CHEMOSPHERE
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2022
·
IF 8.943
Qingyi Zeng,Jing Tan,Beibei Gao,Tao Cai,Qingyan Zhang,Yi-Lin Liu,Sheng Chang,Shuaifei Zhao,Suqing Wu
A cobalt (Co)-doped perovskite molybdenum trioxide (α-MoO 3 ) catalyst (Co-MO) was synthesized by a facile pyrolysis strategy and used for degrading various organic contaminants via peroxymonosulfate (PMS) activation. The doped Co was inserted in the inter space between the octahedron [MoO 6 ], facilitating the growth of the α-MoO 3 crystal on the [010] direction. This unique structure accelerated the activation of PMS as the Co-MO could function as a carrier for electron transfer to facilitate the Co(II)/Co(III) cycle in the Co-MO/PMS system. As a result, the Co-MO/PMS system showed noticeable activity for removing 100% bisphenol A (BPA) under a broad conditions within 30 min. The radical quenching test and electron paramagnetic resonance analysis revealed that singlet oxygen ( 1 O 2 ) was the main active species for BPA degradation in the Co-MO/PMS system, while free radicals, such as O 2 •- , SO 4 •- and •OH, were also produced as the intermediate species. Furthermore, the carrier mechanism may enable the Co-MO/PMS system maintain relatively high performance during repeat use, and also excellent adaptability was revealed by the well function in various water matrices and high activity in degrading various refractory organic pollutants. Our findings pave a useful avenue for the rational design of novel cobalt-doped catalysts with high catalytic performance toward wide environmental applications.
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Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 4
·778-783
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IF 5.2
Huan Liu,Yi-Xuan Yao,Hong-Yan Shang,Da Yang,Yuan-Yu Tian
The tandem hydroformylation–acetalization of olefins with H2O as the hydrogen source was accomplished over an Ir(I)-catalyst using the phased warming strategy. Due to the release of protons by AlCl3-hydrolysis equilibrium, the tandem reaction was significantly enhanced. The conversion of 1-hexene was 100% and the selectivity for oxo-products was 89%, where 91% of acetals was obtained. Moreover, the hydrogenation by-products were detected to be less than 3%, showing that H2O as the hydrogen source inhibited the hydrogenation of olefins in this tandem reaction. Moreover, isotope-labeling experiments confirmed that water was the hydrogen source, and the key Ir–H active species for hydroformylation were captured by high-pressure 1H NMR spectroscopy analyses.
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ADVANCED MATERIALS
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2019
·Vol. 31
·期 11
·1808341
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IF 25.809
Wanbing Gong,Yue Lin,Chun Chen,Mohammad Al-Mamun,Hai-Sheng Lu,Guozhong Wang,Haimin Zhang,Huijun Zhao
Biomass is the most abundant renewable resource on earth and developing high-performance nonprecious selective hydrogenation (SH) catalysts will enable the use of biomass to replace rapidly diminishing fossil resources. This work utilizes ZIF-67-derived nitrogen-doped carbon nanotubes to confine Co nanoparticles (NPs) with Co–N x active sites as a high-performance SH catalyst. The confined Co NPs with Co–N x exhibit excellent catalytic activity, selectivity, and stability toward a wide range of biomass-derived compounds. Such active sites can selectively hydrogenate aldehyde, ketone, carboxyl, and nitro groups of biomass-derived compounds into value-added fine chemicals with 100% selectivity. The reported approach could be adopted to create other forms of catalytically active sites from other nonprecious metals.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yunfeng Hu,Shi Wu,Yong He,Liehua Deng
A redox prodrug consisting of camptothecin-conjugating PEG through the diselenide bond was synthesized, and the resultant amphiphilic prodrug was then used to load the curcumin to form the co-delivery system for the synergetic B16 melanoma cells inhibition. The co-delivery system showed a good response to glutataione, and the prodrug could be degraded and the two loaded drugs were then released. Both camptothecin and curcumin could induce the obvious cytotoxicity to B16 melanoma cells. Particularly, the co-delivery strategy showed a synergetic inhibition effect to B16 melanoma cells through an in vitro assay. In vivo assay also showed that the co-delivery system could inhibit B16 tumor growth and showed much better inhibition effect than that of only camptothecin or curcumin used. Moreover, as an injectable drug delivery system, the biocompatibility including the blood compatibility of the co-delivery system was confirmed, suggesting that the redox co-delivery system have a potential application in B16 tumor therapy.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2019
·Vol. 411
·期 7
·1375-1381
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IF 3.286
Sun Chongmei,Shen Jin,Cui Rongwei,Yuan Fangzheng,Zhang Hui,Wu Xia
A sensitive fluorescent analytical method for the detection of dopamine (DA) was developed based on surface-enhanced Tb(III)/La(III) co-luminescence using silver nanoflowers (AgNFs). Anisotropic AgNFs show strong surface-enhanced fluorescence effect owing to the abundant sharp tips. Tb(III)/La(III)-DA complexes mainly bind to the sharp tips of AgNFs and thus shorten the distance between the complexes. The shortened distance gives rise to obvious surface-enhanced Tb(III)/La(III) co-luminescence effect. In this work, AgNFs offer many superior properties, such as enhanced intrinsic green fluorescence of Tb(III) ( λ ex / λ em = 310/546 nm), increased fluorescence lifetime, and improved energy transfer efficiency. Under the optimum conditions, the fluorescence intensity is linearly correlated with the concentration of DA in the range of 0.80–10 nM ( R 2 = 0.9970), and the detection limit is 0.34 nM ( S/N = 3). The fluorescent nanoprobe was successfully applied to the determination of DA in human serum samples with recoveries ranging from 99.1 to 102.6%.
Graphical abstract
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TALANTA
·
2019
·
IF 4.916
Li Su,Xinai Yu,Yuqi Miao,Guojiang Mao,Wenpei Dong,Suling Feng,Siman Liu,Like Yang,Kaige Zhang,Hua Zhang
Nanozymes’ activities could be regulated by a simple and effective pH change in an in situ manner. In this work, for the first time, the peroxidase-like activity of Ni/Co layered double hydroxides (LDHs) was regulated via the alkaline-promoted reaction of fluorogenic substrate homovanillic acid and H 2 O 2 , and a promising tool for pH sensing was developed over the pH range of 8.3–9.6. As peroxidase nanozyme model, Ni/Co LDHs showed ease of preparation, low-cost, and water-solubility, which played an important role in this luminescence system. Based on the pH-dependent regulation of the Ni/Co LDHs activity, we constructed the bioassay platform for the determination urea, urease, penicillin G, and penicillinase with a wide linear range of 17–1000 µM, 3.3–270 mU mL −1 , 3.3–1300 µM and 3.3–100 mU mL −1 , respectively. This study not only demonstrated the alkaline-promoted modulation the nanozymes’ activities, but also established a facile approach to develop novel bioassays.
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SOLID STATE IONICS
·
2019
·
IF 2.886
Hengxu Song,Yuhong Zhao,Yongqiang Niu,Hua Hou
Medium-temperature molten salt reserve primary cell utilizes low-melting nitrate electrolyte, that is considered suitable for geothermal borehole as well as oil and gas exploration . In this work, Cr 3+ and F − ions were introduced into spinel lithium manganate oxides by high-temperature solid-state method and verified by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The effects of fluorine content on the morphology and discharge performance of the LiCr 0.1 Mn 1.9 O 4− x F x (0 ≤ x ≤ 0.5) have been studied in LiCr 0.1 Mn 1.9 O 4− x F x /LiNO 3 -KNO 3 -Ca(NO 3 ) 2 /Li-Mg-B system. Fluoride-doped samples have a significant improvement in discharge performance at the condition of 10 mA·cm −2 and 250 °C because of the stabilization of the crystal structure. Factors of operating temperature and current density have a significant effect on battery discharge performance, and the surroundings of 10 mA·cm −2 and 200–250 °C contributes the battery to achieve high performance. That indicates the LiCr 0.1 Mn 1.9 O 4− x F x /LiNO 3 -KNO 3 -Ca(NO 3 ) 2 /Li-Mg-B battery shows great potential in geothermal borehole as well as oil and gas exploration environment.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2019
·Vol. 30
·期 7
·6469-6474
·
IF 2.195
Ullah Atta,Liu Hanxing,Pengcheng Zhai,Hao Hua,Iqbal Javed,Cao Minghe,Yao Zhonghua,Ahmad Arbab Safeer,Manan Abdul
Solid-state sintering method was used for the synthesis of Mg 1−x Co x SiO 3 (x = 0–0.25) ceramics. Phase, microstructure and microwave dielectric properties of the ceramics were investigated. With increase in Co 2+ content, the increase was observed in the lattice parameters. The Q u f o value of MgSiO 3 was enhanced from 103,453 to 145,846 GHz with increasing the value of x content from 0 to 0.15. The Co 2+ substitution also led to an obvious decrease in the sintering temperature by ~ 100 °C. Clino-enstatite phase formed for the composition with x = 0 while Proto-enstatite formed as the major along with minor clino-enstatite phase for the compositions with x > 0. Good dielectric properties at microwave frequencies i.e. ε r ~ 8.11, Q u f o ~ 145,846 GHz and τ f ~ − 12 ppm/°C were obtained for the composition with x = 0.15 sintered at 1350 °C for 9 h. This is suggested to be a very favorable dielectric material for millimeterwave applications.
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FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Tao Xie,Jing-Pei Cao,Chen Zhu,Xiao-Yan Zhao,Ming Zhao,Yun-Peng Zhao,Xian-Yong Wei
Selectively cleaving the C O bonds in lignin to produce aromatic products are challenging problems. Currently, catalytic hydrogenolysis of C O bonds in lignin requires harsh conditions. Herein, selectively cleaving C O bond of benzyl phenyl ether (BPE) was studied over Pd/AC, Ru/AC and Ni/AC. Among these catalysts, Pd/AC efficiently cleaved C O bond in BPE under super mild conditions (25 °C, 2 h and 0.1 MPa H 2 ). The products were toluene and phenol without hydrogenation of the aromatic ring . The main competitive step of hydrogenolysis and hydrogenation is sensitive to reaction temperature over Pd catalyst. A mild temperature is preferred for hydrogenolysis, since the H species nearby the oxygen atom are more strongly adsorbed than nearby the benzene rings . With the different H-donor solvents, the highest conversion of BPE was obtained in isopropanol. Based on the experiments, the reactions occurred via cleavage of the C aliphatic -O bond in BPE and the synergetic effects between the H from absorbed H 2 on the surface of the Pd and the intermediates radicals of benzyl and phenoxy should be the key points to such an optimum result.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Xudan Li,Hanwei He
Cobalt hydroxide nanosheets/ruthenium oxide (Co(OH) 2 /RuO 2 ) nanocomposite on nickel foam was successfully synthesized via a simple electrodeposition process as an advanced supercapacitor electrode material. The microscopy studies reveal that RuO 2 nanoparticles are loaded uniformly on interconnected Co(OH) 2 nanosheets forming a three-dimensional (3D) network. The performance optimization of composite is come true through adjusting deposition time of RuO 2 nanoparticles. The electrochemical tests indicate that the optimized Co(OH) 2 /RuO 2 nanocomposite displays excellent super-capacitive properties. The specific capacitance is up to 2168 F g −1 as the current density is 1 A g −1 . Compared with the pure Co(OH) 2 and RuO 2 , the capacitance of the Co(OH) 2 /RuO 2 composite increases by 57% and 80%, respectively. The capacitance maintains at 86.0% after 5000 charging and discharging loops at the constant current density of 5 A g −1 , while the pure Co(OH) 2 only maintains 71.7% of the original capacitance after 5000 loops. The asymmetric capacitor assembled using Co(OH) 2 /RuO 2 nanocomposite as positive electrode and activated carbon (AC) as negative electrode exhibits a high energy density of 58.4 W h kg −1 at a power density of 1.2 kW kg −1 . The good pseudocapacitance behavior of the Co(OH) 2 /RuO 2 composite is mainly in virtue of the good synergies between Co(OH) 2 and RuO 2 insuring large surface area, rich electrochemical reactive sites, the short diffusion pathways of ions and good electroconductivity during the charge-discharge process.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2018
·
IF 4.841
Yuxiang Cai,Xinbo Zhu,Wenshuo Hu,Chenghang Zheng,Yang Yang,Menghan Chen,Xiang Gao
Plasma-catalytic decomposition of low concentration ethyl acetate with LaMO 3 (M = Co, Mn and Fe) perovskite catalyst was investigated in a coaxial dielectric barrier discharge (DBD) reactor. The combination of perovskite catalyst and plasma enhanced ethyl acetate decomposition, and the activity sequence was LaCoO 3 > LaMnO 3 > LaFeO 3 . Characterizations results indicated that the activation of surface oxygen species and amount of oxygen vacancies contributed to ethyl acetate decomposition remarkably. FT-IR analysis demonstrated that the employment of LaCoO3 catalyst also reduced the amount of unwanted by-products. Based on these results, reaction mechanism of ethyl acetate plasma-catalytic decomposition process was proposed.
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Nano Energy
·
2018
·
IF 13.12
Qirui Liang,Huihui Jin,Zhe Wang,Yuli Xiong,Shuai Yuan,Xianci Zeng,Daping He,Shichun Mu
Developing low-cost, highly active, and stable bifunctional electrocatalysts is a challenging issue in electrochemical water electrolysis . Herein, we develop a simple metal organic frameworks (MOFs) based approach to prepare bifunctional Co-NC@ Mo 2 C complex catalysts. Differently from traditional carbon encapsulated functional nanomaterials , herein the carbon-based framework derived carbonitride and Co nanoparticles (Co-NC) are encapsulated with Mo 2 C. Benefiting from the unique reverse-encapsulation structure and synergetic effects of Mo 2 C and Co-NC, the Co-NC@Mo 2 C catalyst shows superior hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance. In alkaline media , it affords the current density of 10 mA cm −2 at low overpotentials of 99 mV and 347 mV for HER and OER, respectively. Interestingly, due to a reversed encapsulation structure where Co nanoparticles are protected by Mo 2 C, it leads to an outstanding HER catalytic activity (a low overpotential of 143 mV) and stability in acidic solutions. Remarkably, when employed as both the cathode and anode for overall water splitting, a low cell voltage of 1.685 V is required to reach the current density of 10 mA cm −2 in alkaline media with excellent stability, making the Co-NC@Mo 2 C an efficient non noble metal bifunctional electrocatalyst toward water splitting.
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