AICHE JOURNAL
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2024
·
IF 3.5
Tong Luo,Qi Liu,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Aqueous amine solution is a promising absorbent for CO 2 capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO 2 for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high-performance CO 2 absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti-degradation CO 2 absorbent.
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CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Yufen Xiao,Jiamin Zhang,Tong Wu,Shuai Chen,Zhixiong Huang,Jianzhong Du
Natural modulators, such as insulin, play a significant role in modulating molecule levels. Inspired by the role of natural modulators, herein, we propose a glucose modulator that is composed of a glycopolymersome only to regulate glucose levels. This insulin- and drug-free strategy can smartly take in and snap out glucose according to the surrounding blood glucose levels (BGLs) by reversible sugar substituting. The glycopolymersome is self-assembled from a biodegradable glycopolymer that is composed of sugar and phenylboronic acid derivative, poly(ε-caprolactone)-block-poly[(3-acrylamidophenylboronic acid-stat-N-acryloyl glucosamine] [PCL-b-P(AAPBA-stat-AGA)]. It exhibits excellent long-term hypoglycemic effects toward type 1 diabetic mice for at least 3 days upon one shot without observed side effects, which is the longest effective sugar-regulation time for the insulin and drug-free strategy. Most notably, we explored the effect of the molecular structure of the glycopolymers on the BGL regulating efficacy, where the glucosyl moiety was polymerized with PBA either randomly or separately. Block-statistical glycopolymersomes exhibited lower binding energy to glucose, better glucose responsiveness, and prolonged hypoglycemic effect due to the abundant intramolecular and intermolecular dynamic covalent bonds between AAPBA and AGA. Our finding confirmed the importance of a block-statistical copolymer structure and the key role of sugar in regulating BGLs without involving medication, which may provide guidance and open new avenues for design blood glucose regulating materials.
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Nanomaterials
·
2024
·Vol. 14
·期 11
·980
·
IF 4.4
Lu Yi,Xiangnan Chen,Heng Su,Chaocan Zhang
In this paper, the oxidation–exfoliation process of graphite is studied experimentally by the mixed-solvent method, the oxidation–exfoliation process of graphite is simulated theoretically, and it is found that Graphene Oxide (GO) is a Janus structure with inconsistent oxidation on both surfaces; hydrophilic on one side and hydrophobic on the other side. This layer structure and layer spacing are due to the inconsistent oxidation on both sides which changes with the polarity of different solvent mixtures. We used a two-phase system of benzyl alcohol and water, as well as controlling the polarity of the surface of the substrate, to achieve (using a mixed solution of GO which has a selectivity more inclined to the oil phase when the aqueous phase is present) the preparation of reduced graphene oxide patterns. We also used a complex solution of hydrogen iodide and a sodium–iodide complex solution for secondary reduction to enhance its conductivity to 8653 S/m.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hui Wang,Hongtu Zhao,Wenbo Wu,Shifan Xu,Na Wang,Ting Wang,Xin Huang,Lina Zhou,Ying Bao,Hongxun Hao
The solubility performance of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane has been investigated by the combination of experimental measurement, solvent parameter analysis, and molecular simulation methods. The solubility in 10 pure solvents at 293.15 K to 343.15 K was determined. It was found that the solubility in nine solvents increased with temperature, except for isoamyl propionate. However, it has the largest solubility in isoamyl propionate (4.36 × 10 −2 ∼ 5.39 × 10 −2 ). Additionally, a correlation analysis was performed using four equations, which showed that the NRTL equation provided the best fit (overall average relative deviation = 3.74 %, overall coefficient of determination = 0.991). Moreover, the solvent effect was analyzed by Hansen solubility parameters, predicting good solubility in solvents with R a(V) ≤ 12.47 MPa 0.5 or Δ δ t ≤ 7.77 MPa 0.5 , indicating weak polarity of solvent and weak solvent–solvent intermolecular hydrogen bonds enhance dissolution. Furthermore, molecular electrostatic potential surface and radial distribution function analyses provided that weak hydrogen bonding C-H···O promotes dissolution.
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LANGMUIR
·
2024
·
IF 3.7
Zeqi Wu,Feng Niu,Wenhao Yao,Siyuan Gao,Da Chen,Yuexiang Huang
The activation of an inert C(sp3)–H bond in selective oxidation of hydrocarbons under mild conditions is a critical and challenging process. Herein, we report a stable chlorine-coordinated metal–organic framework (MOF) photocatalyst, MIL-101(Fe), for efficient visible-light-driven photocatalytic selective oxidation of toluene to benzaldehyde in air under ambient conditions. Encouragingly, a benzaldehyde formation yield of 3.11 mmol·g–1·h–1 with a selectivity of 92.1% is achieved in 5 h, which is superior to most of the reported works. Based on the experimental results and characterizations, the high catalytic performance is mainly due to the promoted rate-limiting step of C(sp3)–H bond activation by a chlorine radical (Cl·) from the coordinated −Cl in the MIL-101(Fe) structure. In addition, the present photocatalyst possesses good substrate tolerance for photocatalytic selective oxidation of various toluene derivatives under optimized conditions.
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2024
·
IF 4.2
Xiangyang Chen,Shun Gong,Biao Zhao,Kai Pan
Biobased thermoplastic polyamide elastomers (TPAEs) have received increasing attention in both academia and industry. Here, a series of semi-biobased long-chain TPAEs are successfully synthesized via one-step melt polymerization, employing polyamide 1210 (PA1210) and polyetheramines (PEAs) as hard and soft segments, respectively. The prepared TPAEs demonstrate excellent mechanical properties, energy dissipation capabilities, low density, good damping, high resilience, and low melting temperature. More interestingly, the properties of the TPAEs can be customized by adjusting the content and molecular weight of PEA. By varying the molecular weights of the PEAs, two different thermal behaviors can be observed in the prepared TPAEs. Specifically, PEA with low molecular weight has good compatibility with PA1210, leading to an increase in the conformation of the crystalline region and a significant decrease in melting temperature. Meanwhile, high molecular weight PEA causes strong phase separation with PA1210, leading to limited crystalline regions and inadequate physical cross-linking, further resulting in suboptimal mechanical properties. This work provides new insights into the design and preparation of PEA-type biobased long-chain TPAEs.
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Food Bioscience
·
2024
·
IF 4.8
Lian Xia,Jia Zheng,Jian Su,Hongli Yang,Zhengmin Xie,Yue Tang,Yuangen Wu
Ethyl carbamate (EC) is a small compound produced and stored during fermentation processes from ethanol, urea, citrulline, and carbamoyl phosphate. EC is commonly found in fermented foods and alcoholic beverages. Prolonged exposure to EC can cause nervous system diseases and liver damage in human beings. EC lacks stable physicochemical properties, and the presence of numerous interfering substances in alcoholic beverages poses challenges for its detection. Herein, it is found that EC1-34 aptamer bound to EC can enhance the laccase-like activity of cubic Ag 2 O nanoparticles (NPs). Subsequently, Ag 2 O NPs are wrapped with EC1-34 aptamer to prepare recognition probes, which are immobilized on a carrier membrane. Thus, a portable paper-based sheet for EC detection in Chinese Baijiu is designed. The visual detection limit of the developed paper-based sheet for EC is 10 μg⋅L −1 , and shows an outstanding linear relationship within the range of 10–200 μg⋅L −1 . Moreover, this colorimetric paper-based sheet has a good practicality in various Chinese Baijiu samples. It is believed that such paper-based sheet can facilitate portable inspection for EC in Baijiu, and may also become a beneficial tool for monitoring EC molecules in other fermented foods.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Deyin Wang,Weixiang Zhai,Wenli Jing,Shuo Zhang,Zishan Gong,Liyan Zhang,Liang Xu
Time-resolved fluorescent nanospheres (TRFNs) are polymer nanospheres with special functional groups on the surface loaded with rare earth complexes which emit fluorescence when irradiated by ultraviolet light. TRFNs offer spherical morphology, homogeneity, good dispersity, large specific surface area, easy chemical modification, high loading capacity and good biocompatibility. The rare earth complexes possess unique properties that render them highly sensitive and capable of effectively excluding unspecific fluorescence. Hence, they constitute an excellent labeling material for the time-resolved fluorescence immunochromatographic assay (TRFIA). The developed method has a linear response to ferritin from 6 to 1000 ng/mL with a detection limit of 3.5 ng/mL, good reproducibility, and good accuracy compared with commercial chemiluminescence measurements of serum. These results suggest that the reported TRFN has utility for time-resolved fluorescence immunochromatographic assays.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuanyan Luo,Tao Zhou,Costas Molochas,Yongkang Tan,Xiaoting Huang,Zhenyu Chen,Jinliang Zhu,Panagiotis Tsiakaras,Peikang Shen
Pt-Pd-Ni polyhedral nanobelt (PNBs) composite catalysts are synthesized in presence of tungsten hexacarbonyl [W(CO) 6 ] by a simple solvothermal method, combining both higher specific surface area and more index active site than the corresponding single-structure catalysts. The thermal decomposition of W(CO) 6 plays a crucial role in the morphology formation. The tenuous composite with a moderate nanobelt width of 7.46 nm formed after heating for 6 h (Pt-Pd-Ni PNBs2) shows better ORR performance and durability than the ternary (Pt-Pd-Ni) and binary (Pt-Pd) single structures. It exhibits a mass activity of 1.49 (A mg Pt −1 ), which only degrades by about 10.63 % after 50,000 durability cycles. The metal regulatory effects induced by the carbonyl compounds cause the contraction of the Pt-Pt bonds. Density functional theory calculations indicate that the compressive strain of Pt-Pd-Ni PNBs2 leads to a decrease in the d-band center and overpotential negatively shifted, thus provide a more sufficient and faster ORR proceeding process in thermodynamics, facilitating a higher energy conversion efficiency.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 142
·期 2
·e56337
·
IF 2.7
ZiXuan Wang,Hao Zheng,Zhengchun Cai,Haian Xia
Bio-based plastics have received much attraction because they are an alternative to petroleum-based plastics in recent years. Among them, aliphatic polyesters have garnered the most attention due to their excellent properties. Polyester is primarily synthesized through ring opening polymerization of monomer, and the catalysts used are mostly synthesized through “click” reaction in the laboratory, which exhibits inferior activity and little commercial value. Herein, a facile approach was developed for the synthesis of high molecular-weight cyclic aliphatic polyesters, specifically poly(valerolactone- co -caprolactone) with varying compositions. This involved the ring-opening copolymerization of ε-caprolactone (ε-CL) and δ-valerolactone (δ-VL) in the absence of an initiator with commercial hydrogen bond donor triclorocarban and an organic base. The structure and properties of the prepared cyclic polyester were investigated using GPC, 13 C NMR, 1 H NMR, MALDI-TOF mass spectrometry, TOF-SIMS mass spectrometry, differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and X-ray diffraction (XRD) techniques. The results show that the molecular weight of cyclic polyester can rapidly exceed 40 kDa, with a PDI of approximately 1.10. In comparison to linear polyester, it has a higher melting point and superior thermodynamic properties, thus presenting greater application potential. Finally, based on nuclear magnetic resonance titration, the potential catalytic processes and mechanisms of bimolecular systems on monomers in different environments were discussed. This study not only offers new insights into the structure and properties of cyclic polyesters, but also presents novel bimolecular catalytic systems using commercial urea hydrogen bond donors for the synthesis of cyclic polymer polyesters.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Luotian Lv,Yao Liu,Yankai Huang,Tong Li,Han Feng,Yongqing Wang
Since the intensification of global environmental pollution and energy shortages, photocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as a promising strategy to convert solar energy into clean chemical energy. Herein, we construct a robust and efficient heterojunction construction photocatalyst for CO 2 RR, composed of the highly reactive CeNi quantum dots (CeNi QDs) and nickel metal–organic layer (Ni-MOL) ultrathin nanosheets. This design facilitates the rapid separation of photogenerated charge carriers, as confirmed by X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and other characterizations. Mechanistic studies with in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and the d-band center calculation indicate that the propensity of photocatalyst for CO 2 absorption and CO desorption, leading to high performance and selectivity. The optimized loading amount of CeNi quantum dots and modified structure result in a CO yield of 30.53 mmol·g −1 within 6 h under irradiation. This work not only paves a new and convenient way for developing high-activity quantum dot materials for CO 2 RR but also exploits novel avenues to fabricate more heterojunction composites for solar energy conversion.
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Foods
·
2024
·Vol. 13
·期 11
·1593
·
IF 4.7
Fangying Xian,Lin Yang,Huaqing Ye,Jinlin Xu,Xiaoping Yue,Xiaolan Wang
Douchi is a Chinese traditional fermented food with a unique flavor. Methyl anthranilate (MA) plays an important role in formation of this flavor. However, the complicated relationship between the MA formation and the metabolic mechanism of the key functional microorganisms remains unclear. Here, we elucidated the response mechanism of aroma production driven by high salt stress inTrichomonascus ciferriiWLW (T. ciferriiWLW), which originates from the douchi fermentation process. The highest production of MA was obtained in a 10% NaCl environment. The enhanced expression of the key enzyme genes of the pentose phosphate pathway and shikimic acid pathway directed carbon flow toward aromatic amino acid synthesis and helped sustain an increased expression ofmetKto synthesize a large amount of the methyl donorS-adenosylmethionine, which promoted methyl anthranilate yield. This provides a theoretical basis for in-depth research on the applications of the flavor formation mechanisms of fermented foods.
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危险品化学品经营许可证（带存储）