Bimetallic metal-organic framework (MOF) has attracted great interest as an electrode for supercapacitors. Most metal sources are limited to valences of + 2 and + 3. We select metal sources of Co (II) and Mo (VI) and demonstrated a crystalline bimetallic MOF precursor prepared by using a facile chemical synthesis. The one-step solvothermal strategy is assisted by thioacetamide (TAA) for the self-assembly Co-Mo-S nanosheet arrays (Co-Mo-S NSAs). TAA-induced etching is essential to regulate the assembly of amorphous structures. Otherwise, only a single-structure crystalline Co-Mo-S could be obtained. The Co-Mo-S NSAs show a large specific capacitance of 1805.28 F g(-1) at a current density of 0.5 A g(-1). A Co-Mo-S NSAs//AC battery-supercapacitor hybrid (BSH) make with activated carbon as the negative electrode and Co-Mo-S NSAs as the positive electrode. At a current density of 0.5 A g(-1), the BSH shows a high energy density of 169.73 Wh kg(-1) and a power density of 371.44 W kg(-1). After 50,000 cycles, the capacitance retention rate is as high as 94.44%, showing good reversibility and cycle life. This work provides an effective strategy for manufacturing bimetallic MOF-based metal sulfide heterostructure electrode materials for practical energy storage and conversion. (C) 2022 Elsevier B.V. All rights reserved.
Noble metal-based catalytic material with maximum utilization is of prime attraction for conserving rare metal resources. Herein, highly dispersion Ni nanoparticles (NPs)-modified N-doped mesoporous carbon material (Ni-N@C) was fabricated by pyrolysis of Ni2+/Histidine cross-linked alginate hydrogels. In a step forward, the obtained Ni-N@C nanocatalyst was treated by the solution of Pd2+, and tiny amount of Pd NPs were deposited on the surface of Ni via the reducibility of Ni to achieve the high dispersion of precious metals material. In the degradation of highly-concentration p-nitrophenol, the catalyst presents excellent performance which could completely degrade pollutants within a very short period. It was demonstrated that pre-embedded Ni NPs could not only increase the efficiency of Pd NPs but also endow the facile separation characteristic to the catalyst. Besides, the catalyst maintained favorable catalytic capacity even after five reaction cycles. In brief, this work may provide novel guidance for the maximum utilization of noble metal-modified mesoporous N-doped carbon-supported catalysts in practical applications of industrial and the treatment highly-concentration p-nitrophenol.
The fabrication of the advanced MOF-based 3D hollow cage ternary bimetallic material CuCo2S4 for high performance asymmetric supercapacitors.
In this work, a Ni/KIT-6 catalyst with the highly uniform Ni dispersion was synthesized by a facile methanol-assisted co-impregnation technique and its activity towards to CO2 reforming of renewable ethanol was depicted for syngas production and CO2 elimination. Herein, its physicochemical features were determined in detail by various characterization technique including XRD, TPR, Raman, SEM and TEM etc. The results revealed the presence of the smaller Ni particles and the stronger Ni-support interaction in the Ni/KIT-6 catalyst compared to the reference Ni/SiO2 sample. More importantly, Ni/KIT-6 catalyst showed the satisfactory activity and stability while a rapid deactivation was noted for Ni/SiO2. Typically, full ethanol conversion was obtained at 550 degrees C for Ni/KIT-6 and no obvious deactivation was observed after 40 h tests. Indeed, this superior behavior was related to the confinement effect of KIT-6 channels which could stabilize Ni particles under the severe reaction conditions. On the other hand, the smaller Ni species greatly inhibited the coke deposition, especially for the encapsulated carbon. Moreover, the existence of strong Ni-support interaction was also responsible for the anti-sintering of active metal and carbon accumulation. This attractive results might be helpful to design high efficient Ni-based catalysts for chemical conversion of the undesirable CO2. (c) 2019 Elsevier Ltd. All rights reserved.
Catalytic production of structured phospholipids (SPLs) containing short-chain fatty acids (SCFAs) in an efficient heterogeneous manner is of great importance from the standpoint of food engineering. Herein, a bifunctionalized sulfonated Zn-SBA-15 catalyst was studied for SPL synthesis through interesterification of soybean lecithin with ethyl propionate or methyl butyrate. Various characterization techniques such as pyridine Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and ultraviolet-visible diffuse reflectance spectroscopy were conducted to determine the physicochemical properties, so as to build the possible structure-reactivity relationship of the catalyst. In screening tests with commercial Amberlyst-15 or other SBA-15-type materials, the as-prepared sample showed promising catalytic performance probably owing to its mesoporous structure and cooperative role of Brönsted and Lewis acid sites. Notably, the sample was easily separated and recycled without obvious deactivation. In general, the investigated catalyst was regarded as one of the promising alternatives to otherwise expensive biocatalysts for SCFA-containing SPL production.
A CuCeZr composite oxide (Cu-Ce0.8Zr0.2O2) was prepared via microwave-assisted co-precipitation method and employed in syngas production from dry reforming of renewable ethanol. Its physicochemical features were deeply investigated by a series of characterization technique (XRD, Raman, TPR, SEM and XPS etc). Indeed, the as-prepared composite oxide presented the flower-like morphology structure and exhibited the superior activity and stability even after 50 h on-stream tests for ethanol dry reforming. This attractive behavior was probably assigned to the uniform dispersion of active Cu species and the strong metal-support interaction which could not only efficiently stabilize Cu nanoparticles during the serious reaction conditions but suppress the deactivated coke formation over catalyst surface. The promising findings in this work might stimulate the development of value-added syngas production from renewable biomass-derived feedstocks. (C) 2020 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.
综述了生物法合成烷基糖苷,包括糖苷酶选择、酶促糖苷化、烷基糖苷的酶促合成等几个方面.与传统化学合成法相比,烷基糖苷的酶促合成提供了极好的环保升级替代方案,具有较大的利用潜能和广阔前景.未来烷基糖苷的酶促合成可以通过开发新型基因工程菌,采用全细胞催化的方法,进行工业化放大研究.
Selective and ultrasorption materials are of practical significance in the fields of rare earth element (REE) capturing and heavy metal (HM) remediation. Here, we exploited ion-imprinted engineering, which was based on a watermelon-inspired strategy. This type of engineering was first coupled with renewable alginate biomacromolecules. The imprinted target metal ions could be optionally changed and recovered for different purposes. La and Pb cations were selected as the representatives for REE and HM to demonstrate the tunable adaption. Sodium alginate is cost-effective and environment-friendly biomass and is thus frequently used as a carbon source or matrix in materials science. Some other high-performance metal-incorporated functional materials for catalysis and microwave shielding might also be synthesized facilely under our engineering. Metal sources for the abovementioned composites might be selectively extracted from natural metal-bearing solution or industrial wastewater by selecting specific target metals.
Dopamine-derived cavities/Fe3O4 nanoparticles-encapsulated carbonaceous composites with self-generating three-dimensional (3D) network structure were successfully fabricated by a facile synthetic method, in which sodium alginate provided carbon matrix pores and excellent microwave absorption performance was established. The hollow cavities derived from the core-shell-like CaCO3@polydopamine were creatively introduced into the 3D absorber to significantly improve the absorption performance. The sample calcined at 700 °C exhibited the most outstanding microwave absorption performance, with minimal reflection loss up to -50.80 dB at 17.52 GHz with a rare thickness of only 1.5 mm when filler loading was 35% in paraffin matrix. The effective absorption bandwidth of reflection loss < -10 dB reached 3.52 GHz from 14.48 GHz to 18 GHz, corresponding to the same thickness of 1.5 mm. In contrast, the sample without hollow dopamine-derived cavities showed poor performance due to poor impedance matching, and this highlights the role of hollow cavities brought into the 3D structure, which led to a difference in interfacial polarization, multiple reflections and scattering. The novel dopamine-derived cavities/Fe3O4 nanoparticles-encapsulated carbonaceous composites with 3D network structure can be regarded as a promising candidate for application as a microwave absorber with strong absorption.
A sulfonated Sn-doped KIT-6 catalyst (Sn-KIT-6-Pr-SO3H) was successfully prepared via the hydrothermal self-assembly method, and its performance towards to value-added lactic acid production from one-pot conversion of renewable cellulose was investigated. Indeed, the physicochemical features of the as-prepared catalysts were deeply characterized by various techniques, including XRD, BET, SEM, FT-IR, XPS, UV-vis and TGA-DSC. The results confirmed its high BET surface area with an ultrahigh cross-linked framework and promising acid strength (co-existence of Brønsted and Lewis acidity). Additionally, the impact of different reaction factors, such as the type of catalysts, temperature, time, recyclability on cellulose conversion and the yield of targeted lactic acid, were determined. Meanwhile, the developed catalyst depicted the promising activity and stability under the optimal reaction conditions. It could be recycled at least four times without any obvious deactivation. This provides insight into developing efficient catalytic systems to convert renewable biomass into value-added chemicals.
Lead(ii) is one of the most toxic heavy metals and is a serious threat to the environment and human health.
Considering that the hazardous heavy metal ions like Cd(II) and Cr(VI) are widely present in the environment, nowadays employing easy-to-handle adsorption-oriented processes are feasible choices towards efficient remediation of Cd(II) and Cr(VI) from aqueous systems. Herein we developed a novel amino-functionalized bead with cost-effectiveness, high sorption capacity and fast sorption kinetics to remove Cd(II) and Cr(VI) from aqueous solution. The carboxyl methylcellulose and chitosan-derived nanostructured sorbents synthesis were mainly through chitosan and dopamine self-polymerization, doped in sodium carboxymethyl cellulose, and glutaraldehyde cross-linking. The pH value, initial concentration and contact time were investigated. Experimental data were commendably described by Freundlich isotherm and Pseudo-second-order model. The maximum adsorption capacities of Cd(II) and Cr(VI) obtained from the experimental data were 470.0 mg/g and 347.0 mg/g, respectively. The adsorbents were collaboratively characterized by FT-IR, SEM, TGA, XPS, etc., and the adsorbent basically exhibited high complexation ability to Cd(II) and showed strong electrostatic effect with Cr(VI) under acidic conditions. The recycling characteristics suggested that it possesses an outstanding recyclability. The adsorbent may have a potential as high-value biological adsorbent to remove heavy metals and it deserves further research into the practical application.
Short, surface rough carbon rods, which were derived from natural sisal fiber and went through two different modifications, with excellent electromagnetic wave absorption performance, were studied in this work for the first time. The structure-property relationship was clearly established here. It was shown that these green, cheap and easily obtained carbon rods with mass preparation possibility presented eye-catching absorbing behaviors towards electromagnetic wave. Based on the natural structure of sisal fiber, the minimum reflection loss of KOH activated product reached 51.1 dB and the maximum effective absorbing bandwidth achieved 7.88 GHz. The magnetically modified sample presented 48.6 dB of minimum reflection loss and 4.32 GHz of optimal absorbing bandwidth. Its pioneering application in this field not only opens a new road for this traditional textile sisal fiber but also would possibly make a referable contribution to the design and synthesis of superior carbonaceous electromagnetic wave absorption materials based on bioresource.
To our knowledge, the utilization of chitosan-derived materials in microwave absorbing is currently scarce. Herein, for the first time, by fully exploiting its potential properties via facile means, chitosan was employed as the exclusive joint source of carbon and nitrogen, and the inherent N-doped honeycomb-like carbon/Fe3O4 composites with favorable versatility that can efficiently treat microwave interference and even wastewater pollution were controllably prepared. The optimal microwave absorbency is attractive, of which the minimum reflecting loss reaches to -59.5 dB, and the maximum effective absorbing bandwidth is 5.36 GHz when filler content is only 10%. Beyond the major trying, another function for wastewater treatment was also demonstrated by excellent toxic Cr(VI) adsorption and peroxymonosulfate activation for organic pollutants (azo-dye Orange II) degradation. More significantly, the embedding magnetic component makes it convenient to be magnetically separated from the testing solution. Totally, these N-doped honeycomb-like carbon/Fe3O4 composites with versatility prepared by simple methods not only open a new road for the diversified utilization of chitosan but also would possibly make a referrable guidance to the design or even synthesis for superior microwave absorption and environmental remediating materials.
Up to date, selective hydrogenation of undesirable CO2 to value-added chemicals is of great interest. To address this issue, the doped CuZnM (M: Ga, Fe) catalysts were synthesized by a facile microwave-assisted technique and its activity towards to CO2 hydrogenation were evaluated. Indeed, the characterization results revealed the positive impact of the promoters on Cu dispersion and the total basicity etc., which were critical for CO2 adsorption/conversion. Interestingly, the Fe dopants accelerated the formation of desirable C2+ oxygenates (ethanol and n-propanol).
An environmentally benign carbonaceous solid acid was synthesized from microalgae residue discarded after biodiesel production. Thereafter, the as-synthesized carbonaceous solid acid was used for catalytic dehydration of fructose into 5-hydroxymethylfurural (5-HMF). Various techniques such as X-ray diffraction, N-2 adsorption-desorption, scanning electron microscopy, Fourier transform infrared, Raman, X-ray photoelectron spectroscopy and pyridine adsorption etc were conducted to elucidate the structural and acidic properties of the solid acid so as to build the structure-performance relationship. The results suggested that large amounts of -SO3H, phenolic -OH and -COOH groups were grafted onto the investigated material and most of the surface acid sites were assigned to strong Bronsted acid sites. In screening tests with other commercial catalysts, the as-prepared sample presented excellent catalytic activity with 76.65 +/- 2.53% yield of 5-HMF under aqueous conditions. The dehydration of fructose in dimethyl sulfoxide-water biphasic system was also tested, affording the 5-HMF yield as high as 93.84 +/- 1.12%. This work provides an efficient and selective solid acid from biodiesel waste and might shed light on an alternative catalyst for highly efficient production of 5-HMF instead of homogeneous catalysts.
To develop the application of saponins from sea cucumber cooking water in the field of cosmetics,three saponin fractions S1,S2 and S3 were obtained from sea cucumber cooking water with methods including alcohol precipitation,macroporous resin absorption and ethanol gradient elution,and characterized by Infrared spectra. The contents of total saponins in the obtained saponin fractions were determined by vanillin-acetic acid method. The antioxidant activity of each fraction aqueous solution and the inhibitory action of tyrosinase activity were determined by 1 ,1-diphenyl-2-picrylhydrazyl (DPPH)method and biochemical-enzymic method. The whitening and antisenility efficacy of each saponin fraction was comprehensively evaluated. The results indicated that fractions S1,S2 and S3 all contained triterpenoid saponins,the corresponding mass fractions were 6. 09%,34. 08% and 63. 51%, respectively. Among the three fractions,fraction S2 aqueous solution possessed promising whitening and antisenility efficacy according to the higher DPPH free radical scavenging capacity and inhibitory action on tyrosinase activity. Specifically,when the concentrations of fraction S2 were greater than or equal to 5 g/L,the scavenging ratios kept at 92. 5%,and when the concentrations were between 50 and 70 g/L,the inhibitory ratios were stable at 30. 4%. Accordingly,fraction S2 may act as an excellent cosmetic additive for skin whitening and antisenility.
Carbon dioxide reforming of ethanol over Rh/CeO2 catalyst was deeply investigated at different reaction temperatures of 450–700 °C and reactant ratios (CO2/ethanol from 1 to 3) under atmospheric pressure. The obtained results indicated that Rh/CeO2 catalyst presented a promising activity and stability for syngas production from renewable bio-ethanol instead of conventional methane. Typically, CO2-rich conditions (CO2/ethanol = 3) were favorable for reaction process and dynamic coke cleaning, which led to remarkably stable performance over 65 h on stream. The strong redox capacity of CeO2 support might also accelerate CO2 activation and prevent the carbon accumulation over the catalyst surface. Additionally, tunable H2/CO ratios were available by changing the CO2/ethanol ratios. The results from characterization of samples before and after catalytic tests allowed to establish the relationship between textural properties and catalytic performance.
The effect of preparation method on the catalytic behavior of Cu based composite oxide catalysts for steam reforming of methanol (SRM) has been deeply investigated in this work. The catalyst synthesized by active carbon co-nanocasting technique (CuZnAlZrGa-A) exhibited a satisfactory activity which showed similar to 86.1% methanol conversion, 74.6 mol% H-2 concentration while no detectable CO was formed at 275 degrees C. However, methanol conversion decreased to ca. 73.3% together with 69.4 mol% H-2 for another investigated catalyst produced by a conventional co-precipitation method (CuZnAlZrGa-C). The CuZnAlZrGa-A catalyst also presented strong resistance to deactivation and maintained consistent behavior during a 70 h stability test. The as-prepared samples were further examined by a variety of characterization techniques including BET, XRD, TPR, TPO, Raman to elucidate the textural and structural properties so as to establish the catalytic performance-structure relationship. The results revealed that the observed excellent catalytic performance for CuZnAlZrGa-A catalyst might be due to its high Cu dispersion and the strong metal-support interaction. (C) 2016 Published by Elsevier Ltd.
常温下经过不同时间的锆化处理,在冷轧板(CRS)表面制得一层淡黄色、金黄色和蓝紫色等不同颜色的转化膜.采用扫描电镜和能谱研究不同颜色转化膜的形貌和元素组成,转化膜主要由C、O、Fe、Zr和F等元素组成.通过电化学阻抗谱(EIS)研究不同颜色转化膜的电化学性能,通过百格试验和中性盐雾试验(NSS)检测粉末涂装后漆膜的附着力和耐腐蚀能力;结果显示,银白色裸板,淡黄色、金黄色、蓝紫色转化膜均具有一定的耐腐蚀能力,不同颜色转化膜可以显著提高冷轧板与粉末漆层的附着力和涂装之后冷轧板的抗腐蚀能力,其中金黄色转化膜表现出更加优异的耐腐蚀能力,其500 h中性盐雾实验评级达到0级.