JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 3
·964-977
·
IF 3.5
Zhu Q.,Wei S.,Wang C.,Yang X. B.,Zhou B.,Xie Z. X.,Duan Z. Q.,Hu Y. M.
Unique wool-ball shaped nanocrystalline CoS was synthesized using solvothermal method in which dopamine (DA) was added as carbon source to combine with the CoS. The DA in situ polymerized and coated on the CoS particle surfaces during the solvothermal process. N, S co-doped carbon-encapsulated CoS(Co 9 S 8 ) were achieved after a post carbonization. In the composites, CoS(Co 9 S 8 ) nanocrystals and carbon are tightly bound and embedded into the amorphous carbon layer to form a spherical core–shell structure. Hybrid counter electrodes (CEs) fabricated with the product have good conductivity, dispersion and stability due to the synergetic effect between carbon and nanocrystalline CoS(Co 9 S 8 ). Charge transfer through the CE/electrolyte interfaces is improved by dopamine-carbon combination. In the optimal case, PCE of 8.82% of the dye-sensitized solar cells (DSSCs) with the hybrid CEs was achieved, which is close to that of the cell with Pt (8.86%) CE, and is a 41.12% increase compared with that of CoS CE cell with the structure of photoanode/N719/electrolyte (I − /I 3 − )/CE. Moreover, stability of the cells with the composite CEs was greatly improved. The results demonstrate that the as-prepared composites are promising alternatives to Pt-CEs for high-performance DSSCs. The reported preparation method will guide further developments in highly efficient carbon-based catalysts for electrochemistry and energy related applications.
研究领域:
材料科学
·
能源技术
·
电化学
·
纳米技术
·
太阳能电池
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Zichun Xiao,Ya-Nan Zhou,Xiaowei Wang,Jiawu Cui,Mingyu Yang,Chengyong Shu,Duzhao Han,Jiangqi Zhou,Chengxin Peng,Wei Tang,Yuping Wu
Lithium metal is considered as the ultimate anode for next-generation high energy-density batteries. However, its practical application is still severely hindered by Li dendrite growth as well as infinite volume variation along plating and stripping. Herein, we report a dual-layered, spatially ordered composite skeleton for bottom-up lithium growth by uniformly incorporating Li6.06La3Zr2Al0.2O12 (LLZO) in the upper layer and ZnO in the bottom layer, respectively, in the matrix of carbon fibers (CFs). The well-dispersed ZnO nanoparticles on CFs in the bottom layer function as lithiophilic nucleation sites to homogenize Li nucleation, while LLZO nanoparticles on CFs in the upper layer facilitate Li ion diffusion and distribution for stable lithium growth owing to the high ion conductivity of LLZO. Benefiting from this synergetic effect, the CFs@LLZO//CFs@ZnO composite skeleton can effectively induce Li plating/stripping in a controllable spatially ordered manner, suppressing the volume variation and inhibiting the formation of dendritic lithium. As a result, the symmetric cell using Li|CFs@LLZO//CFs@ZnO||CFs@LLZO//CFs@ZnO|Li presents good cycling stability over 2500 h with a small overpotential of 12 mV at 1 mA cm–2. Notably, under a harsh negative-to-positive N/P ratio of 1, the Li|CFs@LLZO//CFs@ZnO||NCM811 full cell delivers a lifespan of 100 cycles with a capacity fading of only 0.175% per cycle and an average CE of 99.3%.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Cui Wang,Qiangqiang Yang,Zhenhong Li,Kun-Yi Andrew Lin,Shaoping Tong
A magnetic carbon-coated Fe-C/N composite was synthesized by a simple impregnation method and its performance in activating persulfate (PS) to degrade Acid Red 73 (AR 73) was investigated. The as-prepared carbon-coated Fe-C/N hybrid material was characterized via transmission electron microscopy , Raman spectra, X-ray diffraction and X-ray photoelectron spectrum. Degradation experiments showed that 98.11% of AR 73 could be degraded in 10 min, but its COD was partly removed. The effects of initial reaction pH and temperature were also evaluated. An increase of temperature was beneficial for the removal of AR 73, while the increase of pH had an opposite result. The activation energy of the AR 73 degradation was determined to be 46.12 KJ/mol, smaller than those in relative literatures. The recycling test showed that the carbon-coated Fe-C/N composite had good stability. The mechanism study indicated that the catalytic performance of Fe-C/N was due to the synergistic effect between Fe 3 C and Fe 3 N, and the N doped carbon shell suppressed the rate of Fe leaching, thus enhancing its stability.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 2
·286-301
·
IF 5.365
Mengyuan Zhang,Shipeng Wu,Longchun Bian,Qiue Cao,Wenhao Fang
Ce–Ni mixed oxides with different Ni/Ce molar ratios, promoted by a rather low amount of Pd (0.2 wt%), were prepared by a simple one-pot precipitation method. The thus-synthesized CeNiXOY and Pd–CeNiXOY catalysts were applied respectively to the direct N-alkylation of amine and alcohol via oxidative coupling, under O2 in the absence of basic additives. The CeNiXOY catalyst could provide a >99% yield of imine in the model alkylation reaction of aniline with benzyl alcohol at 100 °C. The Pd-promoted Pd–CeNiXOY catalyst surprisingly showed an enhanced imine yield (>99%) at a mild temperature of 60 °C. This catalyst exhibited good reusability, and moreover, demonstrated high performance towards imine synthesis from various amines with alcohols. The presence of Pd species and the Ni/Ce molar ratio showed a synergistic impact on the conversion of aniline, as well as on the product selectivity, which was believed to be related to the improvement on the intrinsic activity of the oxidation of benzyl alcohol to benzaldehyde. Various physicochemical techniques, including ICP-MS, XRD, N2 adsorption–desorption, UV-Raman, H2-TPR, TEM, EPMA and XPS, were employed to study mainly the composition, structure and redox properties of the catalysts. The proportion of Ce3+ species and oxygen vacancies, which can be manipulated by the Ce–Ni redox system and the interaction between Ce and Ni, was crucial to the selective activation of alcohols in the presence of reactive amines. The activation of alcohol on the highly reactive Pd0 species was the other crucial factor.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Cheng Yang,Chengyong Shu,Zhuofan Gan,Chen Lai,Jijun Ma,Wei Tang,Yuping Wu
ZIF-8-derived Fe–N–S triple doping hollow-shell nanoparticles are prepared by the surface modification of SCN– ligands. Fe3+ ions are highly adsorbed on the SCN–-modified layer, forming a hollow-shell rhombic dodecahedron particle after pyrolysis. Doping extra S atom is found to be an effective method to increase the density of atomically dispersed active sites and boost their catalytic performance. The H-ZIF-Fe-SCN catalyst shows good bifunctional stability toward the oxygen reduction reaction and the oxygen evolution reaction in alkaline solution, the half-wave potential for the H-ZIF-Fe-SCN catalyst was recorded to be 0.889 V vs reverse hydrogen electrode, and a maximum power performance of 158.8 mW cm–2 was achieved when it was used as a cathode catalyst in zinc–air batteries.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2013
·
IF 4.187
Xiu-Juan Shi,Gao-Jian Chen,Yan-Wei Wang,Lin Yuan,Qiang Zhang,David M. Haddleton,Hong Chen
Surface-initiated SET-LRP was used to synthesize polymer brush containing N-isopropylacrylamide and adamantyl acrylate using Cu(I)Cl/Me6-TREN as precursor catalyst and isopropanol/H2O as solvent. Different reaction conditions were explored to investigate the influence of different parameters (reaction time, catalyst concentration, monomer concentration) on the polymerization. Copolymers with variable 1-adamantan-1-ylmethyl acrylate (Ada) content and comparable thickness were synthesized onto silicon surfaces. Furthermore, the hydrophilic and bioactive molecule β-cyclodextrin-(mannose)7 (CDm) was synthesized and complexed with adamantane via host–guest interaction. The effect of adamantane alone and the effect of CDm together with adamantane on the wettability and thermoresponsive property of surface were investigated in detail. Experimental and molecular structure analysis showed that Ada at certain content together with CDm has the greatest impact on surface wettability. When Ada content was high (20%), copolymer–CDm surfaces showed almost no CDm complexed with Ada as the result of steric hindrance.
研究领域:
材料科学
·
生物医学工程
·
高分子化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Caiyan Gao,Xuezhen Feng,Lian Yi,Xiaoyong Wu,Renji Zheng,Gaoke Zhang,Yubiao Li
Formaldehyde (FA), as an important chemical raw material, has been widely used in many fields. However, the discharge of a large amount of FA-containing wastewater poses a serious threat to the environment and human health. Recently, the in-situ hydrogen energy release technology of hydrogen-containing stable liquid has been extensively explored due to its safe storage. Exploring a robust method to achieve FA removal and synchronous in-situ hydrogen release from FA containing wastewater is of great significant for environmental protection and energy crisis alleviation. Here, we have innovatively introduced peroxymonosulfate (PMS) activation technology into FA removal and hydrogen production simultaneously. The composite of nitrogen doped carbon coating Co 9 S 8 nanotubes (Co 9 S 8 @N−C) is employed as a proof of concept for FA decomposition and simultaneously hydrogen production based on PMS activation system. As expected, the Co 9 S 8 @N−C/PMS system presents much superior hydrogen production efficiency and satisfactory FA removal rate towards FA wastewater than those of common catalysis, photocatalysis and Fenton reaction in the basic condition in a wide range of FA concentration. The hydrogen yield reaches a value as high as 471 μmol within 60 min, corresponding to a FA degradation rate of 30% with an initial FA concentration of 0.722 mol L −1 . Characterizations and density functional theory (DFT) calculations suggest that the free radical process dominated by superoxide radical (O 2 ⋅ − ) and nonradical process dominated by singlet oxygen ( 1 O 2 ), which are induced by Co 9 S 8 @N−C/PMS system, are responsible for highly efficient hydrogen production via FA degradation. These generated O 2 ⋅ − and 1 O 2 can extract ⋅ H from FA to form ⋅ OOH intermediate, which can further combine with the ⋅ H from water to produce hydrogen. This study provides an applicable technique for environmental purification and new energy development based on FA containing wastewater.
研究领域:
环境科学
·
化学工程
·
能源技术
·
水处理
✓ 已验证
DOI
高影响因子
Polymer Chemistry
·
2013
·Vol. 5
·期 3
·761-770
·
IF 5.231
Wenlong Li,Peiyi Wu
The influence of different Ionic Liquids (ILs) on the phase transition behavior of poly(N-vinylcaprolactam) (PVCL) solution is investigated by differential scanning calorimetry (DSC) and turbidity measurements, in combination with FT-IR spectroscopy. The DSC and turbidity results reveal that hydrophilic ILs at a concentration of 0.25 mol L−1 only slightly change the transition temperature. The LCST experiences an increase while the phase separation behavior disappears gradually as the concentration of 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]) increases from 0 to 1.0 mol L−1. In contrast, the addition of hydrophobic ILs, especially 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([EMIM][NTf2]), even at a low concentration, greatly raises the LCST, indicating the possibility of hydrogen bonding between [EMIM][NTf2] and PVCL. Finally, temperature-dependent FTIR spectra are employed to elucidate the dynamic mechanism of the different influences on the phase transition of PVCL. The hydrophilic ILs can change the state of the PVCL chains indirectly by varying their interaction with water molecules. For comparison, the formation of hydrogen bonds between the unsaturated C–H of [EMIM][NTf2] and the CO of PVCL results in a higher temperature and more energy to complete the phase transition. However, with the continual increasing of the concentration, extra [EMIM][NTf2] can not be well dispersed in water due to its hydrophobicity, so the LCST undergoes a decrease and finally reaches an equilibrium. Additionally, hydrophilic ILs tend to distribute in the solution, while hydrophobic ILs, especially [EMIM][NTf2], are prone to be wrapped in polymer chains of the aggregates after phase separation. Furthermore, both types of IL experience the process of hydrogen bond disruption and chain aggregation.
研究领域:
高分子化学
·
物理化学
·
热力学
·
药物递送系统
·
刺激响应材料
✓ 已验证
DOI
高影响因子
PROGRESS IN ORGANIC COATINGS
·
2023
·
IF 6.6
Ao Zhou,Hao Yu,Jun Tang,Biao Zhang,Fugang Qi,Yun Zhou,Nie Zhao,Xiaoping Ouyang
With the rapid development of the modern industrial marine economy, metal corrosion and biological fouling of marine ships and engineering equipment have become the main problems affecting the development of the marine industry. Traditional single-function coatings have only anti-corrosion or anti-fouling properties, which cannot meet the current needs of marine industry development for coating protection. In this study, a self-healing coating with good anticorrosion and antifouling properties has been prepared upon functionalization of a film forming resin and modification of a nanofiller. Initially, a modified acrylic resin (PAZ/N-PMI) was successfully synthesized by inserting zinc ions and a structural functional monomer ( N -phenyl maleimide; N-PMI) into the polymer chain of an acrylic resin using free radical solution polymerization . A fluorinated silica coated hydroxylated multi-walled carbon nanotubes nanocomposite (F-MWCNTs-OH@SiO 2 ) was dispersed in PAZ/N-PMI resin to prepare the composite coating samples. The composite coating showed good performance, in which the antibacterial rate of the composite coating against Staphylococcus aureus and Escherichia coli was >99.98 %. When F-MWCNTs-OH@SiO 2 was 3 wt%, the Z f=0.01Hz of the composite coating reached the highest value, which was 3 orders of magnitude higher than that of the PAZ/N-PMI coating. At the same time, the prepared composite coating also exhibited good self-healing properties. This study provides a broad application prospect for the development of high quality marine anti-corrosion and anti-fouling organic coatings .
研究领域:
材料科学
·
海洋工程
·
防腐与防污技术
✓ 已验证
DOI
高影响因子
Science China-Chemistry
·
2022
·Vol. 66
·期 2
·548-561
·
IF 10.138
Zhao Ying-Han,Li Wenhao,Shen Tao,Zhao Yan,Liu Yunqi,Wang Yang
The development of readily accessible high-mobility n-type semiconducting polymers is in great demand for realizing high-performance p-n junction-based organic electronics. In this study, we demonstrate that with the combination of dual-acceptor strategy and C-H direct arylation polymerization (DArP), unipolar n-type semiconducting polymers can be conveniently synthesized. By tuning the monomer concentration, three dual-acceptor polymers, namely, poly(naphthalene diimide- alt -dithiophenyl pyrrolopyrrole-dione) (PNDI-DPP), poly(naphthalene diimide- alt -dithiophenyl isoindigo) (PNDI-IID), and poly (naphthalene diimide- alt -dithiophenyl bezothiadiazole) (PNDI-BT) can be obtained via C-H activation with decent number average molecular weight of ∼10 to 30 kg mol −1 and relatively narrow polydispersity index of ∼2. In addition, these polymers are defect-free in nature as evidenced by the nuclear magnetic resonance. Moreover, we attribute the different molar masses of the three copolymers under the same DArP condition to the different α-C-H acidity, which may stem from different electron-withdrawing capability of the hydrogenated acceptor units. Furthermore, the influence of the hydrogenated acceptor monomers on the optical, electrochemical and charge transporting properties is comprehensively studied. Among the three dual-acceptor polymers, PNDI-BT demonstrates the highest electron mobilities of up to 0.6 cm 2 V −1 s −1 in unipolar n-type organic transistors because of its relatively planar backbone, larger overlaps of the lowest unoccupied molecular orbital and strong H-aggregation. Note that the transistor performance of PNDI-BT synthesized via C-H activation in this study is at least comparable to the one made by conventional C(sp 2 )-C(sp 2 ) Stille or Suzuki cross-coupling polymerization. This study demonstrates the presented protocol can be a useful platform for sustainable and convenient synthesis of high-performance n-type semiconducting polymers.
研究领域:
材料科学
·
有机电子学
✓ 已验证
DOI
高影响因子
Journal of Animal Science and Biotechnology
·
2021
·Vol. 12
·期 1
·1-12
·
IF 5.032
Li Zongjun,Lei Xinjian,Chen Xiaoxu,Yin Qingyan,Shen Jing,Yao Junhu
Background In recent years, nitrooxy compounds have been identified as promising inhibitors of methanogenesis in ruminants. However, when animals receive a nitrooxy compound, a high portion of the spared hydrogen is eructated as gas, which partly offsets the energy savings of CH 4 mitigation. The objective of the present study was to evaluate the long-term and combined effects of supplementation with N-[2-(nitrooxy)ethyl]-3-pyridinecarboxamide (NPD), a methanogenesis inhibitor, and fumaric acid (FUM), a hydrogen sink, on enteric CH 4 production, rumen fermentation, bacterial populations, apparent nutrient digestibility, and lactation performance of dairy goats. Results Twenty-four primiparous dairy goats were used in a randomized complete block design with a 2 × 2 factorial arrangement of treatments: supplementation without or with FUM (32 g/d) or NPD (0.5 g/d). All samples were collected every 3 weeks during a 12-week feeding experiment. Both FUM and NPD supplementation persistently inhibited CH 4 yield (L/kg DMI, by 18.8% and 18.1%, respectively) without negative influence on DMI or apparent nutrient digestibility. When supplemented in combination, no additive CH 4 suppression was observed. FUM showed greater responses in increasing the molar proportion of propionate when supplemented with NPD than supplemented alone (by 10.2% vs. 4.4%). The rumen microbiota structure in the animals receiving FUM was different from that of the other animals, particularly changed the structure of phylum Firmicutes. Daily milk production and serum total antioxidant capacity were improved by NPD, but the contents of milk fat and protein were decreased, probably due to the bioactivity of absorbed NPD on body metabolism. Conclusions Supplementing NPD and FUM in combination is a promising way to persistently inhibit CH 4 emissions with a higher rumen propionate proportion. However, the side effects of this nitrooxy compound on animals and its residues in animal products need further evaluation before it can be used as an animal feed additive.
研究领域:
动物营养学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Yong Wang,Ziyuan Wang,Huifen Yu,Haidong Teng,Jianping Wu,Jiaqi Xu,Lirong Yang
Lipase from Rhizopus oryzae (ROL) exhibits remarkable sn-1,3 stereoselectivity and catalytic activity, but its poor thermostability limits its applications in the production of 1,3-dioleoyl-2-palmitoyl glycerol (OPO, a high-quality substitute for human milk fat). In this work, a semirational method was proposed to engineer the thermostability and catalytic activity of 4M (ROL mutant in our previous study). First, a computer-aided design is performed using 4M as a template, and N-glycosylation mutants are then recombinantly expressed and screened in Pichia pastoris, the optimal mutant N227 exhibited a half-life of 298.8 h at 45 °C, which is 7.23-folds longer than that of 4M. Its catalytic activity also reached 1043.80 ± 61.98 U/mg, representing a 29.2% increase compared to 4M (808.02 ± 47.02 U/mg). Molecular dynamics simulations of N227 suggested that the introduction of glycan enhanced the protein rigidity, while the strong hydrogen bonds formed between the glycan and the protein stabilized the lipase structure, thereby improving its thermostability. The acidolysis reaction between oleic acid (OA) and glycerol tripalmitate (PPP) was successfully carried out using immobilized N227, achieving a molar conversion rate of 90.2% for PPP. This engineering strategy guides the modification of lipases, while the glycomutants obtained in this study have potential applications in the biosynthesis of OPO.
研究领域:
生物技术
·
酶学
·
蛋白质工程
·
生物化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）