GREEN CHEMISTRY
·
2012
·Vol. 14
·期 9
·2506-2512
·
IF 6.32
Jianjian Wang,Jiawen Ren,Xiaohui Liu,Jinxu Xi,Qineng Xia,Yanhong Zu,Guanzhong Lu,Yanqin Wang
5-Hydroxymethylfurfural (HMF) is a very important intermediate in the fine chemical industry. This study aims to investigate the direct conversion of glucose or glucose-based carbohydrates, such as sucrose, cellobiose, inulin, starch and cellulose, to HMF by using a Sn-Mont catalyst. With the use of this catalyst, a HMF yield of 53.5% was achieved from glucose in a mono-phase medium of tetrahydrofuran (THF)/dimethylsulfoxide (DMSO) at 160 °C for 3 h. The success of one-step conversion of glucose to HMF is attributed to the Sn-Mont catalyst containing two types of acid sites, Lewis acid and Brønsted acid sites. The former one plays a crucial role in the isomerization of glucose to fructose and the latter one is active in the dehydration of generated fructose to HMF. Furthermore, Sn-Mont catalyst also demonstrated excellent activity in the conversion of disaccharides and polysaccharides and as high as 39.1% HMF was directly obtained from cellulose in a THF/H2O–NaCl bi-phasic system.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Jiahui Li,Genyan Hao,Gang Jin,Tao Zhao,Dandan Li,Dazhong Zhong,Jinping Li,Qiang Zhao
Replacing the anodic oxygen evolution reaction (OER) in water splitting with 5-hydroxymethylfurfural oxidation reaction (HMFOR) can not only reduce the energy required for hydrogen production but also yield the valuable chemical 2,5-furandicarboxylic acid (FDCA). Co-based catalysts are known to be efficient for HMFOR, with high-valent Co being recognized as the main active component. However, efficiently promoting the oxidation of Co 2+ to produce high-valent reactive species remains a challenge. In this study, Ni-doped CoTe (CoNiTe) nanorods were prepared as efficient catalysts for HMFOR, achieving a high HMFOR current density of 65.3 mA cm −2 at 1.50 V. Even after undergoing five successive electrolysis processes, the Faradaic efficiency (FE) remained at approximately 90.7 %, showing robust electrochemical durability. Mechanistic studies indicated that Ni doping changes the electronic configuration of Co, enhancing its charge transfer rate and facilitating the oxidation of Co 2+ to high-valent CoO 2 species. This work reveals the effect of Ni doping on the reconfiguration of the active phase during HMFOR.
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Journal of Energy Chemistry
·
2017
·
IF 2.594
Xiaoyu Wang,Wei Chen,Zheng Li,Xianhai Zeng,Xing Tang,Yong Sun,Tingzhou Lei,Lu Lin
In this study we report a new reaction pathway in which the hydroxyl and the aldehyde groups of 5-hydroxymethyl furfural were aminated respectively. Hydroxyl group was aminated via Ritter reaction followed by direct reductive amination of aldehyde group. For the Ritter reaction of 5-hydroxymethyl furfural, mixture of trifluoromethane sulfonic acid and phosphoric anhydride showed good performance and the intermediate N -acyl-5-aminomethyl furfural with the highest yield of 89.1 wt% was obtained. Optimization of direct reductive amination of 2,5-bis(aminomethyl) furan was conducted and a yield of 45.7 wt% was achieved. This study presents a simple way for preparing bis(amino)furans from renewable biomass based 5-hydroxymethyl furfural, which enriches the biorefinery concept from biomass.
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JOURNAL OF MATERIALS SCIENCE
·
2016
·Vol. 51
·期 24
·10849-10862
·
IF 2.302
Zhang Man,Li Chuan,Gao Huiqi,Fu Wei,Li Yingying,Tang Liwei,Zhou Zhiming
Twelve salts of 3-nitro-1,2,4-triazol-5-one (NTO) (ammonium, hydrazinium, guanidinium, aminoguanidinium, diaminoguanidinium, triaminoguanidinium, N -carbamoylguanidinium, semicarbazidium, 1,5-diamino-1,2,4-tetrazolium, 3,4,5- triamino-1,2,4-triazolium, 3,6,7-triamino-7H-[1, 2, 4]triazolo[5,1-c][1,2,4]triazol-2- ium, and 4,4′,5,5′-tetraamino-3,3′-bi-1,2,4-triazolium) were synthesized. The new salts were fully characterized by 1 H and 13 C NMR spectroscopy, infrared spectroscopy, and elemental analysis. The crystal structures of salts 10 and 11 were determined by single-crystal X-ray diffraction. All energetic salts except salt 6 exhibit excellent thermal stabilities with decomposition temperatures ranging from 203 to 270 °C. The densities of salts ranged from 1.65 to 1.88 g cm −1 as measured by a gas pycnometer. Theoretical performance calculations (Gaussian 03 and EXPLO5 v6.01) yielded detonation pressures and detonation velocities for the energetic salts, ranging from 24.4 to 38.1 GPa and 8136 to 9575 m s −1 , respectively. In particular, salt 2 has an outstanding detonation performance ( P
cj = 38.1 GPa, v
D = 9575 m s −1 ) with a satisfactory acidity compared to that of NTO ( pK
a = 5.63 versus pK
a = 2.37). Furthermore, the particles of salt 2 form two-dimensional blades of submicron size, as determined by scanning electron microscopy analysis. Meanwhile, salt 2 was compatible with TNAZ, TATB, TKX-50, Al, NH 4 ClO 4 , CL-20, TNT, and F2603 fluororubber, as determined by differential scanning calorimetry or vacuum stability tests.
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SOLID STATE SCIENCES
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2017
·
IF 1.811
Yisong Wang,Tao Du,Yanli Song,Shuai Che,Xin Fang,Lifeng Zhou
ZSM-5 type zeolite with mesoporous structure was prepared and then amine-functionalized with tetraethylenepentamine (TEPA) by wet impregnation method to form a series of CO 2 adsorbents (ZTx). The structural properties of ZSM-5 and ZTx were characterized by XRD , FTIR , TGA/DTG, nitrogen adsorption/desorption, SEM and EDX techniques. The adsorption capacity of the adsorbents with different amine loading was measured at a temperature from 40 to 100 °C and the adsorption capacity of ZT7 was 1.80 mmol/g at 100 °C. The adsorption process and mechanism were studied by fitting the experimental data used the three adsorption kinetic models, and a complex physical and chemical mixing process was produced as the amine entered the surface and pore size of the zeolite. The high adsorption selectivity at 10% CO 2 concentration and the stability of the five adsorption desorption cycles indicated that ZT7 is a suitable and promising CO 2 adsorbent for the purification of industrial flue gas .
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2014
·
IF 3.785
Meixia Xu,Minjie Sun,Hongzhi Qiao,Qineng Ping,Eltayeb Suliman Elamin
Oral modified-release delivery systems, such as bio-adhesive one, enable drug delivery to affected regions and minimize the side effects by reducing the systemic absorption. Our aim was to develop colon adhesive pellets of 5-aminosalicylic acid (5-ASA) for the treatment of ulcerative colitis . The core of the pellet was formulated from bioadhesive agents, Carbomer 940 and hydroxypropyl cellulose (HPC), by extrusion/spheronization method and coated with Surelease ® as inner layer for waterproof and with Eudragit ® S100 as outer layer for pH control. The rat model of ulcerative colitis was used to evaluate the efficiency of our loaded pellets as a drug carrier. Microcrystalline cellulose 101 (PH 301) was found to be the best agent for pellet core. The ratio of CP940 to HPC should be kept as (1:1) to achieve high bioadhesion. When the amount of Surelease ® was from 16% to 20% and of Eudragit ® S100 was 28%, the dissolution profiles of coated pellets revealed no drug release in the artificial gastric fluid (pH 1.0) within 2 h and less than 10% was released in phosphate buffer (pH 6.0) within 2 h whereas complete dissolution was observed in colonic fluid of pH 7.4 for 20 h. The animal experiment showed that 5-ASA loaded colon adhesive pellets had optimal therapeutic effect. We showed a novel approach to prepare effective bioadhesive pellets as colon targeted drug delivery system .
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Catalysts
·
2017
·Vol. 7
·期 6
·182
·
IF 3.082
Xin Yu,Xueying Gao,Ruili Tao,Lincai Peng
The use of common metal salts as catalysts for 5-ethoxymethylfurfural (EMF) synthesis from carbohydrate transformation was performed. Initial screening suggested AlCl3as an efficient catalyst for EMF synthesis (45.0%) from fructose at 140 °C. Interestingly, CuSO4and Fe2(SO4)3were found to yield comparable EMF at lower temperature of 110 to 120 °C, and high yields of ethyl levulinate (65.4–71.8%) were obtained at 150 °C. However, these sulfate salts were inactive in EMF synthesis from glucose and the major product was ethyl glucoside with around 80% yield, whereas EMF of 15.2% yield could be produced from glucose using CrCl3. The conversion of sucrose followed the accumulation of the reaction pathways of fructose and glucose, and a moderate yield of EMF could be achieved.Keywords:carbohydrate;5-ethoxymethylfurfural;catalytic conversion;metal salt;Lewis acid
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Jiansong Wang,Wenru Zhao,Hui Yu,Wei Wang,Yipu Xu,Liu-Liu Shen,Gui-Rong Zhang,Donghai Mei
Nickel-based materials are promising electrocatalysts for anodic oxidation of 5-hydroxymethylfurfural (HMF) to value-added 2, 5-furandicarboxylic acid (FDCA). However, their catalytic efficiency is impeded by the sluggish phase transformation of Ni(II) hydroxide to the active Ni(III) oxyhydroxide. Herein, we demonstrate for the first time that the phase transformation kinetics and the HMF oxidation activity of nickel nanoparticles can be modulated by creating self-assemblies with different particle aggregation structures: ordered nanoarrays, disordered nanoarrays, and random aggregates. Notably, the nanoparticle assembly featuring an ordered nanoarray structure exhibits the highest activity, achieving 99.8 % HMF conversion and 99.2 % FDCA yield at 1.36 V. In situ Raman spectroscopy and electrochemical analysis reveal that the ordered nanoarray effectively accelerates the transformation kinetics, attributed to the reduced dehydrogenation barrier of Ni(II) hydroxide as confirmed by density functional theory calculations. This work contributes new insights into the structure-performance relationship of Ni-based catalysts, offering valuable guidance for designing high-performing electrocatalysts.
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Chem Catalysis
·
2025
·
IF 11.6
Bin Zhu,Jie Yang,Qiuge Wang,Xiao Yu,Shilin Fan,Weiping Xie,Jian Zhang,Chunlin Chen
The intersection of corrosion engineering for constructing high-performance electrocatalysts and the efficient upgrading of biomass represents two vibrant, sustainable research themes that promise exciting outcomes when combined. In this study, we achieve the highly selective hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) over corrosion-induced CoCu microwire arrays on copper foam (CoCuMW/CF). An HMF conversion of 95.7% and a BHMF yield of 85.4% can be achieved in the electrochemical process. Mechanistic investigations indicate that the reaction pathway is primarily governed by the Langmuir-Hinshelwood (L-H) mechanism. Density functional theory (DFT) calculations reveal that the CoCu interface exhibits lower free energy barriers for the hydrogenation steps of HMF, which significantly enhances the catalytic performance and BHMF selectivity. The induction of corrosion enhances the electrochemical hydrogenation performance of the copper-based electrocatalyst, which holds significant value in reducing catalyst costs and accelerating the application of HMF electrohydrogenation.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hexuan Li,Dongdong Li,Yilin Li,Haoran Liu,Junzhi Li,Wei Han
The reaction kinetics of lithium-sulfur (Li-S) battery mainly depends on the capture and catalytic conversion efficiency of lithium polysulfide (LiPSs). The unique electron configuration of the 5d metal and the high electrical conductivity of MXene can enhance the interaction between the catalyst and LiPSs. However, the challenge of enhancing the adsorption of LiPSs by regulating the electronic structure of the catalyst with 5d metal and MXene remains unresolved and obscure. In this work, we have developed molybdenum disulfide (MoS 2 )-tungsten disulfide (WS 2 ) @MXene (MoS 2 -WS 2 @MX) heterostructure catalysts for separator coatings in Li-S batteries by introducing W and MXene for the first time. Theoretical calculations demonstrate that the 5 d metallic and conductive MXene coupling effectively modulate the orbital hybridization degree between the catalyst and LiPSs, thereby reducing the energy barrier for LiPSs conversion. Electrochemical test and in situ tests verify the effectiveness of the strategy on the adsorption and conversion of LiPSs. Consequently, the MoS 2 -WS 2 @MX based batteries exhibit high initial reversible capacity of 950.3 mAh g −1 and low capacity decay of 0.066 % per cycle over 500 cycles at 2 C, which is superior to most reported catalysts. This study provides a dual regulatory strategy for enhancing catalytic activity, offering valuable insights for the advancement of high-performance Li-S batteries.
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Environmental Chemistry
·
2024
·Vol. 20
·期 7
·292-301
·
IF 2
Xiao-Yan Cao,Min Liu,Ling Li,Gui-Peng Yang
Environmental context Organophosphorus (OP) is bioavailable to phytoplankton with photolysis can play an important role in the process. The photolysis behaviour of an OP (adenosine 5′-monophosphate, AMP) in seawater was investigated, and AMP can release inorganic phosphate under environmentally relevant light conditions, indicating OP photodegradation might be important in the phosphorus biogeochemical cycle. The results are helpful to further understand the bioavailability and cycle of OP in marine environment.Rationale Organic phosphorus (OP) is a potential source of bioavailable phosphorus for phytoplankton through photolysis and other degradation processes. Therefore, OP photodegradation plays an important role in phosphorus biogeochemical cycle.Methodology Taking adenosine 5′-monophosphate (AMP) as a model OP, we investigated the photolysis behaviour in seawater and discussed the mechanism. The photolysis dynamics were studied based on the inorganic phosphorus production at appropriate time intervals, which was analysed by spectrophotometric molybdenum blue method. The effects of medium, light and radicals were investigated.Results It was found that AMP can release inorganic phosphate under photosynthetically active radiation and ultraviolet (UV) with UVB being the most reactive band. The degradation of AMP in seawater was lower than that in deionised water under the same conditions, and the fresh seawater was more beneficial than aged seawater. The kinetics could be described by apseudo-first order equation. Fe3+ can promote the photolysis due to the generation of ·OH radicals, while within the range of this study, changes of Fe3+ content have no substantial effect on the promotion. The influence of ethanol and tetrahydrofuran as radical inhibitor showed evident inhabitation to the degradation, indicating that ·OH and 1O2 played an important role in the process, and ·OH seemed more important than 1O2.Discussion OP photodegradation is of importance in the phosphorus biogeochemical cycle. Varying properties of the medium and light can affect the OP transformation in seawater. The results are helpful to further understand the bioavailability and cycle of OP in the marine environment.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Dezhu Zhang,Su Fan,Kenan Xu,Haotian Liu,Nana Chang,Yijie Wang,Yixing Wang,Kang Huang,Zhi Xu
Vanadium flow battery (VFB) shows great potential in balancing the volatility of renewable energy. In this work, we investigated, for the first time, the various properties of crystalline ZSM-5 membranes prepared through the organic template-free gel strategy in VFB. The subnano windows (∼0.55 nm) of ZSM-5 zeolite provided selective transport paths for protons (∼0.27 nm) and blocked the vanadium (>0.6 nm) migration through pore repulsion effect. The zeolite membranes exhibited a very low vanadium penetration rate (0.05 mmol L–1 h–1), achieving a Coulombic efficiency (CE) of 96.1%, a voltage efficiency of 78.3%, and an energy efficiency of 75.3% at the current density of 40 mA cm–2. Notably, ZSM-5 prepared using the template-free strategy eliminates the need for a high-temperature calcination step, and the membrane has a lower defect density and exhibits a higher CE. The self-discharge time of the ZSM-5 zeolite membrane increased up to 78 h. Furthermore, the charge–discharge performance kept stable more than 300 cycles at 60 mA cm–2.
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