ChemistrySelect
·
2023
·Vol. 8
·期 29
·e202300512
·
IF 2.1
Kangjing Wang,Xinyi Dong,Ting Li,Qian Wang,Zhongyang Ding,Weifu Dong
Graphical The contact angle of modified starch was changed from 12.2° to 71.5°, and the particle size was changed from ∼10 μm to ∼300 nm. In the subsequent enzyme catalyzed reaction, the immobilized enzyme is adsorbed at the water oil interface, thereby improving the lipase activity. As a natural macromolecular material, starch is an ideal carrier for enzyme immobilization because of its widely available source, easy regeneration and excellent biodegradability. However, the natural starch cannot be directly used for immobilization due to the large particle size and excessive hydrophilicity. In this paper, the epoxy groups were grafted onto esterified starch by bifunctional reagents. The grafting efficiency of epoxy groups was increased by starvation drop addition. The changes of contact angle and particle size are conducive to the adsorption of immobilized enzyme at the water oil interface in the subsequent enzyme catalytic reaction, hence improve of the lipase activity. The maximum amount of lipase mobilized on such modified starch was ∼143.7 mg/g, which was near 40 mg/g higher than that of those from direct crosslinking. The immobilized enzymes showed excellent resistance to organic solvents and good reusability. Immobilization of lipases on epoxy-functionalized starch nanoparticles can potentially improves the possibility of enzymes industrial application.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Sizhao Zhang,Jing Wang,Zhao Wang,Guangyu Xu,Yonggang Jiang,Yunyun Xiao,Feng Ding
Reusable nanoporous polyimide (PI) aerogels are rather promising for highly efficient thermal insulation of future thermal protection systems demanded in aerospace and domestic applications. However, the development of high-performance PI aerogels is limited by their unsatisfactory high-temperature resistance and poor reusability. Herein, an Al2O3-hybridization strategy toward PI aerogels is demonstrated, and the formed aerogels exhibit a nanoporous structure, unusual reusability, and exceptional high-temperature resistance. Furthermore, the aerogels retain their high-level properties such as the very small changing rates of mass (≤0.3%), shrinkage (≤2.53%), thermal conductivity (≤3%), and bulk density (near-zero difference) even after five cycles of high-temperature assessment (250 °C for 2400 s). The conventional huge heat-induced shrinkage of PI aerogels could be substantially restrained even bearing a high-temperature environment, realizing near-zero thermally insulating degradation, which has an outstanding practical application value. The high-temperature resistance of the aerogel is greatly improved by the Al–O network constructed inside the PI aerogels, and this resistance is retained even after multiple cycles under harsh conditions, ultimately affording superior reusability to PI aerogels for the first time. The high-temperature resistance and ultralow heat-induced shrinkage properties of aerogels, as well as their reusability, make them favorable candidates as thermal protection materials for the future development of aircraft and military.
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Polymers
·
2023
·Vol. 15
·期 16
·3490
·
IF 5
Yujie Wang,Mengmeng Zhao,Yazhou Chen,Haifeng Bao,Chen Li
Dendrite growth and parasitic reactions with liquid electrolyte are the two key factors that restrict the practical application of the lithium metal anode. Herein, a bis(benzene sulfonyl)imide based single-ion polymer artificial layer for a lithium metal anode is successfully constructed, which is prepared via blending the as-prepared copolymer of lithiated 4, 4′-dicarboxyl bis(benzene sulfonyl)imide and 4,4′-diaminodiphenyl ether on the surface of lithium foil. This single-ion polymer artificial layer enables compact structure with unique continuous aggregated Li+clusters, thus reducing the direct contact between lithium metal and electrolyte simultaneously, ensuring Li+transport is fast and homogeneous. Based on which, the coulombic efficiency of the Li|Cu half-cell is effectively improved, and the cycle stability of the Li|Li symmetric cell can be prolonged from 160 h to 240 h. Surficial morphology and elemental valence analysis confirm that the bis(benzene sulfonyl)imide based single-ion polymer artificial layer effectively facilitates the Li+uniform deposition and suppresses parasitic reactions between lithium metal anode and liquid electrolyte in the LFP|Li full-cell. This strategy provides a new perspective to achieve a steady lithium metal anode, which can be a promising candidate in practical applications.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 36
·17072-17079
·
IF 3.3
Hongmei Xie,Guozhi Zhu,Dawei Ye,Weiquan Cai,Junjie Zhang,Kangping Huang,Yuliang Mai,Bing Liao,Jiazhi Chen
Catechyl lignin (C-lignin) is a unique and attractive natural biopolymer used as raw material for the production of chemicals and materials due to its homogeneous linear aromatic structure. Tung nutshells, an important component of industrial solid waste, are rich in C/G-type Lignin. Herein, for the first time, we report that the catalytic oxidation strategy is effective for the conversion of Tung nutshell lignin to value-added C/G-type aromatic monomers using the commercially available CuCl2 catalyst. The reaction conditions, including solvent, temperature, and catalyst dosage, were comprehensively investigated. The optimal yield of 60.8 mg g−1 (or 12.9 wt% Klason lignin) C/G-type aromatic aldehydes and acids was obtained using the CuCl2 catalyst in the CH3CN/H2O (8/2, v/v) solvent mixture at 190 °C for 4 h. The C-type aromatic monomers were formed with an yield of 7.7 mg g−1 (or 1.6 wt%) in the initial 0.2 h and gradually decreased as the reaction progressed. The less amount of C-type lignin-derived aromatic monomers can be attributed to their lower thermal stability under oxidative conditions. The structural evolution study of lignin by GPC and HSQC NMR reveals that the C/G units are effectively depolymerized and transformed into aromatic aldehydes and acids by the CuCl2/CH3CN/H2O catalytic oxidative system.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jingwei Li,Zhengyi Huang,Cong Wang,Lei Tian,Xiaoqing Yang,Rongfu Zhou,Mohamed Nawfal Ghazzal,Zhao-Qing Liu
Refining carrier transfer in bandgap-broken heterojunctions, which consist of two semiconductors with broken bandgaps, is crucial yet highly challenging for photocatalysis. Herein, we incorporated amorphous carbons (AC) into the bandgap-broken V 2 O 5 /GdCrO 3 heterojunctions, inducing a linkage effect to facilitate photoexcited carrier transfer. The created V-O-C and Cr-O-C bonds in V 2 O 5 -AC-GdCrO 3 interfaces show almost identical orbital energies to overcome the broken-gap energy barriers at interfaces. The holes at GdCrO 3 ’s valence band and electrons at V 2 O 5 ’s conduction band tent to migrating toward the carbon ring of amorphous carbon via Cr-O-C and V-O-C bonds, thereby enhancing carrier separation of bandgap-broken V 2 O 5 /AC/GdCrO 3 heterojunction. By controlling the relative amount of metal-O-C bonds in the interface, the modulation of charge transfer kinetics was also achieved on V 2 O 5 /AC/GdCrO 3 , resulting in ∼7 times higher of H 2 generation than V 2 O 5 /GdCrO 3 . The concept could be expanded to the other carbon allotropes, including graphene, carbon nanotube, and graphdiyne conjugated structures, demonstrating a universal strategy in reaching optimal charge transfer of broken-bandgap heterojunctions for photocatalytic H 2 production.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Zicheng Fan,Insub Noh,Changlong Zhuang,Qingqing Liu,Yanbin Wang,Hyung Do Kim,Meng Yue,Hideo Ohkita,Biaobing Wang
With the rapid development and application of 5G technology, design and fabrication of lightweight polymer materials with excellent flame retardancy, low dielectric constant, and high thermal insulation is a worthy but great challenge. In this study, a polar polyimide (PI) contain amide group was designed and incorporated into epoxy resin (EP) to fabricate multifunctional materials combing a small molecule named phenoxycycloposphazene (HPCTP). Due to the synergistic effect of PI and HPCTP in flame retardant, EP blend passed UL-94 V-0 rating only needing 3 wt% PI and 1 wt% HPCTP, meanwhile the limited oxygen index (LOI) obviously increased from 23.8% to 35.0%. More importantly, the dielectric constant obviously decreased at a wide range from 10 −1 to 10 7 Hz and the thermal conductivity also reduced by more than 45% from 0.236 to 0.127 W m −1 K −1 . Due to the good compatibility and reactivity between PI and EP, PI was uniformly dispersed and connected EP to construct intimate 3D interpenetrating polymer network, and thus the tensile and flexural properties were slightly enhanced. Moreover, combustion parameters, including peak heat release rate (PHRR), total heat release (THR), smoke produce rate (SPR) and total smoke production (TSP), all indicated that EP composites significantly reduced fire risk. Overall, this study offers a promising strategy to fabricate flame retardant EP composites with outstanding comprehensive performances.
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Environmental Technology & Innovation
·
2023
·
IF 7.1
Yi-na Tu,Die Zhou,Huaying Liu,Wei Tang,Weilin Wu,Yingjie Li
The dissolved black carbon (DBC) derived from co-pyrolysis of plastic and biomass be released into aquatic environment. DBC was an important photoactive constituent, however, the photochemical activity of DBC from the co-pyrolysis plastic and biomass remains unclear. Herein three popular plastic wastes (polystyrene, PS; polylactic acid, PLA; plastic mulch film, PMF) and pine needle biomass prepared co-pyrolysis biochar, and effects of co-pyrolysis plastics on DBC’s photogeneration ability of reactive intermediates, affecting pollutant photodegradation, were investigated. In comparison to individual DBC, the mixed DBC from co-pyrolysis biochar had a lower molecular weight and more oxygen-containing groups. Quantum yields of singlet oxygen ( 1 O 2 ) and triplet state DBC ( 3 DBC*) from mixed DBC were higher, especially PMF-DBC since its lower aromaticity and molecular weight connected with its higher E 2 / E 3 and lower SUVA 254 values. Steady-state photochemical experiment demonstrated 3 DBC* formation rates for mixed DBC were lower than individual DBC, while the second-order reaction rate constants of 3 DBC* with 2,4,6-trimethylphenol for mixed DBC were higher than that of individual DBC. Quenching experiment by sorbic acid to distinguish high/low-energy triplets revealed that contributions of low-energy triplets to 3 DBC* and 1 O 2 generation decreased relative to individual DBC, indicating the transformation of reductive groups to oxidative groups, which was supported by the phototransformation kinetics. Quantum yields of 3 DBC* and 1 O 2 were positively linear correlations with E 2 / E 3 using twenty DBC samples. These findings are helpful in understanding DBC’s photochemical activity from co-pyrolysis of plastics and biomass, especially in aquatic environments adjacent to soil amended by biochar.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weilong Hou,Kehang Lin,Xiangyu Zhang,Bowen Xu,Yuexia Wang,Xinqing Lu,Yijing Gao,Rui Ma,Yanghe Fu,Weidong Zhu
Nonoxidative propane dehydrogenation (PDH) has been regarded as an economic and efficient route to meet constantly increasing global demands for propylene. However, over industrially applied catalysts, thermally induced deactivation including coke formation and sintering of the active species occurs and simultaneously hydrocarbon cracking significantly reduces the selectivity for propylene. In the present work, titanosilicate-1 (TS-1) zeolite supported catalysts (Pt/TS-1) were developed for PDH. The results on the extensive characterizations of the prepared materials, in combination with density functional theory (DFT) calculations, verify that the framework Ti species in Pt/TS-1 can increase the dispersion and electron density of Pt, which significantly enhances the catalyst stability and selectivity for propylene. Utmost importantly, no sintering of the Pt active species in Pt/TS-1 occurs at the high temperatures required for the reaction and catalyst regeneration processes. Therefore, the current investigation provides a strategy for developing efficient PDH catalysts for practical applications.
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CARBON
·
2023
·
IF 10.9
Yang Zhao,Biao Ma,Xiaomei Liu,Ning Li,Yang Li,Xiaobin Fan,Wenchao Peng
Recently, single atomic metals supported on carbon materials have attracted great interests because of their high catalytic activity and stability in peroxymonosulfate (PMS)-based Fenton-like process. Herein, we propose a convenient strategy to synthesize Co single atoms supported on nitrogen-doped carbon spheres (Co@MNC) via microwave treatment. The microwave irradiation can simultaneously induce the formation of carbon defects and immobilize the Co single atoms in N doped carbon support in a few minutes. The obtained Co@MNC can activate PMS for efficient catalytic oxidation of organic pollutants. The radical quenching tests and electron paramagnetic resonance (EPR) verify that Co (IV)-oxo species, 1 O 2 , and O 2 •− are responsible for the remediation of organic pollutants. Density functional theory (DFT) calculations confirm that unique and low coordinated Co–N 2 on void or edge defects are favorable for PMS adsorption. The electrons will then transfer from Co atoms to adsorbed PMS via the bonded N. Co (IV)-oxo species and other ROSs are therefore generated for pollutants degradation. This work provides a fast method for the synthesis of single atom catalysts for efficient Fenton-like reactions.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Guiquan Liu,Guorong Wang,Zhiliang Jin
Porous carbon is an ingredient for energy transformation and collection systems in terms of electrochemistry. As a new member, graphdiyne (GDY) gradually began to be concerned because of its especially compositional and structural properties. Herein, a lamelliform GDY was successfully prepared by cross-coupling strategy under the catalysis of cuprous iodide. Thanks to the sp and sp 2 hybrid carbon networks, the obtained GDY nano-lamellas promote excellent performance in the electrode of supercapacitors with a gravimetric capacitance of 137.8 F g − 1 at a mass-specific current of 1 A g − 1 , and a relatively good rate performance of 81.28% when the mass-specific current reach to 20 A g − 1 . In addition, the capacitance of the GDY electrode barely decays during the 11,000 cycles of repeated testing. This enables the assembled symmetric supercapacitor provides a acceptable energy density of 6.11Wh kg −1 under a power density of 5500W kg −1 , and with an average decay of 0.5% per cycle at the end of 5000 cycles. The relatively good electrochemical stability of this GDY nano-lamellas material will open the further promotion of graphdiyne-based electrodes in the domain of supercapacitors.
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Communications Biology
·
2023
·Vol. 6
·期 1
·1-12
·
IF 5.9
Wang You-Yuan,Zhen Cheng,Hu Wei,Huang Hui-Huang,Li Yan-Jun,Zhou Ming-Ju,Li Jing,Fu Yu-Long,Zhang Peng,Li Xiao-Yu,Yang Tao,Song Jin-Wen,Fan Xing,Zou Jun,Meng Si-Run,Qin Ya-Qin,Jiao Yan-Mei,Xu Ruonan,Zhang Ji-Yuan,Zhou Chun-Bao,Yuan Jin-Hong,Huang Lei,Shi Ming,Cheng Liang,Wang Fu-Sheng,Zhang Chao
CD8 + T cells are essential for long-lasting HIV-1 control and have been harnessed to develop therapeutic and preventive approaches for people living with HIV-1 (PLWH). HIV-1 infection induces marked metabolic alterations. However, it is unclear whether these changes affect the anti-HIV function of CD8 + T cells. Here, we show that PLWH exhibit higher levels of plasma glutamate than healthy controls. In PLWH, glutamate levels positively correlate with HIV-1 reservoir and negatively correlate with the anti-HIV function of CD8 + T cells. Single-cell metabolic modeling reveals glutamate metabolism is surprisingly robust in virtual memory CD8 + T cells (TVM). We further confirmed that glutamate inhibits TVM cells function via the mTORC1 pathway in vitro. Our findings reveal an association between metabolic plasticity and CD8 + T cell-mediated HIV control, suggesting that glutamate metabolism can be exploited as a therapeutic target for the reversion of anti-HIV CD8 + T cell function in PLWH.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Rui Du,Bin Zhao,Kun Luo,Man-Xi Wang,Quan Yuan,Lei-Xiao Yu,Ke-Ke Yang,Yu-Zhong Wang
Bone tissue engineering involving scaffolds is recognized as the ideal approach for bone defect repair. However, scaffold materials exhibit several limitations, such as low bioactivity, less osseointegration, and poor processability, for developing bone tissue engineering. Herein, a bioactive and shape memory bone scaffold was fabricated using the biodegradable polyester copolymer’s four-dimensional fused deposition modeling. The poly(ε-caprolactone) segment with a transition temperature near body temperature was selected as the molecular switch to realize the shape memory effect. Another copolymer segment, i.e., poly(propylene fumarate), was introduced for post-cross-linking and improving the regulation effect of the resulting bioadaptable scaffold on osteogenesis. To mimic the porous structures and mechanical properties of the native spongy bone, the pore size of the printed scaffold was set as ∼300 μm, and a comparable compression modulus was achieved after photo-cross-linking. Compared with the pristine poly(ε-caprolactone), the scaffold made from fumarate-functionalized copolymer considerably enhanced the adhesion and osteogenic differentiation of MC3T3-E1 cells in vitro. In vivo experiments indicated that the bioactive shape memory scaffold could quickly adapt to the defect geometry during implantation via shape change, and bone regeneration at the defect site was remarkably promoted, providing a promising strategy to treat bone defects in the clinic, substantial bone defects with irregular geometry.
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