TETRAHEDRON
·
2021
·
IF 2.457
Yang-Ping Deng,Qin-Hua Gan,Xu Gao,Xiao-Qiang Jiang,Shi-Fan Wang
A new method for one-step synthesis of oxazolo[3,2- c ] pyrimidine core and its derivatives has been developed in inexpensive and green bio-based solvent lactic acid without any additional catalysts and additives. Density functional theory calculations located the reaction pathway and identified the intermolecular nucleophilic addition step to be the rate-limiting step. By this method, twenty new oxazolo[3,2- c ] pyrimidine derivatives were synthesized in high yield and characterized by spectroscopic analysis and X-ray diffraction.
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DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Ziyi Guo,Yuan Zhang,Dong Wang
A non-radical catalytic ozonation process functionalized by Mn(II)-sites was found effective to degrade oxalic acid as a typical refractory compound that is hard to remove through catalytic ozonation with hydroxyl radical oxidation. Specifically, we prepared functional Mn–C@Fe nanoparticles with carbon shell supporting Mn 3 O 4 for catalysis while encapsulating magnetic iron core for recycle. Batch study shows its excellent catalytic reactivity on the degradation of organics particular for the ozone-recalcitrant oxalic acid (20 min for 90.9% removal, kinetics constant of 0.045 min −1 ). Our mechanism study ruled out the hydroxyl radical oxidation, and highlighted the formation of a heptavalent Mn intermediate oxidant responsible for the fast degradation that was initiated via ozone activation of Mn(II)-sites on the carbon shell. Our findings underscore a non-radical catalytic ozonation as a promising alternative technology for the abatement of aqueous organic pollutants.
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DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 12
·1986-2000
·
IF 4.5
Xue Yi-Fan,Feng Jie,Song Yun-Cai,Li Wen-Ying
Breakage of the C–N bond is a structure sensitive process, and the catalyst size significantly affects its activity. On the active metal nanoparticle scale, the role of catalyst size in C–N bond cleavage has not been clearly elucidated. So, Ru catalysts with variable nanoparticle sizes were obtained by modulating the reduction temperature, and the catalytic activity was evaluated using 1,2,3,4-tetrahydroquinoline and o -propylaniline with different C–N bond hybridization patterns as reactants. Results showed a 13 times higher reaction rate for sp 3 -hybridized C–N bond cleavage than sp 2 -hybridized C–N bond cleavage, while the reaction rate tended to increase first and then decrease as the catalyst nanoparticle size increased. Different concentrations of terrace, step, and corner sites were found in different sizes of Ru nanoparticles. The relationship between catalytic site variation and C–N bond cleavage activity was further investigated by calculating the turnover frequency values for each site. This analysis indicates that the variation of different sites on the catalyst is the intrinsic factor of the size dependence of C–N bond cleavage activity, and the step atoms are the active sites for the C–N bond cleavage. When Ru nanoparticles are smaller than 1.9 nm, they have a strong adsorption effect on the reactants, which will affect the catalytic performance of the Ru catalyst. Furthermore, these findings were also confirmed on other metallic Pd/Pt catalysts. The role of step sites in C–N bond cleavage was proposed using the density function theory calculations. The reactants have stronger adsorption energies on the step atoms, and step atoms have d-band center nearer to the Fermi level. In this case, the interaction with the reactant is stronger, which is beneficial for activating the C–N bond of the reactant.
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Qinghua Tian,Lingxiangyu Li,Li Yang,Jizhang Chen,Shin-ichi Hirano
With a much higher theoretical capacity than that of graphite anodes, SnO 2 has attained great attention as a potential anode material for next-generation lithium-ion batteries. However, it's practical application yet be impeded by such disadvantages of poor conductivity and terrible structure stability during repeated discharge/charge process. Herein, a unique TiO 2 /SnO 2 /C hybrid (TiO 2 SS@SnO 2 @C) consist of one-dimensional TiO 2 nanobelts , zero-dimensional SnO 2 nanoparticles and conformal carbon coating has been fabricated based on a strategy of synergistic effect of components with different dimensional nanostructures , which can provide improved electrochemical kinetic and outstanding structure stability for the TiO 2 SS@SnO 2 @C. As a result, the TiO 2 SS@SnO 2 @C is able to exhibit outstanding lithium storage performance as an anode material, delivering capacities of 904.9 and 492.4 mAhh g −1 after even 400 cycles at 200 and even 1000 mA g −1 , respectively. It is demonstrated that the synergistic effect of these components is responsible for thus outstanding electrochemical performance.
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DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 9
·2889-2900
·
IF 9.48
Song Li,Long Yan,Qiying Liu,Jianguo Liu,Qiyu Liu,Wei Fan,Xuelai Zhao,Xinghua Zhang,Chenguang Wang,Longlong Ma,Qi Zhang
One-pot hydrodeoxygenation (HDO) of biomass furan derivatives into long-chain alkanes remains unclear owing to the complicated reactions at high temperatures. Here, Pd/C combined with phosphotungstic acid (HPW), a strong Brønsted solid acid promoter, was developed to produce decane under mild conditions through the one-pot HDO of δ-furfurylidenelevulinic acid (FDLA). A 93.16% sum yield of alkanes including 89.53% yield of decane was obtained under 3 MPa H2 at 170 °C for 4 h. The ring-opening and HDO of furans are accomplished at preheating stage, which enable to clarify the complicated reaction pathway. In addition, experimental validations and catalytic characterizations confirm that the synergistic effect of active acid–metal sites plays a critical role in the generation of alkanes via the formation and hydrogenolysis of lactone intermediates to aldehyde/alcohol. This work provides guidance for the one-pot HDO of biomass furan derivatives via the combination of metal catalyst and strong Brønsted solid acid under mild conditions.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 23
·13562-13569
·
IF 12.732
Boran Wang,Mengjie Lu,Duo Chen,Qi Zhang,Wenwen Wang,Yutang Kang,Zhenxing Fang,Guangsheng Pang,Shouhua Feng
Self-supported nickel–iron nitride microsheet arrays coated with carbon are grown on commercial Ni foam (NixFeyN@C/NF) and used as an electrocatalyst for splitting of alkaline seawater. The porous architecture and superhydrophilic/superaerophobic surface ensure sufficient exposure of active sites and mass transfer. The synergetic coupling effect between the carbon coating and NixFeyN facilitates electron transport. The optimal anode (Ni3FeN@C/NF) and cathode (Ni3N@C/NF) electrocatalysts are employed to assemble a two-electrode seawater electrolyzer for overall alkaline seawater electrolysis, which delivers a large current density of 500 mA cm−2 at a low cell voltage of 1.91 V. The superior corrosion-resistance and electron conductivity of the electrocatalyst are responsible for its excellent durability up to 100 hours. This result suggests that transition-metal nitrides coated with carbon offer an effective route to fabricate high-performance and durable hybrid electrocatalysts for hydrogen production from seawater electrolysis.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 13
·5371-5386
·
IF 3.5
Cai Haopeng,Lin Zhenqin,Gao Lihua,Feng Chaochao,Tang Rui
Abstract The derivatives of metal–organic frameworks have been proven to be ideal candidates for microwave absorption due to their ability to form diverse microstructures of metals/heteroatom doped-carbon composites. In this study, we synthesized three types of zinc oxide (ZnO)@ZIF-8 with varying ZIF-8 shell thicknesses using ZnO colloidal spheres as sacrificial templates. Subsequently, we investigated the microwave absorption properties of a series of non-magnetic ZnO/N-doped carbon nanospheres pyrolyzed by ZnO@ZIF-8 at different temperatures. Remarkably, the non-magnetic samples (30 wt% filler loading) with a hollow structure pyrolyzed at 800 °C exhibited a broad effective absorption band exceeding 6 GHz. The excellent microwave absorbing performance of the samples pyrolyzed at 800 °C can be attributed to the reduction of the ZnO core to Zn 0 , anchoring it in the graphitized N-carbon layer, and the formation of an inner hollow cavity that enhances impedance matching. Therefore, this research not only provides an array of excellent dielectric-type microwave absorbing materials but also presents a novel strategy for developing lightweight and high-performance non-magnetic carbon-based microwave absorbing materials. Graphical abstract
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2019
·Vol. 30
·期 16
·15267-15276
·
IF 2.195
Zhang Qingji,Jing Jiangping,Chen Zhuoyuan,Sun Mengmeng,Li Jiarun,Li Yan,Xu Likun
g-C 3 N 4 is a promising material for the application in the area of photoelectrochemical cathodic protection. However, it suffers from limited light absorption and lower charge separation efficiency. In this work, a N defects and C deposition co-modified g-C 3 N 4 , C–g-C 3 N x , was prepared by NaOH-assisted sintering and ethanol-assisted hydrothermal treatment. The presence of N defects and C deposition was verified by the XRD, SEM and XPS tests. The N defects changed the band structure of g-C 3 N 4 by lowering down the conduction band position, therefore widening the light absorption range of g-C 3 N 4 . In addition, the N defects and C deposition co-modification promotes the charge transfer process of g-C 3 N 4 , leading to increased separation efficiency of the photogenerated charge carriers. Therefore, C–g-C 3 N x shows enhanced photoelectrochemical cathodic protection performance for the coupled 316L stainless steel. It can provide a photoinduced potential drop of 120 mV and a photoinduced current density of 9.1 μA cm −2 , which is three times that of pristine g-C 3 N 4 .
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高影响因子
ADVANCED SYNTHESIS & CATALYSIS
·
2017
·Vol. 359
·期 13
·2215-2221
·
IF 5.646
Wenhui Zhu,Yingcai Ding,Zhaogang Bian,Ping Xie,Baojun Xu,Qiujie Tang,Wei Wu,Aihua Zhou
Sulfenylation is an important transformation to generate C−S bonds in organic synthesis. Here, two three-component synthetic protocols have been developed by using imidazo[1,2- a ]pyridine, inorganic, odorless S 8 and alcohols or arylboronic acids as reactants to make alkylthio-/arylthio-substituted imidazo[1,2- a ]pyridine derivatives via C( sp 2 )–H functionalization. The reactions proceeded with high efficiency and broad functional group tolerance, affording the products regioselectively and in good yields.
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DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2021
·Vol. 45
·期 10
·14720-14731
·
IF 5.164
Yang Zhan,Qing Wang,Shao-Hua Luo,Si Li,Luo-Xuan Wang,Xin Liu,Ya-Hui Zhang,Long-Jiao Chang
Summary The lithium transition metal orthosilicates (Li 2 MnSiO 4 ) compounds are considered key materials for the next-generation lithium-ion batteries (LIBs). However, they exhibit poor electronic conductivity and structural stability. Herein, the dual-phase ( Pmn2 1 , and Pn ) coexisting Li 2 Mn 1− x Ni x SiO 4 @C is prepared successfully via a two-step calcination process to address the aforementioned problems. The orthorhombic Pmn2 1 and Pn phase are expected to bring well solid-state Li diffusion properties (D Li + ) and structural stability for electrode material, respectively. Also, the Ni doping and carbon coating are expected to raise electronic conductivity. Then, the electrochemical performance of LIBs utilizing LiMn 0.995 Ni 0.005 SiO 4 @C, LiMn 0.985 Ni 0.015 SiO 4 @C, and LiMn 0.92 Ni 0.08 SiO 4 @C (ZNi-02 to ZNi-04) as cathode materials are investigated and compared with that of the LiB using Li 2 MnSiO 4 @C (ZNi-01). The ZNi-04 sample-based LiB shows well D Li + and a peak discharge capacity as high as 188.4 mAh g −1 . In addition, the ZNi-04 sample can still maintain a capacity of about 80 mAh g −1 at rate of 8 C. Such excellent electrochemical performance is ascribed to the synergistic effect of the dual-phase coexistence, the proper amount of Ni doping, and surface coating of carbon, which enhances the electrical conductivity and structural stability. Thus, Li 2 Mn 1− x Ni x SiO 4 @C has broad application chances as a high-performance LIBs electrode material.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Jiang Li,Jiaxing Liu,Junjie Zhang,Tong Wan,Lei Huang,Xintian Wang,Runze Pan,Zhidong An,Dionisios G. Vlachos
Cobalt (Co) catalysis has recently attracted significant attention in the field of biomass conversion. However, the fabrication of highly dispersive Co nanoparticles at high metal loading with selective facet exposure to achieve specific selectivity is still questionable. In this work, a nitrogen-doped carbon-supported Co catalyst is fabricated for efficient conversion of fatty acids and esters to liquid alkanes. Nitrogen-doping facilitates a highly uniform dispersion of Co nanoparticles even at a high Co loading of 10 wt% and after recycling for 5 runs. The Co/N-C catalyst affords an unconventional decarbonylation/decarboxylation (DCOx) dominant selectivity probably due to partial reduction of cobalt oxides to α-Co 0 with only exposure of the (111) facet. Co-existence of Co and N-C leads to strong Lewis acidity and basicity, facilitating the interaction between catalyst and –COOH group, and some important acid-catalyzed step-reactions. The versatility of the Co/N-C catalyst is demonstrated through conversion of various fatty acids and esters.
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DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 50
·31663-31670
·
IF 3.108
Hong Wang,Taotao Jiang,Lei Ma,Hanbing Wang,Xiaoliang Xu,Chunshan Lu,Xiaonian Li
In this study, we found that the phenylhydroxylamine intermediate could desorb more easily from an Ir surface than from a Pt surface, which is beneficial for inhibiting the over-hydrogenation of phenylhydroxylamine to aniline. On the other hand, the Brφnsted acid functionalized ionic liquids with sulfonic acid and bisulfate anions were acidic enough to catalyze the Bamberger rearrangement to form p-aminophenol from phenylhydroxylamine. On this basis, a new catalytic system constructed by Ir/C and Brφnsted acid functionalized ionic liquid was applied, for the first time, to the one-pot hydrogenation of nitrobenzene to p-aminophenol. Our results indicate that the PAP selectivity of Ir/C and [SO3H-bmim][HSO4] Brφnsted functionalized ionic liquid was far more than that of the traditional Pt/C and sulfuric acid catalyst system. Furthermore, the dually functionalized ionic liquid ([HSO3-b-N-Bu3][HSO4]) can be used simultaneously as an acid catalyst and also as a surfactant, due to its higher lipophilicity. Therefore, our new catalytic system has unique advantages in the hydrogenation of nitrobenzene to p-aminophenol.
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高影响因子
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