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Enhanced hydrogen production from aqueous methanol solution using TiO

Paramasivan GOMATHISANKAR,Tomoko NODA,Hideyuki KATSUMATA,Tohru SUZUKI,Satoshi KANECO

《化学科学与工程前沿(英文)》 2014年 第8卷 第2期   页码 197-202 doi: 10.1007/s11705-014-1417-y

摘要: The photocatalytic hydrogen production from aqueous methanol solution using titanium dioxide (TiO ) was investigated in the addition of metal particles including copper, lead, tin, and zinc. The results show that only the addition of copper particles enhances the hydrogen production. The copper usage and reaction temperature were further optimized for TiO /Cu photocatalyts. Under the optimal conditions, the hydrogen production using TiO /Cu as photocatalysts is approximately 68 times higher than that obtained with only TiO .

关键词: photocatalytic hydrogen generation     methanol     copper particles     TiO2     metal-semiconductor interface    

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenationof methyl palmitate to hydrocarbons using methanol as the hydrogen donor

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 443-460 doi: 10.1007/s11705-021-2079-1

摘要: Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

关键词: Stöber method     carbon-coated Ni-Co alloy     in-situ hydrodeoxygenation     methyl palmitate     decarbonylation/decarboxylation    

Transition metal doped mesoporous titania with a crystalline framework as catalysts for oxidation of -bromotoluene to -bromobenzaldehyde

YANG Zehui, OU Encai, WANG Yunan, PENG Li, WANG Jiaqiang, YIN Lihui

《化学科学与工程前沿(英文)》 2008年 第2卷 第3期   页码 296-300 doi: 10.1007/s11705-008-0044-x

摘要: Transition metal M (M = Mn, Fe, Co, Ni, Cu, and Zn) doped mesoporous titania with a crystalline framework was employed as catalysts for the oxidation of -bromotoluene (PBT) to -bromobenzaldehyde (BBD) in acetic acid using aqueous hydrogen peroxide as oxidant. It was found that mesoporous TiO doped with those metals (Fe, Co and Ni) whose atomic radii are relatively smaller exhibited higher conversion rate of PBT. Among these catalysts, the Co/meso-TiO exhibited high substrate conversion and good product (-bromobenzaldehyde) selectivity plus it can be reused once with almost the same activity. The effect of different Ti/Co (molar) ratio on the activities of Co/meso-TiO was also investigated.

关键词: selectivity     conversion     -bromobenzaldehyde     aqueous hydrogen     oxidation    

Alumina modified sodium vanadate cathode for aqueous zinc-ion batteries

《能源前沿(英文)》   页码 775-781 doi: 10.1007/s11708-023-0902-8

摘要: Aqueous zinc-ion batteries (ZIBs) have great prospects for widespread application in massive scale energy storage. By virtue of the multivalent state, open frame structure and high theoretical specific capacity, vanadium (V)-based compounds are a kind of the most developmental potential cathode materials for ZIBs. However, the slow kinetics caused by low conductivity and the capacity degradation caused by material dissolution still need to be addressed for large-scale applications. Therefore, sodium vanadate Na2V6O16·3H2O (NVO) was chosen as a model material, and was modified with alumina coating through simple mixing and stirring methods. After Al2O3 coating modification, the rate capability and long-cycle stability of Zn//NVO@Al2O3 battery have been significantly improved. The discharge specific capacity of NVO@Al2O3 reach up to 228 mAh/g (at 4 A/g), with a capacity reservation rate of approximately 68% after 1000 cycles, and the Coulombic efficiency (CE) is close to 100%. As a comparison, the capacity reservation rate of Zn//NVO battery is only 27.7%. Its superior electrochemical performance is mainly attributed to the Al2O3 coating layer, which can increase zinc-ion conductivity of the material surface, and to some extent inhibit the dissolution of NVO, making the structure stable and improving the cyclic stability of the material. This paper offers new prospects for the development of cathode coating materials for ZIBs.

关键词: cathodes     aqueous zinc-ion batteries     sodium vanadate     alumina     coating    

Isolation of highly purity cellulose from wheat straw using a modified aqueous biphasic system

Lifeng YAN, Yi ZHAO, Qing GU, Wan LI

《化学科学与工程前沿(英文)》 2012年 第6卷 第3期   页码 282-291 doi: 10.1007/s11705-012-0901-5

摘要: Cellulose samples with molecular weights ranging from 8.39 × 10 to 11.00 × 10 g/mol were obtained from wheat straw. The dewaxed wheat straw was pretreated with aqueous hydrochloric acid followed by delignification using an environmentally benign poly(ethyleneglycol)/salt aqueous biphasic system. The yield of cellulose was in the range of 48.9%–55.5% and the cellulose contained 1.2%–3.2% hemicelluloses, and 0.97%–3.47% lignin. All the isolated cellulose samples could be directly dissolved in a 6 wt-% NaOH/4 wt-% urea aqueous solution through a precooling-thawing process to form a homogenous solution. The separation process was investigated and the obtained cellulose and its solution were characterized by Fourier transform infrared spectroscopy, scanning electron microscopy and energy dispersive X-ray apparatus, and X-ray diffraction. The results revealed that aqueous soluble cellulose can be directly prepared from wheat straw by this method and this study opens a novel pathway to prepare cellulosic materials from agricultural waste.

关键词: cellulose     straw     separation     aqueous solution    

USING AN AQUEOUS ENZYMATIC METHOD

《农业科学与工程前沿(英文)》 2021年 第8卷 第4期   页码 623-634 doi: 10.15302/J-FASE -2021400

摘要:

Schizochytrium sp., a marine microalga, is a potential source of edible oil due to its short growth cycle and rapid lipid accumulation, especially of docosahexaenoic acid. An approach to isolate edible microalgal oil from Schizochytrium sp. using aqueous enzymatic extraction (AEE) was developed. Parameters were optimized by single-factor experiments followed by Box-Behnken design. Proteases were effective in extracting oil. The maximum free oil recovery (49.7%±0.58%) and total oil recovery (68.1%±0.94%) were obtained under optimum conditions of liquid-to-solid ratio of 4.8:1, a 2.5% enzyme concentration of papain and an extraction time of 2.2 h. There was a significant difference (P<0.05) in polyunsaturated fatty acid composition between microalgal oil obtained by AEE and by Soxhlet extraction, with the former having superior physiochemical properties and higher concentrations of bioactive components including total phenolic compounds and total tocopherols. These findings indicate a potential application of AEE for extraction of oil from Schizochytrium sp.

 

关键词: antioxidant activity / aqueous enzymatic extraction / edible microalgal oil / fatty acid composition / physicochemical properties    

Conversion of phenol to cyclohexane in the aqueous phase over Ni/zeolite bi-functional catalysts

Jimei Zhang, Fuping Tian, Junwen Chen, Yanchun Shi, Hongbin Cao, Pengge Ning, Shanshan Sun, Yongbing Xie

《化学科学与工程前沿(英文)》 2021年 第15卷 第2期   页码 288-298 doi: 10.1007/s11705-020-1932-y

摘要: A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation (HDO) of phenol. The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites, which further influenced the catalytic performances. The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles, and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons. Importantly, the Ni/HIM-5 bi-functional catalyst exhibited a high activity (98.3%) and high selectivity for hydrocarbons (98.8%) when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.

关键词: aqueous-phase hydrodeoxygenation     phenol     hydrocarbons     Ni/HIM-5     bi-functional catalyst    

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

《化学科学与工程前沿(英文)》 2023年 第17卷 第2期   页码 217-225 doi: 10.1007/s11705-022-2214-7

摘要: Aqueous zinc-ion batteries are attracting considerable attention because of their high safety compared with conventional lithium-ion batteries. Manganese-based materials have been widely developed for zinc-ion batteries cathode owning to their low cost, high security and simple preparation. However, the severe volume expansion and poor stability during charging and discharging limit the further development of manganese-based cathodes. Herein, superior α-MnO2@g-C3N4 was successfully prepared for stable zinc-ion batteries (ZIBs) cathode by introducing g-C3N4 nanosheets. Compared with pure α-MnO2, α-MnO2@g-C3N4 has a specific capacity of 298 mAh·g–1 at 0.1 A·g–1. Even at 1 A·g–1, the α-MnO2@g-C3N4 still retains 100 mAh·g–1 (83.4% retention after 5000 cycles), implying its excellent cycling stability. The α-MnO2@g-C3N4-based cathode has the highest energy density (563 Wh·kg–1) and power energy density (2170 W·kg–1). This work provides new avenues for the development of a wider range of cathode materials for ZIBs.

关键词: α-MnO2 hollow nanorods     g-C3N4     heterojunction     aqueous Zn-ion batteries    

Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

Qishi LUO

《环境科学与工程前沿(英文)》 2014年 第8卷 第2期   页码 188-194 doi: 10.1007/s11783-013-0544-x

摘要: The oxidation of aqueous monochlorobenzene (MCB) solutions using thermally- activated persulfate has been investigated. The influence of reaction temperature on the kinetics of MCB oxidation was examined, and the Arrenhius Equation rate constants at 20°C, 30°C, 40°C, 50°C, and 60°C for MCB oxidation performance were calculated as 0, 0.001, 0.002, 0.015, 0.057 min , which indicates that elevated temperature accelerated the rate. The most efficient molar ratio of persulfate/MCB for MCB oxidation was determined to be 200 to 1 and an increase in the rate constants suggests that the oxidation process proceeded more rapidly with increasing persulfate/MCB molar ratios. In addition, the reactivity of persulfate in contaminated water is partly influenced by the presence of background ions such as Cl , , , and . Importantly, a scavenging effect in rate constant was observed for both Cl and but not for other ions. The effective thermally activated persulfate oxidation of MCB in groundwater from a real contaminated site was achieved using both elevated reaction temperature and increased persulfate/MCB molar ratio.

关键词: persulfate     monochlorobenzene     advanced oxidation process    

Modeling the aqueous reaction kinetics of estriol with ferrate

Cong LI, Naiyun GAO

《化学科学与工程前沿(英文)》 2009年 第3卷 第1期   页码 39-45 doi: 10.1007/s11705-009-0098-4

摘要: In this study the aqueous oxidation kinetics of estriol (E3) by potassium ferrate (K FeO ), a chemical for its strong oxidizing power and for producing a coagulant from its reduced state (i.e. Fe(III)), was evaluated in the range of pH 8-12 with different molar ratios of the reactants. As the degree of Fe(VI) protonation varies with the solution pH, it was found that a first order model was not suitable to describe the oxidation reaction. This paper describes a theoretical representation that closely models the reaction kinetics of E3 and ferrate. From this modeling, the reaction rates of HFe and Fe with E3 have been determined. The results show that the reactivity of HFe with dissociated and undissociated E3 is greater than that of Fe , and that E3 is more reactive in its dissociated state.

关键词: ferrate     estriol     endocrine disruptor     kinetics     oxidation    

Covalent triazine framework with efficient photocatalytic activity in aqueous and solid media

Cyrine Ayed, Wei Huang, Kai A. I. Zhang

《化学科学与工程前沿(英文)》 2020年 第14卷 第3期   页码 397-404 doi: 10.1007/s11705-019-1884-2

摘要: Covalent triazine frameworks (CTFs) have been recently employed for visible light-driven photocatalysis due to their unique optical and electronic properties. However, the usually highly hydrophobic nature of CTFs, which originates from their overall aromatic backbone, leads to limitations of CTFs for applications in aqueous media. In this study, we aim to extend the range of the application media of CTFs and design hybrid material of a CTF and mesoporous silica (SBA-15) for efficient photocatalysis in aqueous medium. A thiophene-containing CTF was directly synthesized in mesopores of SBA-15. Due to the high surface area and the added hydrophilic properties by silica, the hybrid material demonstrated excellent adsorption of organic molecules in water. This leads not only to high photocatalytic performance of the hybrid material for the degradation of organic dyes in water, but also for efficient photocatalysis in solvent-free and solid state. Furthermore, the reusability, stability and easy recovery of the hybrid material offers promising metal-free heterogeneous photocatalyst for broader applications in different reaction media.

关键词: photocatalysis     covalent triazine framework     aqueous medium     SBA-15     solid state    

Pathway of the ozonation of 2,4,6-trichlorophenol in aqueous solution

PI Yunzheng, WANG Jianlong

《环境科学与工程前沿(英文)》 2007年 第1卷 第2期   页码 179-183 doi: 10.1007/s11783-007-0031-3

摘要: The reaction mechanism and pathway of the ozonation of 2,4,6-trichlorophenol (2,4,6-TCP) in aqueous solution were investigated. The removal efficiency and the variation of HO, Cl, formic acid, and oxalic acid were studied during the semi-batch ozonation experiments (continuous for ozone gas supply, fixed volume of water sample). The results showed that when there was no scavenger, the removal efficiency of 0.1 mmol/L 2,4,6-TCP could reach 99% within 6 min by adding 24 mg/L ozone. The reaction of molecular ozone with 2,4,6-TCP resulted in the formation of HO. The maximal concentration of HO detected during the ozonation could reach 22.5% of the original concentration of 2,4,6-TCP. The reaction of ozone with HO resulted in the generation of a lot of OH° radicals. Therefore, 2,4,6-TCP was degraded to formic acid and oxalic acid by ozone and OH° radicals together. With the inhibition of OH°radicals, ozone molecule firstly degraded 2,4,6-TCP to form chlorinated quinone, which was subsequently oxidized to formic acid and oxalic acid. Two reaction pathways of the degradation of 2,4,6-TCP by ozone and O/OH° were proposed in this study.

Reduced texaphyrin: A ratiometric optical sensor for heavy metals in aqueous solution

Harrison D. Root, Gregory Thiabaud, Jonathan L. Sessler

《化学科学与工程前沿(英文)》 2020年 第14卷 第1期   页码 19-27 doi: 10.1007/s11705-019-1888-y

摘要: We report here a water-soluble metal cation sensor system based on the as-prepared or reduced form of an expanded porphyrin, texaphyrin. Upon metal complexation, a change in the redox state of the ligand occurs that is accompanied by a color change from red to green. Although long employed for synthesis in organic media, we have now found that this complexation-driven redox behavior may be used to achieve the naked eye detectable colorimetric sensing of several number of less-common metal ions in aqueous media. Exposure to In(III), Hg(II), Cd(II), Mn(II), Bi(III), Co(II), and Pb(II) cations leads to a colorimetric response within 10 min. This process is selective for Hg(II) under conditions of competitive analysis. Furthermore, among the subset of response-producing cations, In(III) proved unique in giving rise to a ratiometric change in the ligand-based fluorescence features, including an overall increase in intensity. The cation selectivity observed in aqueous media stands in contrast to what is seen in organic solvents, where a wide range of texaphyrin metal complexes may be prepared. The formation of metal cation complexes under the present aqueous conditions was confirmed by reversed phase high-performance liquid chromatography, ultra-violet-visible absorption and fluorescence spectroscopies, and high-resolution mass spectrometry.

关键词: texaphyrin     fluorescent sensor     ion-sensing     indium     mercury    

A systemic review of hydrogen supply chain in energy transition

《能源前沿(英文)》 2023年 第17卷 第1期   页码 102-122 doi: 10.1007/s11708-023-0861-0

摘要: Targeting the net-zero emission (NZE) by 2050, the hydrogen industry is drastically developing in recent years. However, the technologies of hydrogen upstream production, midstream transportation and storage, and downstream utilization are facing obstacles. In this paper, the development of hydrogen industry from the production, transportation and storage, and sustainable economic development perspectives were reviewed. The current challenges and future outlooks were summarized consequently. In the upstream, blue hydrogen is dominating the current hydrogen supply, and an implementation of carbon capture and sequestration (CCS) can raise its cost by 30%. To achieve an economic feasibility, green hydrogen needs to reduce its cost by 75% to approximately 2 /kg at the large scale. The research progress in the midterm sector is still in a preliminary stage, where experimental and theoretical investigations need to be conducted in addressing the impact of embrittlement, contamination, and flammability so that they could provide a solid support for material selection and large-scale feasibility studies. In the downstream utilization, blue hydrogen will be used in producing value-added chemicals in the short-term. Over the long-term, green hydrogen will dominate the market owing to its high energy intensity and zero carbon intensity which provides a promising option for energy storage. Technologies in the hydrogen industry require a comprehensive understanding of their economic and environmental benefits over the whole life cycle in supporting operators and policymakers.

关键词: hydrogen production     hydrogen transportation and storage     hydrogen economy     carbon capture and sequestration (CCS)     technology assessment    

Dibutyl phthalate adsorption characteristics using three common substrates in aqueous solutions

Tiancui Li, Yaocheng Fan, Deshou Cun, Yanran Dai, Wei Liang

《环境科学与工程前沿(英文)》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1205-5

摘要: • DBP adsorption was tested using three kinds of substrates in constructed wetlands. • The DBP adsorption capacity followed the order: steel slag>gravel>shell sand. • High temperatures increased the DBP adsorption capacity in the substrates. • DOM consistently inhibited the DBP adsorption onto steel slag and gravel. In recent years, the presence and adverse impacts of phthalic acid esters in aquatic environments have gained increasing attention. This work investigated the adsorption behavior of a typical phthalic acid ester, dibutyl phthalate (DBP), onto steel slag, gravel, and shell sand (substrates commonly used in constructed wetlands). The influence of dissolved organic matter (DOM) on DBP adsorption was investigated using humic acid as a proxy for DOM. The results demonstrated that the adsorption of DBP to three substrates reached equilibrium within 96 h, and the adsorption kinetics were well fitted by a pseudo-second-order model. The DBP adsorption isotherms were best fitted by the Langmuir adsorption model. The DBP adsorption capacity decreased in the order of steel slag>gravel>shell sand, with values of 656 mg/kg, 598 mg/kg, and 6.62 mg/kg at 25°C, respectively. DBP adsorbed to the surface of all substrates in a monolayer via an endothermic process. The DBP adsorption capacities of steel slag and gravel decreased as the DOM content increased. The DBP adsorption mechanisms to steel slag and gravel mainly involved the surface coordination of DBP with –OH or –COOH groups and electrostatic interactions. The results of this work suggest that steel slag and gravel may be ideal substrates for use in constructed wetlands to treat wastewater polluted with DBP.

关键词: Adsorption     Dibutyl phthalate (DBP)     Dissolved organic matter     Substrates    

标题 作者 时间 类型 操作

Enhanced hydrogen production from aqueous methanol solution using TiO

Paramasivan GOMATHISANKAR,Tomoko NODA,Hideyuki KATSUMATA,Tohru SUZUKI,Satoshi KANECO

期刊论文

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenationof methyl palmitate to hydrocarbons using methanol as the hydrogen donor

期刊论文

Transition metal doped mesoporous titania with a crystalline framework as catalysts for oxidation of -bromotoluene to -bromobenzaldehyde

YANG Zehui, OU Encai, WANG Yunan, PENG Li, WANG Jiaqiang, YIN Lihui

期刊论文

Alumina modified sodium vanadate cathode for aqueous zinc-ion batteries

期刊论文

Isolation of highly purity cellulose from wheat straw using a modified aqueous biphasic system

Lifeng YAN, Yi ZHAO, Qing GU, Wan LI

期刊论文

USING AN AQUEOUS ENZYMATIC METHOD

期刊论文

Conversion of phenol to cyclohexane in the aqueous phase over Ni/zeolite bi-functional catalysts

Jimei Zhang, Fuping Tian, Junwen Chen, Yanchun Shi, Hongbin Cao, Pengge Ning, Shanshan Sun, Yongbing Xie

期刊论文

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

期刊论文

Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

Qishi LUO

期刊论文

Modeling the aqueous reaction kinetics of estriol with ferrate

Cong LI, Naiyun GAO

期刊论文

Covalent triazine framework with efficient photocatalytic activity in aqueous and solid media

Cyrine Ayed, Wei Huang, Kai A. I. Zhang

期刊论文

Pathway of the ozonation of 2,4,6-trichlorophenol in aqueous solution

PI Yunzheng, WANG Jianlong

期刊论文

Reduced texaphyrin: A ratiometric optical sensor for heavy metals in aqueous solution

Harrison D. Root, Gregory Thiabaud, Jonathan L. Sessler

期刊论文

A systemic review of hydrogen supply chain in energy transition

期刊论文

Dibutyl phthalate adsorption characteristics using three common substrates in aqueous solutions

Tiancui Li, Yaocheng Fan, Deshou Cun, Yanran Dai, Wei Liang

期刊论文