2020 Volume 37 Issue 10

Recent Advances in Application of Metal-Orgainic Framework-Derived Catalysts for Hydrogenation of Carbon Dioxide and Fischer-Tropsch Synthesis
LIU Junhui , SONG Yakun , SONG Chunshan , GUO Xinwen
2020, 37(10): 1099-1111  doi: 10.11944/j.issn.1000-0518.2020.10.200128
[Abstract](1505) [FullText HTML] [PDF 979KB](17)
Abstract:
Hydrogenation of CO2 and Fischer-Tropsch synthesis reactions are the important research fields in C1 chemistry. Hydrogenation of CO2 to form value-added chemicals and fuels is beneficial for reducing the CO2 concentration in the atmosphere and mitigating the pressure on fossil fuel consumption. Fischer-Tropsch synthesis is considered as a significant route to produce liquid fuels and chemicals from non-petroleum sources. Development of novel, efficient, and stable catalysts is an urgent point for hydrogenation of CO2 and Fischer-Tropsch synthesis. The metal-organic framework(MOF)-derived catalysts have a good application prospect in hydrogenation of CO2 and Fischer-Tropsch synthesis. This paper reviews the preparation methods of MOF-derived catalysts and the catalytic performance in the reactions. In addition, the current problems are summarized and the future development of this field is pointed out.
Recent Development in Ionic Exchange Groups-Based Anion Exchange Membrane
FU Fengyan , CHENG Jingquan , ZHANG Jie , GAO Zhihua
2020, 37(10): 1112-1126  doi: 10.11944/j.issn.1000-0518.2020.10.200095
[Abstract](827) [FullText HTML] [PDF 887KB](3)
Abstract:
Anion exchange membrane fuel cells (AEMFCs) have attracted worldwide attention. To achieve high performance in AEMFCs, anion exchange membranes (AEMs) should own high ion conductivity and good alkaline stability. AEMs contain cationic groups and polymer backbone, while ionic groups play very important role in determining the overall stability and conductivity for the AEMs apart from polymer backbones. In this paper, the structure, alkaline stability and ion conductivity of AEMs with different kinds of cationic groups such as quaternary ammonium, guanidinium, imidazolium, phosphonium, metal cation, N-spirocyclic cations, piperidinium and pyrrolidinium are introduced in detail, and the development trend of the cationic groups are also discussed.
Application of Quartz Crystal Microbalance with Dissipation in Biomedical Polymer Materials
SUN Bin , LÜ Jianhua , JIN Jing , ZHAO Guiyan
2020, 37(10): 1127-1136  doi: 10.11944/j.issn.1000-0518.2020.10.200078
[Abstract](1213) [FullText HTML] [PDF 983KB](9)
Abstract:
Quartz crystal microbalance (QCM) is an analytical technique based on the piezoelectric effect of quartz crystal, which can provide the information on the mass, thickness and viscoelasticity of the adsorbed layer on the surface of quartz crystal in real time, and thus obtain the surface molecular interaction relationship. Because of the unique viscoelastic analysis, QCM with dissipation (QCM-D) has been rapidly applied in the field of polymer material, especially for biomedical polymer materials. It has been used to evaluate the surface and interface interaction, mechanical property, and biocompatibility of biomedical biomaterials. In this review, the basic principle and theoretical model of QCM-D are briefly introduced. The application of QCM-D in the conformation of polymer chain, protein adsorption, biomolecular interactions, drug release and hydrogels in recent years are emphatically reviewed, and finally the future development trends of QCM-D is forecasted.
Progress in Matrix-Assisted Laser Desorption Mass Spectrometry Imaging for Fingerprint Analysis
LI Wenjie , WANG Lixue , SUN Linghui , YOU Wei , ZHAO Yabin
2020, 37(10): 1137-1146  doi: 10.11944/j.issn.1000-0518.2020.10.200108
[Abstract](607) [FullText HTML] [PDF 1192KB](3)
Abstract:
Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) is a soft ionization mass spectrometry technique with high sensitivity, high throughput and simultaneous analysis of multi-components. It can confirm the molecular structure and obtain the material distribution information through the material analysis and has gained more and more attention in fingerprint analysis. Starting from the condition optimization, this paper describes the process of matrix optimization. Then, the specific application of MALDI-MS imaging (MALDI-MSI) in the field of fingerprint analysis is introduced. In the aspect of morphological analysis, the influence of the combination of MALDI-MSI and the conventional development methods on the imaging effect and the image processing of the difficult fingerprint is summarized. In terms of chemical information analysis and research, the advantages and limitations of each research are reviewed from the perspective of analyzing living habits/pre-crime activities, fingerprint residual time and individual identity based on MS information, and the future development of MALDI-MSI in the field of fingerprint is proposed.
Preparation and Characterization of Hydrogen-Bonded Carbon Nanotubes Reinforced Self-healing Composites
CHENG Yinjie , ZHANG Lu , HU Renjie , WANG Ying , JIN Xuexin , QIU Shuo , ZHANG Haoyan , JIANG Dawei
2020, 37(10): 1147-1155  doi: 10.11944/j.issn.1000-0518.2020.10.200112
[Abstract](985) [FullText HTML] [PDF 865KB](8)
Abstract:
The hydrogen-bonded self-healing composites were manufactured successfully (dimer acid, diethylenetriamine, and urea as raw materials, and carbon nanotubes as reinforcing agents). The composites have good mechanical properties and can self-heal at room-temperature (30 ℃). The mechanism of self-healing was proposed in the paper. The stress-strain tests were performed on self-healing composites with different amounts of carbon nanotubes. It is found that the stress and the strain of the composites increases with the increased addition of carbon nanotubes. The stress of composites can reach 4 MPa and the strain increases more than 6% as 9% (mass fraction) of carbon nanotubes is added into the composites. The surface morphology, self-repairing performance and thermal stability of the self-healing composites with 9% (mass fraction) of carbon nanotubes were tested. The results show that carbon nanotubes have good compatibility with the material, and the morphologies of the surface and fracture surface of the cut composites are similar. The self-healing efficiency of composites can reach 100% at room temperature for 24 h. The self-healing efficiency is more than 90% after 10 fracture-healing cycles. The composites have excellent thermal stability, and the temperature at the maximum mass loss rate is 474 ℃. The composites provide an option for next-generation skin sensors and wearable smart devices.
Preparation and Properties of Mercapto Bentonite
DONG Xun , ZHU Xiaping , CUI Ting
2020, 37(10): 1156-1163  doi: 10.11944/j.issn.1000-0518.2020.10.200075
[Abstract](899) [FullText HTML] [PDF 975KB](17)
Abstract:
In order to simplify the preparation process and reduce the preparation cost of mercapto bentonite (Bent-SH) for practical application, the bentonite(Bent) was synergistically modified by 3-mercaptopropyltrimethoxysilane (MPS) and sodium silicate. The preparation process of Bent-SH was optimized, the structure of Bent-SH was characterized, and the performance of Bent-SH was measured. The best process is:the solid-liquid ratio of Bent to MPS is 1:0.05 (g/mL); the mass ratio of Na2SiO3 to Bent is 7.0:100; the solid-liquid ratio is 1:20 (g/mL); the pH of the modified suspension is 8.0~10.0; the modification time is 5~6 h, and the reaction temperature is room temperature. The gum value, expansion factor and cation exchange capacity of Bent-SH decrease compared with Bent, but the saturated adsorption capacity of Bent-SH for cadmium is 20.86 mg/g, 20 times more than that of Bent. The synergistic modification of sodium silicate and MPS does not change the layer structure of material, but significantly improve the hydrophobicity, dispersity, adsorption capacity and selectivity. The Bent-SH is a promising passivator for heavy metal contaminated soil.
Assembly of Graphene Oxide-Based Flexible Generator and Its Water Evaporation Power Generation Performance
YU Zhiqiang , QU Jiangying , LI Jielan , ZANG Yunhao , GU Jianfeng , GAO Feng
2020, 37(10): 1164-1171  doi: 10.11944/j.issn.1000-0518.2020.10.200087
[Abstract](1878) [FullText HTML] [PDF 883KB](10)
Abstract:
How to use water evaporation energy which is widely existing in nature is a challenging subject. In this paper, graphene oxide (GO) with abundant functional groups and excellent hydrophilicity was used as the power generation material, and reduced graphene oxide (RGO) prepared by hydrazine reduction was used as the electrode material. GO/RGO flexible generator was assembled by a simple dropping method on the polyethylene terephthalate (PET) substrate. The working area of GO film generator was fixed as 4.5 cm by 1.5 cm, and its power generation performance induced by water evaporation was studied. Driven by natural water evaporation at room temperature, it can output an open circuit voltage (Voc) of 90 mV and a short circuit current (Isc) of 0.6 μA as well as power density of 1.25 μW/cm3. The generator also exhibits excellent flexibility and high stability. Based on the classic flow potential theory, the mechanism of GO/RGO generator induced by water evaporation is proposed. This paper provides a new way for the use of water evaporation energy with simple steps, low cost and stable performance.
In Situ Synthesis of Nitrogen-Doped Carbon Coated CoxP Composites and Their Lithium Properties
ZHANG Xinyu , QU Jiangying , TANG Zhanlei , LI Jielan , WANG Tao , GAO Feng
2020, 37(10): 1172-1180  doi: 10.11944/j.issn.1000-0518.2020.10.200072
[Abstract](1958) [FullText HTML] [PDF 1332KB](13)
Abstract:
Nitrogen-doped carbon coated Co2P@N-C and CoP@N-C composites were in situ synthesized at 800 ℃ using zeolitic imidazolate framework-67 (ZIF-67) as cobalt/nitrogen/carbon precursor and red phosphorus as phosphorus source, and their electrochemical properties were studied as anode materials of lithium ion batteries. It is found that the resulted products can be tailored by the ratio of ZIF-67 to red phosphorus. The obtained Co2P@N-C and CoP@N-C composites show regular dodecahedron and the size of about 250 to 400 nm and exhibit good conductivity. When they are used as anode materials, the first discharge capacity of the Co2P@N-C and CoP@N-C composites are 942 and 1170.6 mA·h/g at the current density of 0.05 A/g, respectively. Even at the current density of 1 A/g, their capacities are maintained at 306.6 and 180.3 mA·h/g after 500 cycles, respectively. We have provided a green and easy method for the synthesis of CoxP@C composites for lithium ion battery.
Fade Mechanism of Ternary Lithium Ion Power Battery
YANG Tao , LIU Wenfeng , MA Mengyue , DONG Hongyu , YANG Shuting
2020, 37(10): 1181-1186  doi: 10.11944/j.issn.1000-0518.2020.10.200116
[Abstract](2970) [FullText HTML] [PDF 886KB](58)
Abstract:
Failure analysis is an effective way to analyze the failure phenomena caused by complex physical and chemical changes during battery cycling, optimize the material preparation and the manufacturing processes of battery, and improve the cycle performance. In this paper, after dismantling and analyzing the ternary nickel cobalt manganese (NCM, LiNi0.5Co0.2Mn0.3O2) lithium ion power battery (NCM LIPB) at 1 C in the voltage range of 3~4.2 V for 1000 cycles, it is found that the capacity loss of the cathode electrode is about 2.73%, and the capacity loss of anode electrode is about 2.4%. Comparing the X-ray diffraction and field emission scanning electronic microscope results of cathode and anode electrodes before and after cycling, capacity fade of cathode is mainly caused by the breakage of particles and the structural transformation of the NCM layer. The capacity fade of anode is generated by the damage of graphite layer structure, which is caused by the continuous Li+ de-intercalation during cycling. Moreover, the positive transition cation dissolves and deposits on the surface of electrodes, and catalyzes the side reaction of electrolyte/electrode interface to result in excessive film formation and loss of active lithium, which affects the dynamics of electrode process, one of the reasons for battery failure.
Promotion Effect of Functionalized Carbon Nitride on Pd-Based Catalyst for Hydrogen Generation from Formic Acid
SUN Zhicong , MENG Qinglei , MA Rongpeng , GE Junjie , LIU Changpeng , XING Wei
2020, 37(10): 1187-1194  doi: 10.11944/j.issn.1000-0518.2020.10.200088
[Abstract](712) [FullText HTML] [PDF 834KB](4)
Abstract:
The supported Pd-based catalyst is one of the most effective catalysts for the decomposition of formic acid into hydrogen, in which the N content of the carbon nitride support is relatively high. The carbon nitride prepared by one-step pyrolysis method is usually bulk, which makes it difficult to effectively disperse surface metal nanoparticles (NPs). Functionalized carbon nitride was obtained by pyrolyzing the urea precursor after solvation and used as a support. A functional carbon nitride-supported Pd-based catalyst (Pd/C3N4-F) was prepared by anion exchange and sodium borohydride direct reduction. The structure of the material was characterized by scanning electron microscope (SEM), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS), and the performance of the catalyst was tested by gas mass flow meter. Pd/C3N4-F has excellent catalytic performance for hydrogen production from formic acid decomposition and its initial TOF (total conversion frequency) value and mass specific activity at 30 ℃ are 1824 h-1 and 17.14 molH2/(gPd·h), respectively. The analysis of the product by gas chromatography (GS) shows that no by-product CO is formed, indicating that it has excellent selectivity. With the increase of temperature (30~40 ℃), the catalyst performance gradually improves.
Simultaneous Determination of Catechol and Hydroquinone by Copper Oxide Nanoparticles and Carbon Nanotubes Modified Glassy Carbon Electrode
CHANG Fengxia , SHANG Zongyi , DONG Qing , LONG Zhiyan , DENG Yixue
2020, 37(10): 1195-1202  doi: 10.11944/j.issn.1000-0518.2020.10.200048
[Abstract](917) [FullText HTML] [PDF 840KB](3)
Abstract:
Copper oxide nanoparticles and carboxylated multi-walled carbon nanotubes were used as modification materials for glassy carbon electrodes in this study. This nanocomposite combined the advantages of electrochemical signal amplification and electrocatalysis, and the as-prepared modified electrode could separate the redox peaks of catechol and hydroquinone and enlarge the peak currents further. Thus, this electrochemical sensor based on copper oxide nanoparticles and carbon nanotubes can be used for the simultaneous determination of catechol and hydroquinone. The ratio of copper oxide nanoparticles and carbon nanotubes in the nanocomposite, the cast volume and pH of the electrolyte are optimized via cyclic voltammetry. The optimal mass ratio between copper oxide nanoparticles and carbon nanotubes is 5:1. The optimal cast volume is 9 μL and phosphate buffer solution with pH=7.4 is used as the electrolyte. At the optimized conditions, the peak currents obtained with differential pulse voltammetric determination show good linear relationships with concentrations of catechol and hydroquinone in the range from 6.0×10-7~3.0×10-3 mol/L with detection limits of 1.0×10-7 mol/L and 1.60×10-7 mol/L (S/N=3), resepectively. This method is cheap, easy to operate and fast, and the recovery rates of practical water samples using this method are in a satisfactory range (94.6%~101.1%). Therefore, this proposed method has a good prospect of practical application.
Synthesis of NiO-WO3 Nanocubes and Their Application in Detecting Formaldehyde
SAN Xiaoguang , GONG Xiaohui , LU Yiming , QIAO Tongtong , YOU Yu , MENG Dan
2020, 37(10): 1203-1210  doi: 10.11944/j.issn.1000-0518.2020.10.200059
[Abstract](676) [FullText HTML] [PDF 1029KB](4)
Abstract:
The NiO-WO3 nanocubes are synthesized by hydrothermal synthesis. The p-n junction is formed by introducing p-type NiO to WO3 nanocubes. The products are characterized by XRD and SEM and have cube-like structures which are successfully retained after introducing NiO. The formaldehyde gas sensing properties are systematically investigated between the pure and NiO-WO3 nanocubes. The NiO-WO3 nanocube sensor exhibits enhanced response and lower operating temperature compared to the pure one. Especially, the 5% molar fraction of NiO-WO3 nanocube sensor exhibits the excellent sensing properties. Its highest response to 0.134 mg/L formaldehyde gas is 18.5 at 200 ℃. In addition, fast response and recovery, good reproducibility and stability, and good selectivity to formaldehyde are also obtained, indicating the formation of NiO-WO3 heterojunction in favor of improving the sensing properties. Meanwhile, the sensing enhancement mechanism of the NiO-WO3 nanocubes is also discussed, which is related to the formation of hetrojunction at interface and the high catalytic activity of NiO.
Preparation of Imm-Fe3+-IL with Peroxidase Activity and Its Colorimetric Determination of H2O2 and Glucose
YU Changmu , ZHANG Rong , LU Xiaoluan , YANG Min , PENG Qianrong
2020, 37(10): 1211-1220  doi: 10.11944/j.issn.1000-0518.2020.10.200064
[Abstract](609) [FullText HTML] [PDF 941KB](3)
Abstract:
The Imm-Fe3+-IL nanomaterials prepared by the sol-gel method have peroxidase-like activity, which can catalyze the rapid oxidation of 3, 3', 5, 5'-tetramethylbenzidine (TMB) with hydrogen peroxide (H2O2) to produce corresponding color changes. The steady-state kinetic analysis shows that the catalytic kinetics of Imm-Fe3+-IL follows the typical Michaelis-Menten model, and the Ping-Pong mechanism. Compared with horseradish peroxidase (HRP), Imm-Fe3+-IL nanomaterials have stronger affinity. Combined with glucose oxidase, a colorimetric detection method for H2O2 and glucose is established. The results show that the concentration of H2O2 and glucose shows a good linear relationship with the absorbance of the reaction system. The linear range of H2O2 is 1~200 μmol/L, the linear range of glucose is 10~200 μmol/L, and the limits of detection (LOD) are 0.35 and 3.31 μmol/L for H2O2 and glucose, respectively.
Address:Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888
Powered By info@rhhz.net