Small
·
2023
·Vol. 19
·期 39
·2302530
·
IF 13.3
Xiaotong Li,Minkai Qin,Xiuju Wu,Xiangzhou Lv,Jianghao Wang,Yong Wang,Hao Bin Wu
Electrochemical CO 2 reduction reaction (CO 2 RR) is a promising strategy for waste CO 2 utilization and intermittent electricity storage. Herein, it is reported that bimetallic Cu/Pd catalysts with enhanced *CO affinity show a promoted CO 2 RR performance for multi-carbon (C2+) production under industry-relevant high current density. Especially, bimetallic Cu/Pd-1% catalyst shows an outstanding CO 2 -to-C2+ conversion with 66.2% in Faradaic efficiency (FE) and 463.2 mA cm −2 in partial current density. An increment in the FE ratios of C2+ products to CO for Cu/Pd-1% catalyst further illuminates a preferable C2+ production. In situ Raman spectra reveal that the atop-bounded CO is dominated by low-frequency band CO on Cu/Pd-1% that leads to C2+ products on bimetallic catalysts, in contrast to the majority of high-frequency band CO on Cu that favors the formation of CO. Density function theory calculation confirms that bimetallic Cu/Pd catalyst enhances the *CO adsorption and reduces the Gibbs free energy of the C C coupling process, thereby favoring the formation of C2+ products.
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RSC Advances
·
2023
·Vol. 13
·期 25
·17362-17369
·
IF 3.9
Zhe Zhang,Fanhao Kong,Bizhen Yuan,Yinnian Liao,Xiue Ren,Yu Hou
Solar-driven CO2 reduction into fuels and sustainable energy has attracted increasing attention around the world. However, the photoreduction efficiency remains low due to the low efficiency of separation of electron–hole pairs and high thermal stability of CO2. In this work, we prepared a CdO decorated CdS nanorod for visible light driven CO2 reduction. The introduction of CdO facilitates the photoinduced charge carrier separation and transfer and acts as an active site for adsorption and activation of CO2 molecules. Compared with pristine CdS, CdO/CdS exhibits a nearly 5-fold higher CO generation rate (1.26 mmol g−1 h−1). In situ FT-IR experiments indicated that CO2 reduction on CdO/CdS may follow a COOH* pathway. This study reports the pivotal effect of CdO on photogenerated carrier transfer in photocatalysis and on CO2 adsorption, which provides a facile way to enhance photocatalytic efficiency.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2021
·Vol. 139
·期 15
·51921
·
IF 3.125
Hongxu Meng,Zhisong Li,Linbo Wu,Bo-Geng Li,Yumiao Hu,Kecheng Wang
Poly(ethylene 2,5-furandicarboxylate) (PEF) is a biobased polyester with high gas barrier properties, tensile modulus, and strength. In PEF chain, in addition to ethylene furandicarboxylate repeat unit, there is also a small amount of diethylene glycol furandicarboxylate (DF) unit which is formed by etherification side reactions. However, the effect of DF unit in a wide composition range on polymer properties is still unclear. In this study, random poly(ethylene-co-diethylene glycol 2,5-furandicarboxylate) (PEDF) copolymers were synthesized via melt copolycondensation of 2,5-furandicarboxylic acid, ethylene glycol and diethylene glycol. The copolymers were characterized and evaluated by intrinsic viscosity, 1 H NMR, thermal transition, thermogravimetric analysis, tensile, impact, and O 2 penetration tests. The copolymers are amorphous in the full composition range. The presence of less than 58 mol% DF unit in PEDFs neither improves the tensile ductility nor deteriorates the oxygen barrier performance, but reduces the glass transition temperature clearly. In comparison with poly(ethylene terephthalate), the PEDF copolymers containing <58 mol% DF unit have higher tensile modulus, strength, and O 2 barrier properties.
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OPTICAL MATERIALS
·
2021
·
IF 3.08
Xing Zhang,Xinyou Huang,Ziyu Liu,Yagang Feng,Nan Jiang,Lexiang Wu,Zhaoxiang Yang,Tengfei Xie,Jiang Li
Ytterbium-doped yttrium oxide (5 at.%Yb:Y 2 O 3 ) nanopowders were synthesized by the co-precipitation method in this work. The influence of the molar ratio of ammonium hydrogen carbonate to metal ions (NH 4 HCO 3 /M 3+ , defined as R) on the properties of the precursors and powders was studied. The powders calcined at 1100 °C from the precursors with different R showed the same phase as the pure cubic Y 2 O 3 . However, the agglomerations of the calcined powders were influenced by the R evidently and the 5 at.%Yb:Y 2 O 3 powders with R = 4.0 showed better dispersivity. Using the obtained powders as starting materials, 5 at.%Yb:Y 2 O 3 transparent ceramics were fabricated by vacuum sintering and hot isostatic pressing (HIP) post-treating. The 5 at.%Yb:Y 2 O 3 ceramics with R = 4.0 possessed the best optical quality with the in-line transmittance of 81.2% at 1100 nm with fine grains. In addition, the microstructures of the 5 at.%Yb:Y 2 O 3 transparent ceramics with different R values were also studied and the HIP post-treated ceramics exhibited homogeneous microstructures. Meanwhile, the absorption and emission cross-sections of the 5 at.%Yb:Y 2 O 3 ceramics were calculated to be 0.99 × 10 −20 cm 2 at 976 nm and 0.97 × 10 −20 cm 2 at 1031 nm, respectively. The gain spectra also were obtained from the absorption and emission spectra.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Zhenhua Zhang,Liping Fan,Weiqi Liao,Feiyue Zhao,Cen Tang,Jing Zhang,Ming Feng,Ji-Qing Lu
Several CeO 2 -CuO/Cu 2 O nanocomposites with different CuO structures were used to identify the structure sensitivity of CuO in the CeO 2 -CuO/Cu 2 O catalyzed CO oxidation. The CO oxidation catalyzed by various CuO-CeO 2 interfacial sites involves a typical Mars-van Krevelen mechanism, in which the CuO-CeO 2 interfaces in the CeO 2 -CuO/c-Cu 2 O (cubes) nanocomposites are more intrinsically active, exhibiting ca. 15 kJ mol −1 lower activation energy than those in the CeO 2 -CuO/o-Cu 2 O (octahedra) and CeO 2 -CuO/d-Cu 2 O (rhombic dodecahedra) nanocomposites at CeO 2 loadings no less than 0.75 wt%. The higher activity is relevant to lower coordinated oxygen ions on CuO/c-Cu 2 O surface and thus better CO reactivity for the CeO 2 -CuO/c-Cu 2 O nanocomposites, which therefore indicates that the active oxygen species on CuO-CeO 2 interface should come from CuO rather than CeO 2 . Moreover, a highly active 13.2 %CeO 2 -CuO/c-Cu 2 O(s) catalyst for CO oxidation is realized on fine Cu 2 O cubes, which thus has high density of active sites.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2021
·
IF 5.268
Jingyi Liu,Zhoutong Dai,Yu Zhou,Wangwang Tao,Hongxiang Chen,Zuyi Zhao,Xinghua Liao
In order to obtain drug delivery carriers with good stability in blood and high cellular uptake efficiency, carboxyl groups and tertiary amine groups were respectively introduced into polyurethane to synthesize two kinds of amphiphilic polyurethanes with opposite charges (PUC and PUN). Their structures were characterized by Fourier transform infrared (FTIR) spectroscopy, nuclear magnetic resonance ( 1 H NMR) spectroscopy and gel permeation chromatography (GPC). PUC-PUN co-assembled nanomicelles were prepared by electrostatic interaction between PUC and PUN micelles , which showed acid-sensitive property. When the pH of the solution was decreased from 7.4 to 6.5, PUC-PUN-1 micelles showed negative-to-positive charge-reversal property among these micelles. The results of stability and cell experiments demonstrated that PUC-PUN-1 micelles not only had excellent stability in simulated normal physiological environment but also could obviously enhance the cellular uptake efficiency. PUC-PUN-1 micelles had low cytotoxicity against SGC-7901 and MGC-803 cells, whereas PUC-PUN-1/DOX micelles had higher cytotoxicity compared to pure DOX and PUN-1/DOX micelles. Moreover, the results of in vivo antitumor activity experiments showed that PUC-PUN-1/DOX micelles had better tumor inhibition ability and safety than pure DOX. In addition, the results of in vitro drug release experiments indicated that PUC-PUN-1/DOX micelles had almost no burst release or leakage of drugs in pH 7.4 environment. However, the drug release was accelerated in pH 5.0, which followed Fickian diffusion mechanism.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jiaxin Li,Yifei Liang,Zhao Li,Ke Fan,Chunxue Wang,Kai Li,Yuan Li,Xin Sun,Ping Ning,Fei Wang
The synthesis of methane from syngas represents a pivotal technology in the artificial synthesis of natural gas, with the study of methanation catalysts being a fundamental aspect of this process. Extensive research has focused on CO methanation using Ni/Al 2 O 3 catalysts; however, enhancements in catalyst stability and low-temperature activity are still required. This research investigated the structure of Ni/Al 2 O 3 under H 2 reduction at varying temperatures and the catalytic performance in natural gas synthesis (SNG) through CO methanation. It was observed that a higher reduction temperature resulted in nickel species agglomeration. Notably, Ni catalysts reduced at 600 °C demonstrated optimal CO conversion and CH 4 selectivity under the tested conditions. Characterization studies uncovered a synergistic effect between Ni and NiO species, which was most effective for catalytic activity under hydrogen reduction at 600 °C but only at an appropriate reduction temperature. These insights are significant for the advancement of Ni/Al 2 O 3 methanation catalysts in natural gas production .
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AICHE JOURNAL
·
2023
·
IF 3.7
Xin Zhao,Ruiqi Fang,Zirong Shen,Fengliang Wang,Yingwei Li
Transition-metal catalysts with metal nanoparticles (NPs) as active sites are widely utilized in various reactions. In this work, we report the atomic decoration of Pt upon Co NPs for enhanced catalytic performances in oxidation esterification. Systematical characterizations imply the single-atom nature and homogeneous distribution of Pt throughout the formed single-atom alloy (SAA). The synergistic interactions between Pt and Co lead to significant charge redistribution and up-shifted density of states (DOS) toward the Fermi level, which are verified favorable for the adsorption and activation of substrates. The esterification performances of Pt 1 Co@C are evaluated in the transformation of 54 kinds of aromatic alcohols (5-hydromethylfurfural, furfural, and benzyl alcohols) into the corresponding mono- and diesters. Pt 1 Co@C shows not only remarkably enhanced reactivity but also reliable durability in both batch and continuous flow reactors. Mechanism investigations clearly reveal the rapid transformation of 5-hydromethylfurfural over Pt 1 Co@C through a simplified route with reduced energy barriers.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Wang Zhongyan,Ren Chunhua,Shang Yuna,Yang Cuihong,Guo Qingxiang,Chu Liping,Liu Jianfeng
The utilization of nanotechnology to deliver vaccines and modulate immunity has shown great potential in cancer therapy. Peptide-based supramolecular hydrogels as novel vaccine adjuvants have been found to effectively improve the immune response and tumor curative effect. In this study, we designed a set of reduction-responsive self-assembled peptide precursors (Fbp-GDFDFDYD(E, S, or K)-ss-ERGD), which can be reduced by glutathione (GSH) into Fbp-GDFDFDYD(E, S or K)-SH for forming of hydrogel with different surface properties (E-gel, S-gel, and K-gel, respectively). Using the same method, co-assembled hydrogel vaccines (E-vac, S-vac, and K-vac, respectively) can also be prepared by mixing different precursors with antigens before GSH reduction. Through TEM observation of the nanostructure, we found that all the co-assembled hydrogels, especially K-vac, possessed much denser and more unified nanofiber networks as compared with antigen-free hydrogels, which were very suitable for antigen storage and vaccine delivery. Although the three peptides adopted similar β-sheet secondary structures, the mechanical properties of their resulted co-assembled hydrogel vaccines were obviously different. Compared to E-vac, S-vac had a much weaker mechanical property, while K-vac had a much higher. In vivo experiments, co-assembled hydrogel vaccines, especially K-vac, also promoted antibody production and anti-tumor immune responses more significantly than the other two vaccines. Our results demonstrated that co-assembled hydrogels formed by peptides and antigens co-assembly could act as effective vaccine delivery systems for boosting antibody production, and different immune effects can be acquired by tuning the surface properties of the involved self-assembling peptides.
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ACS Catalysis
·
2026
·
IF 13.6
Liu Meng-Nan,He Zhen-Hong,Chen Zhuo,Wang Sen-Wang,Ruan Miao,Luo Yanping,Wang Kuan,Wang Weitao,Wang Huan,Liu Zhao-Tie
Direct hydrogenation of CO 2 to liquid hydrocarbons (C 5+ ) at low temperature is a highly desirable but challenging transformation, as conventional catalysts typically operate at high temperatures via indirect pathways by producing and using a CO intermediate. In this work, we report an inverse ZrO 2 /Co catalyst that enables direct CO 2 hydrogenation to C 5+ hydrocarbons at a low temperature of 200 ° C. Under optimal conditions, the catalyst achieves a high CO 2 hydrogenation activity of 26.0 mmol CO2 ·g Co –1 ·h –1 with 58.9 C-mol % selectivity toward C 5+ liquid hydrocarbons and negligible CO formation. The inverse architecture of ZrO 2 /Co, wherein ZrO 2 nanoislands are dispersed over metallic Co 0 particles, concurrently not only enhances CO 2 adsorption and suppresses H 2 adsorption but also delivers a surface C/H ratio approximately 31 times higher than that of pristine Co 0 , thereby promoting chain growth. In situ DRIFTS reveals that the inverse catalyst generates abundant oxygen-containing intermediates (HCOO–, HCO 3 –, CH 3 O–, and CH 3 COO–), which are subsequently hydrogenated to CH x for chain growth over Co 0 sites. This work not only provides a low-temperature catalyst for direct CO 2 -to-C 5+ conversion but also establishes inverse oxide/metal interfaces as a general platform for tuning C–C bond coupling in CO 2 hydrogenation.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xiangqiong Wang,Quan Wang,Jie Li,Naixin Wang,Quan-Fu An
Pervaporation is an effective technique to improve the conversion of acetic acid in the esterification reaction through in situ removing the product water. In this study, a co-solvent assisted contra-diffusion strategy was used to prepare covalent organic framework (COF) pervaporation membrane on the polyacrylonitrile porous substrate. Fatty alcohol was used as the co-solvent in the organic phase to tune the reaction region. Subsequently, the COFs were formed in the sub-surface of the substrate to form a nanoconfined composite membrane , which was then modified by polyvinyl alcohol through spinning coating. The obtained COF composite membranes were used to in situ remove water during the esterification from acetic acid and ethanol. Consequently, compared with the esterification without pervaporation, the conversion of acetic acid was enhanced from 74% to 90%, which exhibited an excellent intensification for the esterification reaction.
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International Journal of Applied Ceramic Technology
·
2023
·
IF 2.1
Xiao-Chun Deng,Xiao-Dong Kang,Guo-Hua Zhang
(HfNbTaZrTiMo)C-Co high entropy carbide cermet was fabricated by conventional vacuum sintering. The effect of WC addition on the mechanical properties of cermets was also investigated. For cermets without WC addition, with the extension of sintering time, the hardness of cermets first rose and then fell, while the fracture toughness showed a decreasing trend. The increase in sintering temperature led to a decline in hardness and an enhancement of fracture toughness. The (HfNbTaZrTiMo)C-15 wt. % Co cermet sintered at 1450°C for 2 h had the best comprehensive properties, with the hardness and fracture toughness of 16.36 ± 0.17 GPa and 7.19 MPa·m 1/2 , respectively. After adding WC, there was a typical black core (undissolved (HfNbTaZrTiMo)C phase)-gray rim (seven-component (HfNbTaZrTiMoW)C solid solutions) structure in the cermets. Meanwhile, Mo diffused into WC to form (Mo, W)C solid solutions. The formations of (HfTaZrNbMoTiW)C and (Mo, W)C solid solutions resulted in an improvement in hardness. In addition, since the addition of WC enhanced the wettability between carbides phase and Co phase, the comprehensive properties of cermets were improved. The hardness and fracture toughness of the (HfNbTaZrTiMo)C-42.5 wt. % WC-15 wt.% Co cermet sintered at 1450°C for 2 h were 17.42 ± 0.06 GPa and 8.22 MPa·m 1/2 , respectively.
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