SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Huimin Yang,Zhenming Du,Yazhou Yang,Xiang Li,Qirui Wu,Jiahong Tang,Xiaoxia Wang,Dawen Zeng
Nitrogen dioxide (NO 2 ) is a common gas that can cause irreversible damage to human health, emphasizing the essentiality of developing highly sensitive NO 2 sensors with good selectivity and low consumption. Here, a facile in–situ cation exchange method was employed to successfully synthesize interlayer expansion Ag intercalated SnS 2 with S vacancies for NO 2 gas sensing. The presence of S vacancies strongly improves the electronic structure of SnS 2 and significantly facilitates the interaction of NO 2 with the sensor. Moreover, the interlayer spacing of SnS 2 is expanded by 0.48 Å after Ag intercalation, prompting diffusion behavior of NO 2 molecules between the interlayers. Benefiting from the factors above, SnS 2 –Ag exhibited excellent gas sensing performance for NO 2 with a high response to 5 ppm NO 2 (response value = 8.37) and detection limits as low as 200 ppb at a low temperature of 100 °C. This work combines defect engineering with interlayer engineering to provide a new perspective for extending the application of SnS 2 gas sensors.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yuelong Xu,Jingyue Wang,Shasha Wang,Zuozhao Zhai,Bin Ren,Zhi Tian,Lihui Zhang,Zhenfa Liu
Multifunctional electrocatalysts are desirable for overall water splitting and zinc-air batteries. In this work, N, S co-doped carbon nanotubes (CNT-NS) with a plentiful of defects were obtained through a novel molecular-level codoped and lattice defect construction method. Thiamine hydrochloride and thiocarbamide were adopted as new precursors in situ doping N and S into multi-walled CNTs surfaces, and lattice defects were constructed by in situ chemical etching using ammonium chloride and ammonium bicarbonate . These surface defects and N,S biatom co-doping synergistic effects can accumulate the CNT-NS to exhibit the superior behavior for electrocatalysis of water splitting and zinc-air batteries. The overpotential for overall water splitting was 1.61 V and the specific capacity for zinc-air batteries was 781 mA h g −1 , which was superior to previous works. According to the Operando Raman spectroscopy measurements, the S atoms can serve as the intrinsic catalytic sites for HER and OER , and the defective CNT structures could enhance the catalytic kinetics by the electron-transfer process. Further, density functional theory (DFT) results also indicated the contribution of binary atoms co-doping for low ΔG H∗ values. Therefore, this work provides the valuable reference for rational design/construction for metal-free catalysts of overall water splitting.
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Bioresources and Bioprocessing
·
2023
·Vol. 10
·期 1
·1-10
·
IF 4.6
Zhang Man,Huang Zheng-Yu,Su Ying,Chen Fei-Fei,Chen Qi,Xu Jian-He,Zheng Gao-Wei
Tetrahydroisoquinoline alkaloids (THIQAs) are ubiquitous compounds with important pharmaceutical and biological activity. Their key N-heterocyclic structural motifs are synthesised via Pictet–Spengler (P–S) reaction by norcoclaurine synthases (NCS) in plants. The synthesis of 1-aryl-tetrahydroisoquinoline alkaloids has attracted increasing attention due to their antitumor and antivirus activities. Herein, the L68T/M97V mutant of NCS from Thalictrum flavum with improved activity was developed by semi-rational design. This mutant not only showed higher catalytic performance (> 96% conversion) toward benzaldehyde and dopamine over the wild-type enzyme, but also catalysed the P–S reaction of the bulky substrate 4-biphenylaldehyde and dopamine with high conversion (> 99%) for the effective synthesis of 1-aryl-THIQA. In terms of stereoselectivity, all products synthesised by the L68T/M97V mutant showed high optical purity (92–99% enantiomeric excess).
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Advanced Healthcare Materials
·
2023
·
IF 10
Zhuoran Yang,Chunyu Yang,Dan Yang,Ye Zhang,Qingzhu Yang,Fengyu Qu,Wei Guo
Ferroptosis has recently attracted much attention as an anti-tumor therapy. Evidence suggests that ferroptosis can induce oxidative stress and accumulation of lethal lipid peroxides in cancer cells, leading to cell damage. However, unsuitable pH, H 2 O 2 levels, and high glutathione (GSH) expression in the tumor microenvironment hinder the development of ferroptosis-mediated therapy. In this study, an l -arginine ( l -arg)-modified CoWO 4 /FeWO 4 (CFW) S-scheme heterojunction is strategically designed and constructed for ultrasound (US)-triggered sonodynamic- and gas therapy-induced ferroptosis. CFW not only has excellent Fenton-catalytic activity, outstanding GSH consumption capacity, and excellent ability to overcome tumor hypoxia, but its S-scheme heterostructure can also avoid the rapid combination of electron (e) and hole (h + ) pairs, thereby enhancing the sonodynamic effects. As a precursor of nitric oxide (NO), l -arg is modified on the surface of CFW (CFW@ l -arg) to achieve controlled NO release under US irradiation, thereby enhancing ferroptosis. In addition, poly(allylamine hydrochloride) is further modified on the surface of CFW@ l -arg to stabilize l -arg and achieve controllable NO release. Both in vitro and in vivo results demonstrate that such a multifunctional therapeutic nanoplatform can achieve high therapeutic efficacy through sonodynamic and gas therapy-enhanced ferroptosis. This designed oncotherapy nanoplatform provides new inspiration for ferroptosis-mediated therapy.
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NEW CARBON MATERIALS
·
2023
·
IF 5.7
Jing-yi Niu,De-qi Jing,Xing-hua Zhang,Wei-guo Su,Shou-chun Zhang
Hollow porous carbon fibers for Li-S battery electrodes were prepared by the KOH activation of carbon prepared from hollow polyacrylonitrile fibers. The fibers had a high specific surface area of 2 491 m 2 ·g −1 , a large pore volume of 1.22 cm 3 ·g −1 and an initial specific capacity of 330 mAh·g −1 at a current density of 1 C. To improve their electrochemical performance, the fibers were modified by treatment with hydrazine hydrate to prepare nitrogen-doped hollow porous carbon fibers with a specific surface area of 1 690 m 2 ·g −1 , a pore volume of 0.84 cm 3 ·g −1 and a high nitrogen content of 8.81 at%. Because of the increased polarity and adsorption capacity produced by the nitrogen doping, the initial specific capacity of the fibers was increased to 420 mAh·g −1 at a current density of 1 C.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Qiang Li,Lijie Wang,Jupu Song,Linshen Zhang,Chunfeng Shao,Hong Li,Hemin Zhang
Construction of heterojunction photocatalysts is a valid tactics to boost the photocatalytic property of catalyst. Herein, a novel S-scheme heterojunction of zero/three dimensional (0D/3D) In 2 S 3 /Bi 2 WO 6 hybrid catalyst was obtained by assembling In 2 S 3 nanoparticles on floriated shaped Bi 2 WO 6 microsphere through a simple precipitation route for the first time. The morphology, structures, composition, chemical and optical properties of the resulting materials were carefully researched through various instruments. The degradation experiments revealed that In 2 S 3 /Bi 2 WO 6 composites exhibited superior photocatalytic behavior for dyes decomposition. The optimized In 2 S 3 /Bi 2 WO 6 composite showed remarkable photocatalytic decomposition Rhodamine B (RhB) and Methylene blue (MB), 16.0 (2.68)-fold and 70.3 (1.66)-fold larger than that of pristine Bi 2 WO 6 (In 2 S 3 ), and it also possessed good stability and reusability. The largely improved photoactivity may derive from the formed S-scheme heterojunction between Bi 2 WO 6 and In 2 S 3 , which accelerated photocarriers disassociation and retained strong redox power. Liquid chromatography-mass spectrometry (LC-MS) was applied to reveal the RhB decomposition pathway. Besides, the S-scheme charge transfer mechanism was well elucidated based on in-situ X-ray photoelectron spectroscopy analysis, density functional theory calculation (DFT), and trapping experiment along with electron paramagnetic resonance (EPR) tests.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Honghong Lei,Peng Jiang,Bin Li,Yuncheng Zhou,Rui Zhang,Jianlei Kuang,Wenbin Cao,Wei Wang
The (S, N) co-doped Ba 2 In 2- x Cr x O 5+ y (0 ≤ x ≤ 0.5) oxides are successfully obtained by mixing the Ba 2 In 2- x Cr x O 5+ y oxides and thiourea through a simple ball milling method followed by sintering at 400 °C for 3 h. The colors of the compounds change from orange-brown to yellow-green after reacting with thiourea. When Cr amount is small ( x = 0.1), the crystal structure of (S, N) co-doped Ba 2 In 2- x Cr x O 5+ y is orthorhombic Ba 2 In 2 O 5 phase. When x ≥ 0.3, the crystal structure of the sample is cubic BaInO 2.5 phase. And this phase transition is the same as Ba 2 In 2- x Cr x O 5+ y . XPS results reveal that Cr 6+ in Ba 2 In 2- x Cr x O 5+ y (0 ≤ x ≤ 0.5) oxides are reduced to Cr 3+ after sintering. S exists in both cation and anion forms, and N exists in substitutional forms. UV–Vis analysis indicates that the yellow-green hue comes from the d-d transition of Cr 3+ , and the doping of S, N ions leads to a red shift of the absorption edge of the samples.
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ADVANCED SYNTHESIS & CATALYSIS
·
2019
·Vol. 361
·期 13
·3191-3199
·
IF 5.451
Shuyun Ju,Mingxin Qian,Gang Xu,Lirong Yang,Jianping Wu
Optically pure 1,2,3,4-tetrahydroisoquinoline carboxylic acids constitute an important class of building blocks for the synthesis of natural products and synthetic pharmaceuticals. However, redox deracemization of racemic 1,2,3,4-tetrahydroisoquinoline carboxylic acids as an attractive method is still challenging for the lack of suitable oxidoreductases. Herein, a D-amino acid oxidase from Fusarium solani M-0718 ( Fs DAAO) with broad substrate scope and excellent enantioselectivity was exploited through genome mining, and applied for the kinetic resolution of a number of racemic 1- and 3-carboxyl substituted tetrahydroisoquinolines to yield the corresponding ( S )-enantiomers with excellent enantiomeric excess ( ee ) values (up to >99%). By using Fs DAAO in combination with ammonia-borane in one pot, deracemization of these racemic carboxyl-substituted tetrahydroisoquinolines was achieved with conversions up to >98% and >99% ee . Preparative-scale deracemization of racemic 1,2,3,4-tetrahydroisoquinoline-1-carboxylic acid and 1,2,3,4-tetrahydroisoquinoline-3-carboxylic acid was also demonstrated with good isolated yields (82% and 73%, respectively) and ee >99%. Our study provides an effective method for the synthesis of enantiomeric pure 1,2,3,4-tetrahydroisoquinoline carboxylic acids. This method is expected to provide access to chiral carboxyl-substituted 1,2,3,4-tetrahydroquinolines and 1,2,3,4-tetrahydro-ß-carbolines.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Yinglin Yan,Mangmang Shi,Yiming Zou,Yiqi Wei,Liping Chen,Chaojiang Fan,Rong Yang,Yunhua Xu
It had been proven that carbon aerogel (CA) can effectively improve the conductivity of sulfur (S) and suppress the shuttle effect of polysulfides in Li-S batteries, due to its outstanding electrical conductivity and micropore-rich structure. However, the microstructure of CA was easy to collapse and shrink during carbonization, resulting in a dramatically drop in specific surface area and porosity. Herein, graphene nanosheets (GNs) were introduced in CA to reinforce the structural stability. As-prepared CA/GNs composites were fabricated from in-situ polymerization of resorcinol (R) and formaldehyde (F) in graphene oxide (GO) solution. It was found that the mass concentration of the GO solution had a significantly positive effect on hierarchical porous structure of the CA/GNs composites, which presented improve the electrochemical performances due to the combination of micro-, meso- and macro-pores. It is worth noting that the CA/GNs0.1 sample, obtained from 10 wt % GO solution, possessed the largest specific surface area of 665.477 m 2 g −1 and the largest pore volume of 0.912 cm 3 g −1 . Especially, after incorporated with moderate amount of S (58.86 wt %), the CA/GNs0.1/S cathode exhibited the best electrochemical performances (initial discharging capacity of 1501 mAh g −1 at 0.1C and reversible capacities of 471 mAh g −1 after 100 cycles and 341 mAh g −1 after 500 cycles at 1C). This was attributed to the tunable hierarchical porous microstructure of the CA/GNs0.1 sample. Unfortunately, when increased the S content to 68.39 wt %, the electrochemical performance deteriorated in all aspects because of their sluggish reaction kinetics. These all results suggested that introducing GNs can feasibly enhance the performance of CA as matrix in Li-S batteries.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2019
·Vol. 21
·期 44
·24308-24315
·
IF 3.567
Leipeng Li,Xudong Qi,Feng Qin,Lu Li,Hong Gao,Yangdong Zheng,Zhiguo Zhang
A guideline for designing sensitive thermometry is proposed. It reveals that using two emission bands that possess the opposite change tendencies against temperature makes it easier to achieve a larger relative sensitivity. Based on the guidelines, a highly sensitive strategy for optical thermal detection that depends on the Tb3+-to-Eu3+ emission ratio is designed by exciting Eu3+/Tb3+'s unusual absorption lines. This can be easily driven by a commonly used and cheap 405 nm laser diode. Moreover, its maximum relative sensitivity reaches up to 2.02% K−1 at 610 K, one of the largest sensitivities reported so far.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Jiaona Shi,Qi Kang,Yan Mi,Qingquan Xiao
Lithium-sulfur (Li–S) batteries have attracted extensive attention in the past decades owing to their high theoretical energy density, low-cost and eco-friendliness. However, poorly cycling stability and rapidly decay caused by shuttle effects at high-sulfur loading condition restrain their practical applications. Focusing on these issues, N-doped hollow porous carbon nanotubes (N-HPCNT) as a self-supporting sulfur cathode is developed. The inherent conductivity and abundant pores of 3D continuous framework not only allow a high-sulfur content (67 wt%) and block the polysulfides via physical confinement, but also trap the polysulfides by the nitrogen heteroatoms (4.60 wt%) via strong chemisorption . Benefiting from the above-mentioned merits, the self-supporting S/N-HPCNT cathode with 3 mg cm −2 sulfur delivers high reversible capacity, super rate capability (1152 and 852.8 mAh g −1 at 0.2 and 3 C, respectively) and long cycling stability (717.9 mAh g −1 after 500 cycles at 1 C). Even under a higher sulfur loading (8 mg cm −2 ), it still exhibits a stable areal capacity of 7.72 mAh cm −2 (corresponding to 965.1 mAh g −1 ) after 60 cycles. This work provides a pathway for developing high performance Li–S batteries.
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POLYMER
·
2019
·
IF 3.771
Longfei Li,Hong Zhai,Tao Wang,Xibo Qiu,Na Qiang,Peng Dong,Ying Bai,Ai-Yun Peng,Daping Quan
The ring-opening copolymerization of lactide with carbonate is an available strategy to incorporate reactive groups to the pendent sites of copolymer for further functional modification. A series of random and block copolymers were synthesized from l -lactide ( L -LA) and 2-bromomethyl-2-methyltrimethylene carbonate (BMTC) using dodecanol as initiator and stannous octoate as catalyst. The structures of the copolymers were characterized by nuclear magnetic resonance ( 1 H NMR, 13 C NMR), gel permeation chromatography (GPC) and differential scanning calorimetry (DSC). The composition of the copolymers can be controlled through changing the feed ratios of n BMTC / n L -LA . It was found the random P(BMTC- co - L LA) copolymers had the semicrystalline characteristic due to the relative long block-like segments of P L LA ( L L , P L LA = 5.3–7.3) and the polar interactions from bromo groups , but their crystallinity ( X c, P L LA ) and melting temperature ( T m, P L LA ) decreased when the BMTC content increased. The X c, P L LA and T m, P L LA of P(BMTC- b -P L LA) block copolymers were relatively higher than the corresponding random copolymers, and approached gradually to the pure P L LA with the increase of the molecular weight of P L LA block. Finally, the pendent bromo groups of P(BMTC- co - L LA) were easily transformed into azides , which could proceed the azide-alkyne click reaction smoothly and quantitatively at room temperature .
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