. Four phase splitting agents with different hydrophobicities, such as 1,3-dimethyl-2-imidazolidinone (DMI), 1-methyl-2-pyrrolidinone (NMP), N,N-dimethylformamide, and sulfolane, were dosed to biphasic solvents, triethylenetetramine and 2-(diethylamino)ethanol. Experimental results revealed that they can tune the phase separation behavior during CO2 absorption. Generally, under the same CO2 loading, the volume ratio of the rich phase increased with their hydrophobicity (log P), which accounts for over 50%. Moreover, their influences on absorption capacity, kinetics, and thermodynamics were also investigated. After dosing NMP, the heat duty was decreased by 22%. Furthermore, a phase splitting agent with a positive log P was more conducive to reducing the heat duty, and one with a negative log P enhanced the absorption rate. With DMI, the absorption rate was 114% higher than that of MEA at rich loading. The 13C NMR analysis showed that the agents were not involved in CO2 absorption and did not affect the reaction mechanism. Furthermore, quantum calculation was used to verify the reaction mechanism, confirming that the phase splitting agent increases the reaction equilibrium constant and makes it proceed more thoroughly.

研究领域: 化学工程 · 环境科学 · 材料科学
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BIOMACROMOLECULES · 2021 · IF 6.988

Understanding Acid-Promoted Polymerization of the N-Substituted Glycine N-Thiocarboxyanhydride in Polar Solvents

Botuo Zheng,Songyi Xu,Xufeng Ni,Jun Ling

Polymerization of N-substituted glycine N-thiocarboxyanhydrides (NNTAs) is a promising pathway to prepare functional polypeptoids benefiting from their tolerance to nucleophilic impurities. However, controlled NNTA polymerization is hard to achieve in amide polar solvents, including N,N-dimethylacetamide (DMAc), N,N-dimethylformamide (DMF), and N-methyl pyrrolidone (NMP), the only aprotic solvents for many biomacromolecules and polypeptoids. In the present work, we successfully achieve controlled NNTA polymerization in amide polar solvents by adding acetic acid as a promoter. The promotion is applied to the polymerization of sarcosine NTA, N-ethyl glycine NTA, and N-butyl glycine NTA. DMAc, DMF, and NMP are suitable solvents to prepare polypeptoids with designable molecular weights and low dispersities (1.06–1.21). The polysarcosines with high molecular weights are prepared up to 35.2 kg/mol. A kinetic investigation quantitatively reveals that the presence of acetic acid not only accelerates the polymerization, but also suppresses H2S-catalyzed decomposition of NNTAs by decreasing the concentration of H2S dissolved in polar solvents. Benzoic acid is also able to promote the polymerization, while trifluoroacetic acid, phosphoric acid, and phenol are not appropriate promoters. The moderate acidity of acids is essential. l-Methionine, l-tryptophan, and l-phenylalanine, which are dissolved in DMF, initiate the controlled polymerization of sarcosine-NTA in the presence of acetic acid and introduce functional end groups to polysarcosines quantitatively. In DMAc, hydrophilic vancomycin is grafted by poly(N-butyl glycine). The amphiphilic product dissolves in dichloromethane and stabilizes water-in-oil emulsion.

研究领域: 高分子化学 · 材料科学 · 生物技术
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