CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2023
·Vol. 39
·期 6
·948-953
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IF 3.1
Xu Henan,Zhang Lingling,Wang Huilin,Zhang Shaopeng,Li Wei,Wang Xiao,Song Shuyan,Wang Daguang,Shi Zhan
N anozymes have shown great potential for life sciences owing to their distinct advantages, such as low cost and high stability, compared with natural enzymes. Despite significant progress, state-of-art nanozymes commonly suffer from relatively low specific activities. Herein, we propose a promising to address this issue by creating single-atom nanozymes. A ball-milling-assisted strategy has been developed to induce the transformation of Cu species from bulk to single atoms. The highly-simplified steps allow a large-scale synthesis, that over 4.2 g of single-atom Cu−N doped carbon nanozymes can be achieved in one pot. It exhibits a remarkably improved peroxidase-like activity and stability compared with N doped C anchored Cu nanoparticles. Further experimental firmly reveals the crucial role of the single-atom Cu site that can generate more active ·OH species for boosting the catalytic process.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Weiting Yu,Leben Qiu,Jieyun Zhu,Sizhuo Chen,Shuang Song
The selective catalytic reduction of nitroaromatics towards aromatic amines under mild reaction condition is an important approach to reduce the toxicity of waste effluents from industry and afterwards utilize the product as important fine organic chemical raw materials. P-nitrophenol (PNP) is chosen as the probe molecule of nitroaromatics in this study. A Fe-embedded N-doped Carbon (Fe-N-C) catalyst prepared using ZIF-8 has been identified as a highly active, selective and stable catalyst in the selective catalytic reduction of PNP. The Fe-N-C catalyst is for the first time applied in PNP reduction and found to present 100% conversion and 100% product selectivity . A mechanism investigation has been carried out to conclude that in the PNP reduction on Fe-N-C, water acts as the main hydrogen provider and sodium borohydride is the electron donator. Furthermore, the Fe-N-C catalyst works well when it is applied in PNP degradation in real water samples, which further indicates its applicability in industrial wastewater treatment . This work offers a simple and useful strategy to design robust catalysts for the selective catalytic reduction of nitroaromatics.
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CARBOHYDRATE POLYMERS
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2023
·
IF 11.2
Hongyi Shang,Xinxin Yang,He Liu
The growth of plants is highly dependent on sufficient water and suitable fertilizer nutrients, but the soil often loses moisture and the fertilizers are low efficiency. To address this issue, the temperature-responsive hydrogels were developed using the N-vinylcaprolactam (NVCL) dispersed in water through the emulsification of carboxymethyl cellulose (CMC) and acrylamide (AM), and urea was loaded into the hydrogel as a fertilizer. The amount of CMC and monomer have an effect on the structure, mechanical properties, swelling ability, and temperature sensitivity of the hydrogel. Therefore, the maximum swelling ratio of the hydrogel can reach 2056 % with the increasing hydrophilic groups, and the hydrogel exhibits a deswelling behavior as the temperature rises to higher than LCST due to the temperature responsiveness. Moreover, the fertilizer can rapidly release when the temperature is higher than LSCT, and exhibits similar release behavior in water and soil. Thus, the temperature-responsive hydrogel shows a great potential application for the controlled release of water and fertilizer in agriculture and forestry.
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CURRENT APPLIED PHYSICS
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2023
·
IF 2.4
Youjun Zhao,Lixin Yu,Yakun Deng,Kangliang Peng,Shuai Huang
The nitrogen-doped carbon dots (NCDs) are facilely fabricated by a one-step hydrothermal strategy using citric acid and o-phenylenediamine as start ingredient. The as-synthesized NCDs with a high quantum yield of 38.63% at 370 nm excitation maintain significant fluorescence stability in various complex environments, indicating that NCDs have the possibility of application in harsh environments. Moreover, after adding the Fe 3+ to this as-synthesized NCDs, the emission intensity at 446 nm is remarkably reduced and exhibits line-dependent relationship in the range of 0.5–90 μM with a detection limit of 0.37 μM. Meanwhile, the fluorescence lifetime and absorption characteristics are compared respectively, and Stern−Volmer is calculated. These results illustrate that the quenched fluorescence is attributed to the synergistic effect of internal filtration effect (IFE) and static quenching. Moreover, this carbon-based sensing material has elevated efficiency in detecting Fe 3+ in practical samples, implying that the sensing probe provides a fast and accurate new technique for the detection of Fe 3+ .
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Inorganics
·
2023
·Vol. 11
·期 4
·155
·
IF 2.9
Tie Shi,Yanmei Feng,Yi Zhong,Hao Ding,Kai Chen,Daimei Chen
High photoelectrochemical water oxidation efficiency can be achieved through an efficient photogenerated holes transfer pathway. Constructing a photoanode semiconductor heterojunction with close interface contact is an effective tactic to improve the efficiency of photogenerated carrier separation. Here, we reported a novel photoanode p-n junction of Ti:Fe2O3/Cu2O (n-Ti:Fe2O3and p-Cu2O), Cu2O being obtained by in situ reduction in CuAl-LDH (layered double hydroxides). The Ti:Fe2O3/Cu2O photoanode exhibits a high photocurrent density reaching 1.35 mA/cm2at 1.23 V vs. RHE is about 1.67 and 50 times higher than the Ti:Fe2O3and α-Fe2O3photoanode, respectively. The enhanced PEC activity for the n-Ti:Fe2O3/p-Cu2O photoelectrode is due to the remarkable surface charge separation efficiency (ηsurface85%) and bulk charge separation efficiency (ηbulk72%) formed by the p-n junction and the tight interface contact formed by in situ reduction. Moreover, as a cocatalyst, CuAl-LDH can protect the Ti:Fe2O3/Cu2O photoanode and improve its stability to a certain extent. This study provides insight into the manufacturing potential of in situ reduction layered double hydroxides semiconductor for designing highly active photoanodes in the field of photoelectrochemical water oxidation.
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Catalysts
·
2023
·Vol. 13
·期 4
·651
·
IF 3.9
Jiaqi Du,Yidan Peng,Xu Guo,Guoliang Zhang,Fengbao Zhang,Xiaobin Fan,Wenchao Peng,Yang Li
Researchers studying heterogeneous catalysis are intrigued by single-atom catalysts (SACs) due to their ultrahigh atomic utilization. However, only a few reports on SAC-catalyzed classical organic transformations are available. In this work, atomically dispersed Pd sites are confined to a ZrO2hybridized N-doped carbon skeleton with a smart design. UiO-66-NH2is used to anchor Pd atoms by the coordination of the donor atoms including lone pairs of electrons and metal atoms. Subsequently, the in situ introduction of ZrO2doping is achieved using pyrolysis, which helps improve the catalytic performance by modulating the electronic state. The Pd@ZrO2/N–C catalyst obtained from the unique design exhibits a high yield (99%) in eco-friendly media with an extremely low noble metal dosage (0.03 mol% Pd) for the Suzuki reaction. Moreover, Pd@ZrO2/N–C remains highly active after being reused several times and possesses versatility in a variety of substrates. This strategy offers a feasible alternative to designing SACs with atomically dispersed noble metals for heterogeneous reactions.Keywords:palladium;heterogeneous catalyst;Suzuki reaction;ZrO2doping;N-doped carbon
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2023
·Vol. 98
·期 6
·1435-1442
·
IF 3.4
Hongyu Liu,Xin Wen,Meng Hu,Huan Zhang,Junfu Wei
BACKGROUND Biochar has received much attention for disposal of aqueous organic contaminants because of its great potential in adsorption and catalysis. N-doped rice husk biochar (N-BC) was synthesized in this work and used to activate potassium peroxymonosulfate (PMS) to remove different types of dyes. The influence of preparation conditions of N-BC and reactive conditions on removal rate was discussed in detail. Free radical quenching experiment and electron spin resonance were used to analyze the active species and mechanism in the reaction. RESULTS N-BC with abundant graphitic-N, which is the main form of N to activate PMS, can be obtained by N-doping with carbamide at 900 °C. The removal rate for new coccine can reach nearly 100% in 30 min. Furthermore, the removal rate can still be maintained at 77.21% after reusing four times only washing with water, and it can be further promoted to 98.78% after annealing treatment at 900 °C. N-BC has excellent applicability to different types of dyes. CONCLUSION Consequently, the mechanism is the combination of radical (O 2 •− ) and nonradical ( 1 O 2 ) oxidation. First, the preparation method in this work is relatively simple. Second, the material can adapt to a very wide pH range. Third, the material shows high efficiency at room temperature (the removal rate can reach nearly 100% in 30 min). Fourth, the material shows high efficiency with only a small amount. This study provides a new path of rapid dye water purification using biochar, with simple synthesis, wide pH range adaptability, and high efficiency with only a small amount. © 2023 Society of Chemical Industry (SCI).
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
·
IF 6
Xi Han,Zhenjian Jia,Weixing Zhou,Haiyan Zhang
The chemical heat sink of endothermic hydrocarbon fuel has been used to solve the thermal protection problem caused by the high temperature of the scramjet combustion chamber. The fuel is usually in a supercritical state in the cooling channel, so we studied the cracking of n-decane initiated by nitromethane under supercritical pressure in an electrically heated flow reactor. Based on the experimental results, the published low-pressure cracking model and the latest theoretical results, a detailed kinetic reaction model under supercritical conditions of n-decane cracking initiated by nitromethane, including 271 species and 1863 reactions, was established. Through the simulation of the experimental results and the experimental results in the literature, it was proven that this model had good simulation accuracy. The formation rate of n-decane was analyzed to obtain the consumption path of n-decane under supercritical pressure, especially the generation process of C 3 above alkanes. The influence of nitromethane on n-decane consumption and product distribution and the cause of its range of action were also analyzed, which provided a theoretical and model basis for the engineering application of fuel.
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TALANTA
·
2023
·
IF 6.1
Yichen Lu,Chengrun Du,Hongmei Ying,Yunfan Lin,Qinying Gu,Fangfang Kong,Hongli Zhao,Minbo Lan
The development of facilely synthetic materials acts an essential role in glycoproteome analysis, especially for the highly efficient enrichment of N-linked glycopeptides . In this work, a facile and timesaving route was introduced in which COF TP-TAPT served as a carrier and poly (ethylenimine) (PEI) and carrageenan (Carr) were successively coated on the surface via electrostatic interaction . The resultant COF TP-TAPT @PEI@Carr showed remarkable performance in glycopeptide enrichment with high sensitivity (2 fmol μL −1 ), high selectivity (1:800, molar ratio of human serum IgG to BSA digests), large loading capacity (300 mg g −1 ), satisfactory recovery (102.4 ± 6.0%) and reusability (at least eight times). Due to the brilliant hydrophilicity and electrostatic interactions between COF TP-TAPT @PEI@Carr and positively charged glycopeptides , the prepared materials could be applied in the identification and analysis in the human plasma of healthy subjects and patients with nasopharyngeal carcinoma. As a result, 113 N-glycopeptides with 141 glycosylation sites corresponding to 59 proteins and 144 N-glycopeptides with 177 glycosylation sites corresponding to 67 proteins were enriched from 2 μL plasma trypsin digests of the control groups and patients with nasopharyngeal carcinoma, respectively. 22 glycopeptides were identified only from the normal controls and 53 glycopeptides were detected only from the other set. The results demonstrated that this hydrophilic material was promising on a large scale and further N-glycoproteome research.
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JOURNAL OF COORDINATION CHEMISTRY
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2023
·
IF 1.9
Ming-Ming Wang,Xiaofei Kuang,Ting-Ting Li,Hui Yang,Ying-Hao Mi,Ying-Chao Xu,Can-Zhong Lu
Luminescent Cu(I) complexes have drawn considerable attention as alternative materials to precious transition metal complexes due to their low cost and electron configuration. Discrete heteroleptic diamine-diphosphine copper(I) complexes have been investigated owing to their outstanding photophysical features. However, heteroleptic copper(I) coordination polymers remain mostly unexplored. Herein, we report the synthesis and photophysical characterization of a heteroleptic copper(I) coordination polymer by employing bidentate oxybis(2,1-phenylene)bis(diphenylphosphine) (POP) diphosphine and nitrogen heterocyclic 5-[4-(1-imidazolyl)phenyl]-2H-tetrazole (ipt) as ligands. By utilizing the mixed-solvent strategy, a one-dimensional (1D) linear chain was constructed under solvothermal reaction conditions. Temperature-dependent emission spectra combined with decay time measurements demonstrate that emission originated from triplet phosphorescence at ambient temperature.
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Nanomaterials
·
2023
·Vol. 13
·期 7
·1188
·
IF 5.3
Lina Sun,Liping Sun,Lihua Huo,Hui Zhao
H2O2generation via an electrochemical two-electron oxygen reduction (2e−ORR) is a potential candidate to replace the industrial anthraquinone process. In this study, porous carbon catalysts co-doped by nitrogen and oxygen are successfully synthesized by the pyrolysis and oxidation of a ZIF-67 precursor. The catalyst exhibits a selectivity of ~83.1% for 2e−ORR, with the electron-transferring number approaching 2.33, and generation rate of 2909.79 mmol g−1h−1at 0.36 V (vs. RHE) in KOH solution (0.1 M). The results prove that graphitic N and –COOH functional groups act as the catalytic centers for this reaction, and the two functional groups work together to greatly enhance the performance of 2e−ORR. In addition, the introduction of the –COOH functional group increases the hydrophilicity and the zeta potential of the carbon materials, which also promotes the 2e−ORR. The study provides a new understanding of the production of H2O2by electrocatalytic oxygen reduction with MOF-derived carbon catalysts.Keywords:porous carbon;two-electron reduction of oxygen;hydrogen peroxide;electrocatalyst
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Food Science and Human Wellness
·
2023
·
IF 7
Linglin Fu,Rongrong Wang,Jinru Zhou,Chong Wang,Yanbo Wang
N -glycans in many proteins are of great concern because of their strong association with food allergies. Triticum aestivum (bread wheat), a major food crop, is known as one of the “Big Eight” allergenic groups. However, little research has been done about N -glycans in wheat glycoproteins. In this study, a soluble wheat glycoprotein was purified from wheat and further identified as globulin-1 S allele (GSA). The wheat GSA displayed significant IgE-binding activity. Moreover, one N -glycosylation site and 6 kinds of N -glycans were identified by mass spectrometry, including 3 high mannose types and 3 complex types. Furthermore, the IgE-binding activity of wheat GSA is proved to be reduced by the removal of N -glycan, thermal treatment (temperatures > 80 °C), and strong acidic treatment (pH 3.0). These findings would provide a better understanding of the effects of N -glycosylation, thermal treatment, and acidic treatment on the molecular characteristics of GSA, and further provide new insights into the development of hypoallergenic wheat products.
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