Green Energy & Environment
·
2020
·
IF 6.395
Zhaoning Song,Juncong Yuan,Zhenping Cai,Dong Lin,Xiang Feng,Nan Sheng,Yibin Liu,Xiaobo Chen,Xin Jin,De Chen,Chaohe Yang
The advocacy of green chemical industry has led to the development of highly efficient catalysts for direct gas-phase propene epoxidation with green, sustainable and simple essence. The S-1/TS-1@dendritic-SiO 2 material with three-layer core–shell structure was developed and used as the support for Au catalysts, which showed simultaneously fantastic PO formation rate, PO selectivity and stability (over 100 h) for propene epoxidation with H 2 and O 2 . It is found that silicalite-1 (S-1) core and the middle thin layer of TS-1 offer great mass transfer ability, which could be responsible for the excellent stability. The designed dendritic SiO 2 shell covers part of the acid sites on the external surface of TS-1, inhibiting the side reactions and improving the PO selectivity. Furthermore, three kinds of SiO 2 shell morphologies (i.e., dendritic, net, mesoporous shell) were designed, and relationship between shell morphology and catalytic performance was elucidated. The results in this paper harbour tremendous guiding significance for the design of highly efficient epoxidation catalysts.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Haoran Wang,Wenjun Cai,Shun Wang,Baozong Li,Yonggang Yang,Yi Li,Qi-Hui Wu
Helical silica nanofibers have been prepared based on a sol-gel transcription approach. After covering a layer of m-phenylenediamine formaldehyde resin and consequent carbonization , SiO 2 @Fe–N doped C nanofibers with C content of 33.7 wt% and N content of 3.86 wt% were produced successfully. When applied as the electrode material for lithium-ion batteries (LIBs), they exhibit a high reversible capacity of 1274 mA h g −1 in the 1000th cycle and superior rating capability, implying the possibility as outstanding candidate anode materials for LIBs. Additionally, owing to the doping of Fe 2 O 3 and N, the nanofibers also exhibit a well-performed oxygen reduction reaction activity, which is comparable to the commercial Pt/C catalyst.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 6
·1-9
·
IF 6.232
Qin Peige,Zhu Wenli,Han Lizhen,Zhang Xiaowan,Zhao Bing,Zhang Xuebin,Lu Minghua
The monodispersed mesoporous SiO 2 @metal-organic framework (MSN@MIL-101(Fe)) composites were prepared by grafting MSN-NH 2 onto MIL-101(Fe) particles with a solvothermal method. The adsorption ability of the composites was greatly improved compared to that of pristine MSNs or MIL-101(Fe) for phytohormones (Phys). The MSN@MIL-101(Fe) composites were characterized by scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, energy dispersive spectrometer, and mapping analysis. Using MSN@MIL-101(Fe) composites as sorbent, a dispersive solid-phase extraction procedure (dSPE) was developed to extract three endogenous Phys (abscisic acid (ABA), indole-3-aceticacid (IAA), and indole-3-butyric acid (IBA)) and two exogenous Phys (1-naphthylacetic acid (1-NAA) and 2-naphthylacetic acid (2-NAA)) prior to HPLC-DAD analysis. The experimental parameters including sample volume, sorbent amount, adsorption time, adsorption pH, desorption time, and desorption solvent on extraction efficiency were optimized and evaluated. Under optimized conditions, the working range of 0.08 to 0.45 ng mL −1 with enrichment factors from 144 to 207 were achieved. The linear range is 0.75–200 ng mL −1 for IAA, 0.20–200 ng mL −1 for ABA, and 1.0–200 ng mL −1 for IBA, 1-NAA, and 2-NAA. With MSN@MIL-101(Fe) as sorbent for extraction of Phys and determination by HPLC-DAD, two endogenous Phys (IAA and ABA) were detected from mung bean sprouts which were made in a laboratory, and the results were further confirmed by high-resolution mass spectrometry. The composites can be applied to extract other small molecules, which have similar chemical structures with Phys in biological, environmental, and food samples.
Schematic presentation of a dispersive solid-phase extraction using monodispersed mesoporous SiO 2 @metal-organic framework composites (MSNs@MIL-101(Fe)) as the sorbent for extraction, clean-up, and preconcentration of phytohormones in mung bean sprouts prior to HPLC-DAD analysis.
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 15
·5149-5162
·
IF 5.721
Tongyang Song,Wei Chen,Yuanyuan Qi,Jiqing Lu,Peng Wu,Xiaohong Li
Achieving high catalytic performance with Cu-based catalysts is crucial for the hydrogenation of CO2-derived ethylene carbonate (EC) to simultaneously yield methanol (MeOH) and ethylene glycol (EG). Although Cu-based catalysts are widely studied for the target reaction, there are still some issues to be clarified. In this study, we prepared a 29.1 wt% Cu/SiO2-MHT catalyst by a modified hydrothermal method and successfully applied it to the hydrogenation of EC. In comparison with its three analogues having similar Cu loading and comparable Cu particle size but prepared by different methods, we found that the catalytic performance of the Cu/SiO2 catalysts, including the activity and the selectivity to MeOH, could be tuned by adjusting the Cu+/(Cu0 + Cu+) ratio via different preparation methods. As a result, the Cu/SiO2-MHT catalyst furnished 89% MeOH yield and 37.6 h−1 turnover frequency. To our best knowledge, these values are one of the highest among all heterogeneous Cu catalysts up to now. The results reveal that a cooperative effect exists between Cu0 and Cu+. When the Cu0 species are sufficient to activate H2, a more favorable formation of MeOH can be achieved with more Cu+ species and greater Cu+ surface areas. Furthermore, a greater amount of Lewis acid on the Cu/SiO2-MHT catalyst is also beneficial for MeOH formation.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Pengpeng Zhang,Chao Xue,Yukun Li,Shuaiwei Guo,Xilai Zhang,Peng Zhang,Guosheng Shao
High-efficiency light utilization and prolonged lifetime of photo-induced charge carriers is a key step towards superior photocatalytic H 2 evolution. Herein, the design of a novel spatially separated Ni 2 P co-catalyst decorated SiO 2 /rGO/Cd 0.5 Zn 0.5 S yolk-shell structural photocatalytic nanoreactor is reported. In this system, the advantages of ultrathin mesoporous shell and yolk-shell structure not only facilitate the mass diffusion with short length, but also allow broad-spectrum light absorption and increase the density of catalytic active sites. Importantly, the photo-generated electrons can be directionally injected from the outermost Cd 0.5 Zn 0.5 S shell to the spatially separated Ni 2 P co-catalyst. The dynamic behaviors of photo-induced charge carriers can be rationally regulated by the suitable energy level alignment and the built-in electric fields derived from both sides of embedded rGO interlayer. The synergistic effects of the excellent light-harvesting ability, more exposed active sites and improved charge separation efficiency significantly boosted the photocatalytic performances of hydrogen evolution. As a result, the optimal SiO 2 /Ni 2 P/rGO/Cd 0.5 Zn 0.5 S composite exhibited the highest hydrogen generation of 11.65 mmoL‧g −1 ‧h −1 , even after five cycles. This work proposes new insights into the design of the efficient hollow sphere structural heterojunctions for photocatalytic water splitting applications.
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ENERGY
·
2020
·
IF 6.082
Jie Ding,Xiaodong Wu,Xiaodong Shen,Sheng Cui,Xiangbao Chen
In this work, palmitic acid (PA) is used as the PCM , while a novel kind of 3D porous carbon/silica composite aerogel (CSA) is involved as porous supporting material to prepare the form-stable PCM composites (PA/CSA). The carbon aerogel supported PCM composite (CA/PA) is provided as control. PCM infiltration mainly occurs for the large pores rather than micropores or mesopores. PA molecules are physically well combined with CA and CSA due to capillary force and surface tension. The addition of amorphous CA and CSA limits the crystalline growth of PA molecules. The CA/PA shows a separated and layered structure while the CSA/PA presents a CSA@PA core-shell structure with a rough surface due to large pores within the CSA pore matrix. The PCM loading mass fraction of CSA/PA (82.2%) is much larger than that of CA/PA (64.1%), and liquid leakage test indicates its excellent form-stabilization property. The melting point and melting latent heat of CA/PA sample is 39.73 °C and 96.27 J/g, respectively, while the melting latent heat of the CSA/PA sample is as high as 187.7 J/g. The CSA/PA possesses excellent thermal stability during cycling test and its short-term thermal insulation property has also been verified in this study.
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IONICS
·
2019
·Vol. 26
·期 2
·639-648
·
IF 2.289
Tang Jie,Dai Xinyi,Wu Fuzhong,Mai Yi,Wang Xiao,Jin Huixin,Gu Yijing,Xie Yanfang
Materials with nanotubular structure have attracted wide attention in electrochemical energy storage due to their good structural stability, high specific surface area, and internal and external wall activity. Here, we report a simple and efficient one-pot method for the synthesis of SiO 2 nanotubes with controlled aspect ratios. The influence of parameters, such as the monomer concentration and reaction time on the aspect ratio, were inspected systematically. The results confirmed that the aspect ratio of SiO 2 nanotubes increases with the reaction time before tetraethyl orthosilicate is added, and the length of SiO 2 nanotubes can also be altered by tuning the hydrazine hydrate/NiCl 2 ratio. The SiO 2 nanotubes as an anode material for lithium-ion batteries exhibited an initial discharge capacity of 625.5 mAh g −1 and maintained 232.5 mAh g −1 after 100 cycles at 40 mA/g, which is 75.7% relative to the second cycle, showing good electrochemical performance.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Nian Cao,Faqiong Zhao,Baizhao Zeng
In this work, a novel self-enhanced solid state electrochemiluminescence (ECL) platform, based on polyethyleneimine (PEI) capped CdS quantum dots (PEI-CdS QDs) as coreactant and [email protected] 2 @Ru(bpy) 3 2+ doped silica ( [email protected] 2 @RuDS) nanocomposite as ECL emitter, was constructed. The PEI-CdS QDs integrated double coreactant of PEI and CdS QDs, thus significantly promoted the ECL of [email protected] 2 @RuDS. Polyaniline hydrogel was introduced to boost the electron transfer and to improve the immobilization of PEI-CdS/ [email protected] 2 @RuDS. In addition, creatinine imprinted poly(o-aminophenol) film was electrodeposited on the PEI-CdS/ [email protected] 2 @RuDS surface as recognition element. Thus, the obtained sensor possessed high sensitivity, stability, reproducibility and selectivity for creatinine sensing. The change of ECL intensity and logarithm of creatinine concentration showed a good linear relationship in the range of 0.05 nM to 5 μM, and the detection limit was low to 0.02 nM. The sensor was applied to detect creatinine in human serum and urine samples, and the results were in good agreement with those of commercial enzyme-linked immunosorbent assay kit.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 11
·1-11
·
IF 6.408
Zhang Jing-Xian,Lv Chun-Lin,Tang Chang,Jiang Lu-Yao,Wang Ai-Jun,Feng Jiu-Ju
Squamous cell carcinoma antigen (SCCA) is one of the common squamous cell carcinomas (SCC) in women, which usually works as a tumor biomarker for cervical cancer in diagnostic applications. Herein, bimetallic PtCo highly branched nanocrystals (PtCo BNCs) acted as electrode substrates to construct sandwich-typed electrochemical immunosensor for ultrasensitive detection of SCCA, by using dendritic mesoporous SiO 2 @AuPt nanoparticles (DM-SiO 2 @AuPt NPs) to adsorb electroactive thionine (Thi) as a signal label. The PtCo BNCs enlarged the loading of the primary antibody (Ab 1 ), showing effective improvement in conductivity and sensitivity. The DM-SiO 2 had abundant pores to incorporate more Thi, on which the decorated AuPt NPs created a great number of active sites to immobilize the secondary antibodies (Ab 2 ), thereby obviously amplifying the detection signals. The prepared sensor exhibited a broader linear range (0.001–120 ng mL –1 ) and a lower detection limit (0.33 pg mL –1 , S / N = 3), combined with high reproducibility, a low relative standard deviation (below 2.5%) and acceptable recovery (from 98.5 to 110.0%) even in diluted human serum samples. This research provides a substantial platform for clinical diagnosis of SCCA in practice. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lifang An,Jie Fan,Buhuan Wang,Jingyi Yang,Guolian Wang,Meng Zhang,Zhongyi Liu
Ru/Fumed SiO 2 achieves 100% DMT conversion and 100% DMCD selectivity. • Macropores of Fumed SiO 2 lower diffusion barriers and enhance active site utilization. • Strong Ru-O-Si interaction promotes Ru dispersion and ensures 5-cycle reusability. • Low apparent activation energy enables high-efficiency aromatic ring hydrogenation. The growing accumulation of waste polyethylene terephthalate (PET) causes severe resource depletion and environmental pollution, making its high-value chemical recycling essential for sustainable development. PET methanolysis affords dimethyl terephthalate (DMT), and its selective hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate (DMCD) connects waste PET valorization with high-performance polyester synthesis. Herein, a series of Ru-based catalysts supported on microporous-dominated S-1, ordered mesoporous MCM-41 and SBA-15, and Fumed SiO 2 with the open interparticle macro-mesoporous were prepared by the incipient wetness impregnation, and the role of support pore structure in DMT hydrogenation to DMCD was systematically examined. The results show that the open interparticle macro-mesoporous framework of Fumed SiO 2 alleviates diffusion constraints and improves the accessibility of Ru active sites. This structure enables uniform Ru dispersion, giving Ru/Fumed SiO 2 the smallest average Ru particle size (6.0 nm). Surface Si-OH groups anchor Ru species through Ru-O-Si interfacial structures, which strengthens metal-support interactions and promotes H 2 activation and active-site utilization. Under 180 °C, 3.0 MPa H 2 , and 3 h, Ru/Fumed SiO 2 delivers 100% DMT conversion and 100% DMCD selectivity. It also shows the lowest apparent activation energy (39.0 kJ·mol −1 ), stable performance over five cycles, and over 93% conversion and selectivity for representative substituted aromatic compounds. These findings demonstrate that an open interparticle macro-mesoporous framework could improve molecular accessibility, mitigate mass-transfer limitations, and enhance hydrogenation efficiency. Download: Download high-res image (185KB) Download: Download full-size image
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Surfaces and Interfaces
·
2023
·
IF 6.2
Kun Wan,Chao Mei,Wei Liu,Xuebin Zhang,Zhongqiu Zou,Hailin Su
Optimizing dense insulating shells plays a crucial role in developing high-frequency soft magnetic composites (SMCs) working in acidic and salty environments. Herein, raspberry-like and litchi-like SiO 2 shells are fabricated on FeNi particles by using both 3-aminopropyl triethoxysilane (APTES) and tetraethyl orthosilicate. It is found that low dosages of APTES lead to raspberry-like shells consisting of internal SiO 2 layer and attached SiO 2 particles. While high dosages of APTES result in litchi-like shells, owing to a much higher coordinated growth rate between the inner layer and SiO 2 particles. With regard to corrosion resistance performance, the litchi-like shell contributes to a more positive corrosion potential of -0.076 V, a lower corrosion current density of 2.512 × 10 −6 A/cm 2 , a higher corrosion protection efficiency of 96.70 % and a lower ion concentration in the HCl etching solution. As for magnetic properties, higher resistivity of 1.46 × 10 8 Ω·m, lower eddy current loss with μ′ of 13.98 and lower tan δ of 0.01148 at 2000 kHz can be realized by the dense litchi-like shell structure. This work not only demonstrates detailed growth mechanisms of different SiO 2 shells, provides FeNi SMCs with desirable high frequency and anti-corrosion performance, but also offers deeper insights into functional shell design.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 42
·15353-15359
·
IF 4
Peng Zhang,Liming Chen,Xiaoyan Cai,Binbin Luo,Tianju Chen,Haini Chen,Guoliang Chen,Feiming Li
A traditional fluorescence–scattering intensity based ratiometric sensing system utilizes both inherent scattering and fluorescence intensity and has drawn extensive attention owing to its simplicity and self-calibration properties. In this work, we propose a novel ratiometric fluorescence sensing system that combines a fluorescence wavelength shift and scattering in a single window, using second-order scattering (SOS) as the representative scattering signal based on the halide exchange of CsPbBr3@SiO2 perovskite nanocrystal composites. We observe a fast halide exchange within 10 seconds, resulting in an identifiable fluorescence wavelength blue shift, while the scattering wavelength remains relatively constant for self-correction. This system could be applied for ratiometric sensing of Cl− in the serum without any sample treatment. The established wavelength-based ratiometric system demonstrates high reliability and reproducibility, paving a new way for fluorescence sensing.
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