JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
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IF 10.319
Xiaotong Feng,Lifen Gu,Naiyu Wang,Qiaosheng Pu,Guangli Liu
Carbon-based adsorption and TiO 2 -based photocatalysis are both safe and low-cost ways of pollutant purification. Constructing C-TiO 2 architectures can effectively improve removal efficiency. However, most of those carbon frames only acted as supporting substrates, exhibiting rather limited synergistic action from TiO 2 and carbon. Herein, Fe/N co-doped nano-TiO 2 wrapped on mesoporous carbon spheres with a core-shell structure was designed. The Fe, N co-doped carbon sphere with a hierarchical structure improved the synergy of adsorption and transfer during the photocatalytic process. Without extra dopant, the Fe and N partly exposed on the surface realized the in-situ migrating into the TiO 2 shell to enhance the interface effect, which significantly promoted the photocatalytic efficiency of the composite. Furthermore, the photocatalytic efficiency of the composite was investigated through two typical pollutants under visible-light irradiation. The degradation efficiencies for rhodamine B and paraxylene were 96.2% in 60 min and 94.1% in 20 min, respectively, with the apparent rate constant of 0.045 min –1 and 0.049 min –1 , 8.3 and 11.4 times of that for bare TiO 2 . The composite is likely advantageous for treating diverse environmental pollutants.
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 15
·4720
·
IF 4.927
Xinjun Yu,Zengchao Jiang,Xiaodan Xu,Changyi Huang,Zheyi Yao,Xiao Yang,Yinjun Zhang,Dongsheng Wang,Chun Wei,Xuwei Zhuang
Chitin, the second richest polymer in nature, is composed of the monomer N-acetylglucosamine (GlcNAc), which has numerous functions and is widely applied in the medical, food, and chemical industries. However, due to the highly crystalline configuration and low accessibility in water of the chitin resources, such as shrimp and crab shells, the chitin is difficult utilize, and the traditional chemical method causes serious environment pollution and a waste of resources. In the present study, three genes encoding chitinolytic enzymes, including the N-acetylglucosaminidase fromOstrinia furnacalis(OfHex1), endo-chitinase fromTrichoderma viride(TvChi1), and multifunctional chitinase fromChitinolyticbacter meiyuanensis(CmChi1), were expressed in thePichia pastorissystem, and the positive transformants with multiple copies were isolated by the PTVA (post-transformational vector amplification) method, respectively. The three recombinants OfHex1, TvChi1, and CmChi1 were induced by methanol and purified by the chitin affinity adsorption method. The purified recombinants OfHex1 and TvChi1 were characterized, and they were further used together for degrading chitin from shrimp and crab shells to produce GlcNAc through liquid-assisted grinding (LAG) under a water-less condition. The substrate chitin concentration reached up to 300 g/L, and the highest yield of the product GlcNAc reached up to 61.3 g/L using the mechano-enzymatic method. A yield rate of up to 102.2 g GlcNAc per 1 g enzyme was obtained.Keywords:chitinase;shrimp and crab shell;N-acetylglucosamine;mechanoenzymology;heterologous expression
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高影响因子
LANGMUIR
·
2022
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IF 4.331
Changsheng Sun,Shujing Zhou,Jinjing Li,Chenze Qi,Yong Gao
Nonaqueous Pickering emulsions exhibit promising applications in many industrial areas but have been relatively less studied in the past. In this study, n-hexane-in-DMF nonaqueous Pickering emulsions stabilized by core cross-linked copolymer worms with mixed shells are demonstrated for the first time. Core cross-linked copolymer worms with mixed shells were prepared by seeded reversible addition–fragmentation chain transfer (RAFT) quasi-solution polymerization. Specifically, polystyrene-poly(4-vinylpyridine) (PS-P4VP) diblock copolymer worms were first prepared via RAFT-mediated dispersion polymerization in toluene under the given conditions using PS as both the macro-CTA and the stabilizer block. After the chemical cross-linking of P4VP cores, PS-P4VP diblock copolymer worms were chain-extended with LMA in DMF/toluene (1:9, weight ratio) mixed solvents, producing core cross-linked PS-P4VP-PLMA worms with PS/PLMA mixed shells. The as-prepared core cross-linked PS-P4VP-PLMA worms with mixed PS/PLMA shells were further utilized as Pickering emulsifiers for the generation of nonaqueous n-hexane-in-DMF Pickering emulsions. The emulsifying performances of mixed-shell copolymer worms were compared with those of their spherical and linear analogues with entirely identical chemical compositions as well as PS-P4VP diblock copolymer worm precursors, respectively.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Qing Xu,Linlin Zang,Ziying Li,Fengtong Shen,Yanhong Zhang,Liguo Sun
As a new generation of non-precious metal catalysts , nickel phosphide is regarded as an ideal substitute for precious metal platinum in electrochemical hydrogen evolution . Here, a hydrogen evolution reaction (HER) electrocatalyst is developed by in situ growth of Ni 2 P/Ni 5 P 4 heterostructures on porous N decorated rGO foam (named Ni 2 P/Ni 5 P 4 /N-rGO). The porous rGO foam structure provides a larger surface area and abundant active sites. The Ni 2 P/Ni 5 P 4 nanoparticles with heterostructures are uniformly distributed on the rGO sheet, which enhance the charge transfer ability. The decorating of N element also correspondingly improves the HER performance. The as-prepared Ni 2 P/Ni 5 P 4 /N-rGO exhibits excellent HER performance in alkaline medium . When the current density is 10 mA cm −2 , the overpotential is only 22 mV. No obvious loss of HER activity after 2000 cyclic voltammetry indicates that the composite has excellent stability. This work presents a valuable route for fabricating inexpensive and high-performance catalysts for electrocatalysis .
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CATALYSIS TODAY
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2022
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IF 6.562
Linhao Yu,Hong Chen,Yingying Li,Zhe Wen,Yongdan Li
The metallic cobalt supported on nitrogen dopped carbon material was employed as an efficient catalyst in the oxidative esterification of 5-hydroxymethylfurfural (HMF) to furan-2,5-dimethylcarboxylate (FDMC). The carbonization temperature has a significant effect on the morphology and structure of Co/N-C samples. The Co/N-C calcined at 900 °C exhibits the best catalytic performance and a 73.8% FDMC yield at 91.7% HMF conversion is measured at 130 °C for 20 h with K 2 CO 3 under 1 MPa O 2 . The catalytic activity of Co/N-C was benefited by the synergistic effect between the metallic cobalt and nitrogen-doped carbon material. The reaction mechanism of FDMC formation was proposed.
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高影响因子
FUEL
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2022
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IF 8.035
Yang Liu,Xiaobei Cheng,Yuchen Ya,Bowen Wang,Pu Zhang,Kai Zhang,Yishu Xu
PODE 3 , with the molecular formula of CH 3 O(CH 2 O) 3 CH 3 , is considered a highly competitive alternative fuel due to the absence of C C bond and its high oxygen content, and have been shown to significantly reduce soot emission when applied as a diesel fuel additive. However, the effect of PODE 3 addition on the oxidation reactivity of soot generated in the flame remains unclear which is of great importance for the optimal design of the post-treatment devices during its application. In this work, the impact of PODE 3 (0 %, 10 %, and 20 % by volumetric fraction) addition on the oxidation reactivity of soot at different maturity and oxidation degrees in n -heptane/toluene co-flow diffusion flames was specially investigated combining information on thermogravimetric analysis, high-resolution transmission electron microscope, and Raman spectroscopy. Results showed that PODE 3 substitution significantly shrank soot generation region, and increased the flame temperatures before height above burner (HAB) < 45 mm. The addition of PODE 3 improved the soot oxidation reactivity, which had a strong ability to hinder the growth of the microcrystalline carbon layers and resulted in a high content of amorphous carbon in soot particles. Specifically, it had more significant impacts on the soot in the oxidation stage than the surface growth stage. These can be explained that with PODE 3 addition, on the one hand, the “reliable carbon atom” for soot formation is significantly reduced and the amount of oxidizing species is increased, resulting in a smaller particle size and a higher content of disordered and amorphous carbon in soot particles. On the other hand, the flame temperatures increased where HAB < 45 mm, which would promote the soot formation reactions. The combined effects of these factors make PODE 3 have more significant inhibitory impacts in reactivity of soot sampled at oxidation stage than that at surface growth stage. Therefore, the impact of PODE 3 addition on soot nanostructures and oxidation reactivity is not only reflected in its chemical effect but also in temperature effect.
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高影响因子
RSC Advances
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2022
·Vol. 12
·期 32
·20481-20491
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IF 4.036
Yanming Miao,Xinhao Zhang,Jinyao Li,Wenli Yang,Xiaomin Huang,Jinzhi Lv
Room-temperature phosphorescent (RTP) N-doped carbon-dots (CNDs) featuring eco-friendliness, low cost and high biocompatibility, are ideal photodynamic antibacterial and anticancer nanomaterials. However, the existing CNDs are limited by low singlet oxygen (1O2) quantum yield, which has become a bottleneck in the development of CNDs. One basic reason is the short T1-state exciton lifetime of CNDs. Herein, triethylenetetramine hexaacetic acid was used to synthesize CNDs via a one-step hydrothermal method. CNDs are characterized with low toxicity, high biocompatibility and ultralong-lifetime RTP (URTP). In addition to the URTP (average lifetime 414 ms) under solid conditions, CNDs even had URTP (average lifetime 320 ms) in a water environment. The ultralong T1 exciton lifetime largely extends the collision time between T1 state excitons and O2 and prolongs the energy transfer time, not only improving the quantum yield (0.63) of singlet oxygen (1O2) in solution, but also facilitating the photodynamic antibacterial and anticancer effects.
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
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2021
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IF 3.205
Lei Feng,Xianyu Liang,Xuejin Mao,Hao Wan,Yan Wu,Quanbin Han
N-phenylglycine (NPG) in human urine could be an important biomarker for predicting cancers, but its detection has difficulty due to its low abundance in urine. Herein, we report a molecular imprinted polymer (MIP) method to efficiently recognize NPG in urine. The MIP was prepared by precipitation polymerization, adopting NPG as the template, acrylamide (AM) as functional monomer, trimethylpropane triacrylate (TRIM) as crosslinking agent, and acetonitrile as porogen. The specificity and selectivity of MIP towards NPG in human urine were determined by comparing MIP's adsorption to the NPG and N-crotonylglycine (NTG) under the same conditions. The result β = Q MIP-NPG / Q MIP-NTG = 4.7 indicated the satisfactory specificity and selectivity. Parameters affecting the extraction efficiency were further optimized. Under the optimum conditions, the linear range, limit of detection, and limit of quantification of NPG were 0.5–100 mg∙L −1 , 1.6 × 10 −2 mg∙L −1 , and 5.5 × 10 −2 mg∙L −1 , respectively. Recoveries of NPG in human urine were in the range of 84.7–100.0% with RSD S of 3.8–10.8%. The developed method demonstrated superior selectivity to the target analyte, which can be applied to separate and enrich the NPG from urine samples.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Xueping Sun,Peng Wei,Jinxu Zhang,Songqi Gu,Ruoou Yang,Chun Fang,Qing Li,Jiantao Han,Zheng Jiang,Jianhua He
Integrating the unique metalloid behaviour of monometallic phosphides and modified local electronic/geometric structures of active sites, bimetallic phosphides have emerged as promising candidates for water splitting reaction, but they are still synthesized by toxic, corrosive, and high-temperature methods, which inevitably resulted in an increase of particle size and the decrease of catalytic activity area. Herein, the ultra-fine bimetallic NiCoP catalysts in-situ embedded in P, N-codoped carbon nanofibers (NiCoP@PNCNF) were successfully fabricated via a facile electrospinning method with the help of phytic acid. Profiting from the unique macro-structural design and micro-electronic/geometric modification, as-prepared NiCoP@PNCNF catalysts exhibited excellent catalytic performance both for HER (η 10 = 98 mV) and OER (η 10 = 260 mV) in terms of the low overpotential and robust stabilities in alkaline solution. Meanwhile, XAFS analysis further demonstrated that the remarkable catalytic performance not only attributed to the introduction of heteroatom-doped carbon fibers as their improvements in the corrosion resistance, anti-agglomeration abilities, and conductivity, but also benefited from the local electronic/geometric structure alternations as the strong synergic effects between Ni/Co and P atoms. For practical application, the water splitting performance based on NiCoP@PNCNF electrodes was also investigated and exhibited a lower splitting potential (E J=10, 1.645 V) over long-term stability tests. These insightful findings undoubtedly shed light on the design and fabrication of cost-effective and robust bifunctional transition-metal phosphides electrocatalysts.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yanling Chen,Xue Bai,Yetong Ji,Ting Shen
A novel reduced graphene oxide-supported hollow Co 3 O 4 @N-doped porous carbon (Co 3 O 4 @NPC/rGO) composite was synthesized via self-assembly and pyrolysis-oxidation using bimetallic zeolite imidazolate frameworks and graphene oxide as precursors. The as-obtained composite exhibited superior performance on peroxymonosulfate (PMS) activation over a wide pH range. Complete removal of sulfamethoxazole (SMX, 25 mg·L −1 ) was achieved within 5 min and the reaction rate constant was higher than those of the most reported heterogeneous catalyst/PMS systems for SMX degradation. It was demonstrated that both radical pathways (SO 4 − , OH, and O 2 − ) and non-radical pathways ( 1 O 2 and direct electron transfer) were involved in the SMX degradation. Significantly, the contribution ratio of each reactive oxidative species (ROS) in the bulk solution or on the catalyst surface was differentiated and calculated for the first time. SO 4 − both in the bulk solution and on the catalyst surface as well as the 1 O 2 in the bulk solution were the dominant ROS. The possible degradation mechanism of SMX by Co 3 O 4 @NPC/rGO/PMS system was proposed. Co active sites with high activity, the electron-rich ketonic group and the nitrogen doping sites within Co 3 O 4 @NPC/rGO contributed to the excellent catalytic activity. The ecotoxicity of SMX and its intermediates was investigated. Besides, the reusability, stability and application potential in actual waterbodies of Co 3 O 4 @NPC/rGO were evaluated. Overall, this work expands the environmental application of metal–organic frameworks (MOFs)-derived hollow nanomaterials and provides a promising heterogeneous catalyst for the elimination of refractory contaminants by sulfate radical-based advanced oxidation processes (SR-AOPs).
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Inorganic and Nano-Metal Chemistry
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2021
·
IF 1.716
Zhihang Li,Kaikai Hu,Weiqiang Xu,Shouwen Jin,Liqun Bai,Daqi Wang
Seven organic-inorganic hybrids [(H2L1)3(Bi2Br9)(BiBr6)(H2O)] (1) (L1 = N,N,N′,N′-tetramethylethylenediamine), [(HL2)3(SbCl5)] · Cl (2) (L2 = 4-chlorobenzylamine), [(HL3)3(SbCl4)] · Cl2 (3) (L3 = 2,6-dimethylaniline), [(HL3)2(ZnCl4)] · 2H2O (4), [(HL4)4(Bi2Br10)] (5) (L4 = 2-methylquinoline), [(HL4)2(SbCl5)] (6) and [(H2L5)2(SbCl5)2] · H2O (7) (L5 = bis(N-imidazolyl)methane) were prepared and characterized by IR, XRD, EA and TG analysis. XRD analysis told that all complexes were built from non-covalent bonds between the cations and the perhalometallates anions. The lattice H2O also played crucial role in structure extension in the respective hybrids.Extensive intermolecular interactions have been used in the self-assembly of diverse motifs, ranging from strong X-H···Y (X = O, N; Y = Br, Cl, O) H-bonds to weak CH-M (M = Cl, Br), CH2-M (M = Cl, Br), CH3-M (M = O, Cl, Br), CH3-CH3/CH3-CH/CH2-CH/CH-CH, Cl-Cl, CH3-π and π-π associations. Among them, 3 D architectures are found in 1–2 and 4–7, but only 2 D motif is appeared in 3. The arrangements of the anions and cations in the solid mode are ruled not only by the size and symmetry of the cations, but also by the non-covalent bonds in the crystals.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zichen Zhang,Hengjun Gai,Qun Li,Bingxiao Feng,Meng Xiao,Tingting Huang,Hongbing Song
In this work, N-rich ionic liquid based on 1,3,5-triimidazole triazine was used to construct poly(ionic liquid) (PIL) through free radical polymerization, and support palladium nanoparticles (Pd NPs), which were used in the catalytic hydrogenation of nitrobenzene. The resulting N-rich PIL had a good dispersion effect and ultrafine Pd NPs as shown by SEM and TEM, thereby significantly enhancing the stability of the loaded metal NPs. The XPS results indicated that the metal-support interaction improved the catalytic performance of the catalyst. In particular, the effects of different anions (Tf 2 N - , PF 6 - , and Cl - ) on the PILs were investigated, and the results showed that the Tf 2 N anion exhibited the best catalytic effect on the hydrogenation of nitrobenzene. Furthermore, density functional theory calculation confirmed that anions played a key role in activating the substrate in the hydrogenation of nitrobenzene. The corresponding results were consistent with the experimental results, which provided reference and research for the application of PILs in the future.
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危险品化学品经营许可证（带存储）