CELLULOSE
·
2023
·Vol. 30
·期 16
·10243-10255
·
IF 5.7
Liu Yaqing,Zhang Xi,Huang Xudong,Shao Linjun,Xing Guiying,Qi Chenze,Zhou Shujing,Li Jinjing
Palladium cation embedded cellulose acetate/poly(vinyl butyral) composite superfine fibers were successfully fabricated by electrospinning. Then, these composite fibers were treated with hydrazine hydrate/NaOH/ethanol solution to regenerate cellulose from cellulose acetate and poly(vinyl alcohol) from poly(vinyl butyral). Meanwhile, the Pd 2+ cations were reduced to Pd 0 nanoparticles, which were evenly dispersed inside the fibers. The catalytic performance of these embedded Pd 0 nanoparticles were evaluated by Suzuki reaction. The catalysis results show that this novel fibrous catalyst was highly active to catalyze the Suzuki reaction of aromatic iodides and bromides with yields over 90%. Moreover, this fibrous palladium catalyst could be readily recovered and reused for 15 times with little loss of initial catalytic activity. The high catalytic activity can be ascribed to the superfine diameter of fibers while the excellent recyclability can be attributed to the embedment of active palladium species inside the fibers. Therefore, we have developed a facile method to prepare highly active and stable cellulose supported palladium fibrous catalysts.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 11
·4477-4488
·
IF 1.6
Zou Jin-Zhao,Xu Shi-Zhuan,Wang Peng,Cao Chang-Qing,Yan Chao,You Yan,Lu Jun-Qiang,Zhu Li-Bing,Zhu Zhi-Yong,Lin Jun
A solid-phase metallurgy combined with spark plasma sintering technology was used to prepare U 3 Si 2 pellets. The thermal conductivity and oxidation behavior of the pellets were studied. The pellets were highly dense (> 98% theoretical density) and had an ultra-high phase purity. The thermal conductivity of the U 3 Si 2 pellets increased linearly with temperature from 300 to 973 K. By further annealing the pellets at 300 °C in air for two hours, the oxidation onset temperature was increased from 490 to 520 °C. A mechanism of pore passivation was proposed to account for the enhanced oxidation resistance.
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Communications Chemistry
·
2023
·Vol. 6
·期 1
·1-10
·
IF 5.9
Li Pan,Gemayel Rachel,Li Xue,Liu Jiangping,Tang Mingjin,Wang Xinming,Yang Yan,Al-Abadleh Hind A.,Gligorovski Sasho
Heterogeneous reaction of gas phase NO 2 with atmospheric humic-like substances (HULIS) is potentially an important source of volatile organic compounds (VOCs) including nitrogen (N)-containing compounds, a class of brown carbon of emerging importance. However, the role of ubiquitous water-soluble aerosol components in this multiphase chemistry, namely nitrate and iron ions, remains largely unexplored. Here, we used secondary electrospray ionization ultrahigh-resolution mass spectrometry for real-time measurements of VOCs formed during the heterogeneous reaction of gas phase NO 2 with a solution containing gallic acid (GA) as a proxy of HULIS at pH 5 relevant for moderately acidic aerosol particles. Results showed that the number of detected N-containing organic compounds largely increased from 4 during the NO 2 reaction with GA in the absence of nitrate and iron ions to 55 in the presence of nitrate and iron ions. The N-containing compounds have reduced nitrogen functional groups, namely amines, imines and imides. These results suggest that the number of N-containing compounds is significantly higher in deliquescent aerosol particles due to the influence of relatively higher ionic strength from nitrate ions and complexation/redox reactivity of iron cations compared to that in the dilute aqueous phase representative of cloud, fog, and rain water.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·111152-111164
·
IF 5.8
Yang Qian,Wang Xueting,Shi Jing,Wei Jiaqi,He Yangqing
Despite S-doped C 3 N 4 can exhibit more efficient photo-reactivity than pure C 3 N 4 , there is still some space to further improve the detaching efficiency of electron-hole and enhance the photocatalytic efficiency of S-C 3 N 4 . The construction of heterojunction is an effective method to promote the photocatalytic efficiency. ZnIn 2 S 4 , as a novel photocatalyst, its VB (1.37 V) and CB (− 1.09 V) can match with S-C 3 N 4 . Therefore, we hope to construct the ZnIn 2 S 4 /S-C 3 N 4 heterojunction for boosting the photocatalytic activity of S-C 3 N 4 . In this paper, ZnIn 2 S 4 /S-C 3 N 4 heterojunction was prepared through hydrothermal method using S-C 3 N 4 , ZnCl 2 , InCl 3 ·4H 2 O, and thioacetamide as raw materials and heated at 160 °C for 16 h. The optimum 18% ZnIn 2 S 4 /S-C 3 N 4 nanocomposites exhibit dramatically enhanced photocatalytic performance for degradation of tetracycline with 86.3% removal rate within 120 min, higher than 50% degradation efficiency of pure S-C 3 N 4 . And in the process of photodegradation for tetracycline, the largest contribution rate is the photo-excited cavity (h + ), followed by ·O 2 − and ·OH. Herein, we have provided a good example for removing antibiotic residues by using S-C 3 N 4 -based heterojunction towards environmental remediation.
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Light-Science & Applications
·
2023
·Vol. 12
·期 1
·1-12
·
IF 19.4
Liu Dongjie,Li Guogang,Dang Peipei,Zhang Qianqian,Wei Yi,Qiu Lei,Lian Hongzhou,Shang Mengmeng,Lin Jun
Achievement of high photoluminescence quantum efficiency and thermal stability is challenging for near-infrared (NIR)-emitting phosphors. Here, we designed a “kill two birds with one stone” strategy to simultaneously improve quantum efficiency and thermal stability of the NIR-emitting Ca 3 Y 2-2 x (ZnZr) x Ge 3 O 12 :Cr garnet system by chemical unit cosubstitution, and revealed universal structure-property relationship and the luminescence optimization mechanism. The cosubstitution of [Zn 2+ –Zr 4+ ] for [Y 3+ –Y 3+ ] played a critical role as reductant to promote the valence transformation from Cr 4+ to Cr 3+ , resulting from the reconstruction of octahedral sites for Cr 3+ . The introduction of [Zn 2+ –Zr 4+ ] unit also contributed to a rigid crystal structure. These two aspects together realized the high internal quantum efficiency of 96% and excellent thermal stability of 89%@423 K. Moreover, information encryption with “burning after reading” was achieved based on different chemical resistance of the phosphors to acid. The developed NIR-emitting phosphor-converted light-emitting diode demonstrated promising applications in bio-tissue imaging and night vision. This work provides a new perspective for developing high-performance NIR-emitting phosphor materials.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Xiong Lianhu,Wei Yun,Chen Chuanliang,Chen Xin,Fu Qiang,Deng Hua
Passive daytime radiative cooling is a promising path to tackle energy, environment and security issues originated from global warming. However, the contradiction between desired high solar reflectivity and necessary applicable performance is a major limitation at this stage. Herein, we demonstrate a “Solvent exchange-Reprotonation” processing strategy to fabricate a lamellar structure integrating aramid nanofibers with core-shell TiO 2 -coated Mica microplatelets for enhanced strength and durability without compromising optical performance. Such approach enables a slow but complete two-step protonation transition and the formation of three-dimensional dendritic networks with strong fibrillar joints, where overloaded scatterers are stably grasped and anchored in alignment, thereby resulting in a high strength of ~112 MPa as well as excellent environmental durability including ultraviolet aging, high temperature, scratches, etc. Notably, the strong backward scattering excited by multiple core-shell and shell-air interfaces guarantees a balanced reflectivity (~92%) and thickness (~25 μm), which is further revealed by outdoor tests where attainable subambient temperature drops are ~3.35 °C for daytime and ~6.11 °C for nighttime. Consequently, both the cooling capacity and comprehensive outdoor-services performance, greatly push radiative cooling towards real-world applications.
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Nano Research
·
2023
·Vol. 16
·期 11
·12697-12705
·
IF 9.9
Gao Xinshuang,Zheng Jia-jia,Li Hanbo,Cai Rui,Gao Xingfa,Wu Xiaochun
Nanozymes, as a novel form of enzyme mimics, have garnered considerable interest. Despite overcoming the main disadvantages of their natural analogs, they still face challenges such as restricted mimic types and low substrate specificity. Herein, we introduce a reactive ligand modification strategy to diversify enzyme mimic types. Specifically, we have utilized helical plasmonic nanorods (HPNRs) modified with para -nitrothiophenol (4-NTP) to create an oxygen-sensitive nitroreductase (NTR) with light-controllability. HPNRs act as a light-adjustable source of nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate (NAD(P)H), providing photon-generated energetic electrons to adsorbed 4-NTP molecules. In the presence of O 2 , the activated 4-NTP transfers the captured electron to the adsorbed O 2 , mimicking the electron transfer process in its natural counterpart. This enhanced O 2 activation notably boosts the oxidative coupling of para -aminothiophenol (4-ATP). Density functional theory (DFT) calculations reveal that hot electrons injected into the lowest unoccupied molecular orbital (LUMO) energy level of 4-NTP can be transferred to that of molecular oxygen. In conclusion, our findings underline the potential of the reactive ligand modification strategy in developing new types of enzyme reactions, which opens up promising avenues for the enhancement and diversification of nanozyme functionalities.
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CELLULOSE
·
2023
·Vol. 30
·期 16
·10519-10531
·
IF 5.7
Tang Xin,Zhang Zaixing,Jing Lingxiao,Luan Kun,Zhou Sha,Zhang Tonghua
The incorporation of a single antimicrobial agent on textiles has been proven to be effective to enhance the antibacterial efficacy against single bacteria family. However, the daily usage of textile products face challenges from multiple microbes, i.e., bacterial, fungal, or/and viral, which threaten human’s safety and health. A “combination” of antimicrobial agents could be efficient and accessible to against several microbes at one time. In this study, a Schiff base-pyridinium quaternary ammonium salt-halamine precursor compound (E)-3-(((2,4-dioxoimidazolidin-1-yl)imino)methyl)pyridin-1-ium (4-DMPY) was synthesized and grafted onto MPTES-treated cotton fabric by thiol-ene click chemistry. The results of NRM, FTIR, Raman, EDX, XPS and SEM tests showed that 4-DMPY was synthesized and grafted onto cotton fabrics. The antibacterial test results showed that 4-DMPY had antibacterial activity against both Staphylococcus aureus and Escherichia coli . The antibacterial activity of 4-DMPY-finished cotton fabric was significantly enhanced after chlorination treatment, which could kill 98% of S. aureus and 98.9% of E. coli at a concentration of 5 g/L, confirming the enhanced synergistic effect between 4-DMPY and N -chloramine. The antimicrobial substance on the cotton fabric is non-soluble, which kills 98.4% E. coli and 98.3% S. aureus within 1 min by a direct contact. In addition, the produced fabric retained 81% and 63% of active chlorine content after 30 washes and 30 days of storage, indicating a good antimicrobial durability. Herein, we anticipate the technology can be used to enhance antibacterial function of cellulose products and thus resist the potential threats from microbes to ensure human’s health.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 31
·期 5
·7027-7042
·
IF 5.8
Chen Xuewen,Quan Hongping,Yu Jie,Hu Yuling,Huang Zhiyu
In order to reduce the impact of greenhouse gases on the environment, the development of various new CO 2 capture materials has become a hot spot. In this work, a novel composite amine solid adsorbent was prepared by simultaneously using tetraethylenepentamine (TEPA) and 2-[2-(dimethylamino) ethoxy] ethanol (DMAEE) for amine functionalization on the polyester microsphere carrier. The introduction of methyl methacrylate (MMA) with high glass transition temperature into the polyester carrier makes the carrier microspheres have high hardness. At the same time, the carrier also contains active epoxy groups and hydrophobic glycidyl methacrylate (GMA, which can undergo ring-opening reaction with composite amines to achieve high-load and low-energy chemical grafting of amines on the carrier. The composite aminated polyester microspheres were used as an efficient adsorbent for CO 2 in simulated flue gas. The results show that the synergistic effect of TEPA-DMAEE composite amine system in the adsorbent is beneficial to the improvement of CO 2 capture capacity. When the total amine content in the impregnating solution is 45 wt% and the composite amine ratio is TEPA: DMAEE = 6: 4, the CO 2 adsorption capacity can reach the optimal value of 2.45 mmol/ g at 70 °C. In addition, the composite amine microsphere adsorbent has cyclic regeneration performance. Importantly, through kinetic fitting, the Avrami kinetic model fits the CO 2 adsorption better than the quasi-first-order and quasi-second-order kinetic models, which proves that physical adsorption and chemical adsorption coexist in the adsorption process. This simple, long-term stable and excellent selective separation performance makes amine-functionalized adsorbents have potential application prospects in CO 2 capture. Graphical abstract
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Zhang Xian,Liu Ze,Khan Hafiz Ihsan Ul haq,Barati Bahram,Parakhonskiy Bogdan,Skirtach Andre G.,Rousseau Diederik P. L.,Van Hulle Stijn
Nitrogen source–modified biochar was produced from rice straw–derived biochar (RSBC) via pyrolysis carbonization using nitrogen sources such as ammonium chloride, dicyandiamide, melamine, thiourea, and urea. The characteristics of the resulting biochars were compared, including their elemental compositions, surface functional groups, and morphology. The N-modified biochar contained N- and O-based groups (N–H, C–N, C≡N, O–H, and C–O), primarily consisted of mesopores (3.01 ~ 14.42 nm pore diameter), and had a specific surface area ranging from 95.87 to 167.86 m2 g −1 . The N-modified biochar’s BPA adsorption capacity was correlated to the activation temperature (correlation coefficient n = 0.5), with adsorption capacities varying from 7.43 to 63.09 mg g −1 . Ammonium chloride–modified biochar synthesized at 800 °C had over twice the BPA adsorption capacity of pristine biochar (28.80 mg g −1 ) among various nitrogen sources evaluated. The pseudo-second-order model characterized the adsorption kinetics of BPA, while the Freundlich model faithfully captured its isotherms. This study emphasizes the significance of proper nitrogen source selection and optimal modification temperatures to enhance the BPA adsorption capacity of biochar. Graphical Abstract
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Frontiers of Chemical Science and Engineering
·
2020
·Vol. 15
·期 2
·269-278
·
IF 3.552
Hou Yuexin,Li Xiaoyun,Sun Minghui,Li Chaofan,Bakhtiar Syed ul Hasnain,Lei Kunhao,Yu Shen,Wang Zhao,Hu Zhiyi,Chen Lihua,Su Bao-Lian
Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios (Hier-ZSM-5- x , where x = 50, 100, 150 and 200) were synthesized using an ordered mesoporous carbon-silica composite as hard template. Hier-ZSM-5- x exhibits improved mass transport properties, excellent mechanical and hydrothermal stability, and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction. Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores, which increases the final catalytic conversion. The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites. These poisoned Hier-ZSM-5- x shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite, which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant, leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites. This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.
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AMINO ACIDS
·
2019
·Vol. 52
·期 3
·361-369
·
IF 2.52
Li Jinlei,Lu Kui,Lv Mingxiu,Liu Guangbin,Ma Li,Qi Jianzhao
Breast cancer susceptibility gene 2 ( BRCA2 ) is an important tumor suppressor, which is participated in repair of damaged DNA by its highly conserved BRC repeat motifs regulating RAD51 protein homologous recombination and thereby preventing cell carcinogenesis. In this study, the BRCA2(1524–1548)–RAD51(241–260) complex structure was obtained based on PDB bank data 1N0W, which provided the basis for site-specific mutation of BRCA2(1524–1548). The BRC4 and BRC4 analogous peptides were synthesized, and the interaction between BRC peptide and RAD51(241–260) was studied by fluorescence spectroscopy, circular dichroism spectroscopy and microscale thermophoresis (MST). The results of circular dichroism showed that the changes in secondary structures of RAD51(241–260) occurred after adding BRC4 analogous peptides, and the α-helix content increased significantly. Fluorescence spectral data demonstrated that the model of BRC peptide binding to RAD51(241–260) was static quenching, and the binding constants of BRC4, P1, P2, P4 with RAD51(241–260) were 1.647 × 10 −4 L mol −1 , 2.532 × 10 −4 L mol −1 , 3.161 × 10 −4 L mol −1 , 1.705 × 10 −4 L mol −1 , respectively. The results of MST indicated that P2 and RAD51(241–260) have better affinity for dissociation constant 44.286 μM. The strongest affinity between P2 and RAD51(241–260) indicated that the mutation of amino acid residue constituting BRC α-helix affects the structure and interaction of BRC peptide and RAD51(241–260).
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