ACS Catalysis
·
2022
·
IF 13.7
Yichao Jin,Sarina Sarina,Hongwei Liu,Wayde Martens,Eric R. Waclawik,Erandi Peiris,Jianfeng Jia,Jing Shang,Liangzhi Kou,Cheng Guo,Huai-Yong Zhu
Production of 2,5-furandicarboxylic acid (FDCA, a platform chemical for the chemical industry in the future) by the selective aerobic oxidation of 5-hydroxymethyl-furfural is a crucial component to enable the FDCA production from sugars. The challenge is to achieve a high FDCA yield at low temperatures. Here, we report a catalyst composed of alloyed nanoparticles (containing 1.5 wt % Ag and 1.5 wt % Pd) supported on CeO2 nanofibers, which achieved an excellent FDCA yield (93%) at 20 °C. Interesting observations include yield deterioration at higher reaction temperatures; water is the source of the oxygen atom(s) added to the oxidized intermediates and product, while O2 molecules adsorbed onto the catalyst scavenge electrons, yielding OH• radicals from OH– ions in the reaction system to drive the oxidation. At 20 °C, we avoid side reactions, but there is no external energy provided for overcoming the activation barriers. The barriers for activating the alcohol groups are significant. We find that the appropriate chemisorption on the catalyst is critical for a high FDCA yield. By tuning the Ag/Pd ratio, we attained the most catalytically active sites, bimetallic surface sites, at the boundaries between Ag and Pd clusters. The chemisorption at these sites is strong enough to cause the selective oxidation of both the aldehyde and alcohol groups in HMF at 20 °C, avoiding side reactions at high temperatures. The knowledge acquired from this study is expected to have implications for other catalytic systems where competitive reactions proceed.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2018
·
IF 3.057
Chao Xia,Caiyan Yu,Mengmeng Cao,Jinfeng Xia,Danyu Jiang,Guohong Zhou,Dafeng Zhang,Huili Li
In this work, a new Eu and Tb co-doped luminescent compound based on MOF-5, [Zn 4 O(BDC) 3 ], (named as compound 1 ) was successfully synthesized. The structure and morphology characterizations demonstrate that the initial framework of MOF-5 is retained well after co-doping Eu and Tb. The systematic investigations of photoluminescence behaviors reveal that the heat-treated compound 1 (called as compound 1a ) can be utilized as a multi-channel readout luminescent thermometer in emission intensity ratio, decay time ratio, and luminescence color. It simultaneously exhibits the excellent repetitiveness and reversibility under high temperature region from 303 to 473 K. The relative sensitivity of 1.8%/K at 473 K is much higher than the best one of 1.19%/K previously reported for the mixed-lanthanide MOF Tb 0.8 Eu 0.2 BPDA. Until now, such a ratiometric luminescent thermometer with a high sensitivity at the temperature as high as 473 K has been rarely explored.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Chemical Engineering
·
2019
·
IF 0
Qiuyun Zhang,Xiaofang Liu,Tingting Yang,Quanlin Pu,Caiyan Yue,Shuya Zhang,Yutao Zhang
Direct conversion of fructose into 5-hydroxymethylfurfural (HMF) is achieved by using modified aluminum-molybdenum mixed oxide (S-AlMo) as solid acid catalysts. The synthesized catalyst was characterized by powder XRD, nitrogen adsorption-desorption isotherm, NH3-TPD, and SEM. As a result, the presence of strong acidity, mesostructures, and high surface area in the S-AlMo catalyst was confirmed by nitrogen adsorption-desorption isotherm and NH3-TPD studies. A study by optimizing the reaction conditions such as catalyst dosage, reaction temperature, and time has been performed. Under the optimal reaction conditions, HMF was obtained in a high yield of 49.8% by the dehydration of fructose. Moreover, the generality of the catalyst is also demonstrated by glucose and sucrose with moderate yields to HMF (24.9% from glucose; 27.6% from sucrose) again under mild conditions. After the reaction, the S-AlMo catalyst can be easily recovered and reused four times without significant loss of its catalytic activity.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
Energy & Environmental Materials
·
2024
·
IF 13
Li Zhang,Peiyue Jin,Ze Wu,Bo Zhou,Junchang Jiang,Aomeng Deng,Qiuyue Li,Tanveer Hussain,Yiqiong Zhang,Hanwen Liu,Shuangyin Wang
The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value-added chemicals and nitrogen cycling. Herein, in this work, CuO/Co 3 O 4 with heterogeneous interface is successfully constructed as a bifunctional catalyst for the electrooxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and the electroreduction of nitrate to ammonia (NH 3 ). The open-circuit potential spontaneous experiment shows that more 5-hydroxymethylfurfural molecules are adsorbed in the Helmholtz layer of the CuO/Co 3 O 4 composite, which certifies that the CuO/Co 3 O 4 heterostructure is conducive to the kinetic adsorption of 5-hydroxymethylfurfural. In situ electrochemical impedance spectroscopy further shows that CuO/Co 3 O 4 has faster reaction kinetics and lower reaction potential in oxygen evolution reaction and 5-hydroxymethylfurfural electrocatalytic oxidation. Moreover, CuO/Co 3 O 4 also has a good reduction effect on NO 3 − $$ {\mathrm{NO}}_3^{-} $$ . The ex-situ Raman spectroscopy shows that under the reduction potential, the metal oxide is reduced, and the generated Cu 2 O can be used as a new active site for the reaction to promote the electrocatalytic conversion of NO 3 − $$ {\mathrm{NO}}_3^{-} $$ to NH 3 synthesis. This work provides valuable guidance for the synthesis of value-added chemicals by 5-hydroxymethylfurfural electrocatalytic oxidation coupled with NO 3 − $$ {\mathrm{NO}}_3^{-} $$ while efficiently producing NH 3 .
研究领域:
化学工程
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 4
·404-414
·
IF 4.5
Cheng Junjun,Zhao Yitao,Xu Guohao,Zhang Peng,Zhu Xuedong,Yang Fan
Alkylation of benzene with carbon dioxide and hydrogen to produce toluene and xylene could increase the added-value of surplus benzene as well as relieve environmental problems like green-house effect. In this work, the alkylation benzene with carbon dioxide and hydrogen reaction was proceeded by using the mixture of zinc-zirconium oxide and HZSM-5 as bifunctional catalyst. The equivalent of Zn/Zr = 1 displays the best catalytic performance at 425 °C and 3.0 MPa, and benzene conversion reaches 42.9% with a selectivity of 90% towards toluene and xylene. Moreover, the carbon dioxide conversion achieves 23.3% and the carbon monoxide selectivity is lower than 35%, indicating that more than 50% carbon dioxide has been effectively incorporated into the target product, which is the best result as far as we know. Combined with characterizations, it indicated that the Zn and Zr formed a solid solution under specific conditions (Zn/Zr = 1). The as-formed solid solution not only possesses a high surface area but also provides a large amount of oxygen vacancies. Additionally, the bifunctional catalyst has excellent stabilities that could keep operating without deactivation for at least 80 h. This work provides promising industrial applications for the upgrading of aromatics.
研究领域:
催化化学
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环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
COLLOID AND POLYMER SCIENCE
·
2025
·
IF 2.3
Wang Ying,Yang YunXia,Zhu Daliang,Zhang Hongmei,Wang Yanqing
Polysaccharide-based drug delivery systems have gained significant attention due to their biocompatibility and potential for targeted therapy. In this study, we utilized Ganoderma lucidum polysaccharides (GLP) as a macromolecular carrier to synthesize polysaccharide drug conjugates by forming ester bonds with 5-fluorouracil (5-FU) derivatives (5-FUAC). This not only improves the solubility and stability of 5-FU but also enhances its targeted delivery to tumor tissues, potentially reducing systemic toxicity. Utilizing Ganoderma lucidum polysaccharides (GLP) as a macromolecular carrier, we successfully synthesized GLP-5-FU conjugates by forming ester bonds with 5-fluorouracil derivatives (5-FUAC). These conjugates were then characterized using spectrum analysis technologies. The drug loading capacities of 5-FU in the GLP-5-FU conjugates were found to be approximately 4.7%. Morphological observations revealed that the GLP-5-FU conjugates had a regular spherical shape. In terms of drug release, 5-FU was found to be released faster at pH 6.8 compared to pH 7.4. To investigate the dynamic viscoelastic behavior of GLP and GLP-5-FU conjugates in water, dynamic rheology analysis was conducted. In terms of cytotoxicity, the GLP-5-FU conjugates exhibited greater inhibition of proliferation compared to 5-FU and GLP alone in HeLa, 786-O, and SKOV3 cells. Furthermore, the GLP-5-FU conjugates showed lower cytotoxicity to 293A cells. Graphical
研究领域:
药理学
·
生物材料
·
肿瘤学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 16
·11311-11321
·
IF 3.9
Tong Wan,Qianqian Zhang,Guocheng Jin,Shiai Xu
This work aims to determine the optimal conditions for emulsion cross-linking of chitosan (CHS) with various molecular weights using glutaraldehyde as a cross-linking agent to produce 5-fluorouracil-loaded CHS microspheres (5-FU/CHS). Their drug loading and encapsulation efficiencies are found to be in the range of 3.87–12.35% and 20.13–70.45%, respectively. The dynamic light scattering results show that 5-FU/CHS microspheres are micron-sized with a uniform size distribution, and the scanning electron microscopy results show that they are spherical. The results of thermogravimetric analysis, X-ray diffraction, and Fourier transform infrared spectroscopy demonstrate that 5-FU is successfully incorporated into the microspheres. The in vitro release tests show that 5-FU/CHS have a prolonged, pH-responsive release pattern of 5-FU, and the cumulative release rate under acidic condition is much larger than that under neutral conditions. The drug release kinetic analysis further demonstrates that the release of 5-FU can be well described by the Fickian diffusion model.
研究领域:
药剂学
·
生物材料
·
肿瘤治疗
✓ 已验证
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Weiwei Liu,Zichen Yu,Zhichao Chen,Ling Ma,Yanghao Liu,Zhen Zhang,Qingyang Xu
5-Hydroxytryptamine (5-HT), also known as serotonin, plays a critical role in mood regulation, insomnia treatment, and free radical scavenging. Currently, 5-HT production primarily relies on plant extraction, which is challenged by limited raw materials and environmental concerns, emphasizing the need for innovative green production strategies. In this study, we explored a high-performance producer for biosynthesizing 5-HT in Escherichia coli. First, we constructed and optimized the 5-HT biosynthetic pathway to convert L-tryptophan (l-Trp) to 5-HT, avoiding the accumulation of tryptamine and 5-hydroxytryptophan. Moreover, precursor enrichment eliminated the need for l-Trp supplementation and dynamic downregulation of pyruvate kinase balanced growth and production. Further, the metabolic flux between the tetrahydrobiopterin (BH4) module and the hydroxylation-decarboxylation module was optimized, reducing l-Trp accumulation. A novel “GXAA” system was implemented to enhance intracellular NAD(P)H supply, including (1) expression of gdhbsu (glucose dehydrogenase) from Bacillus subtilis, gapXfbr (mutated glyceraldehyde-3-phosphate dehydrogenase) from Corynebacterium glutamicum, and pntAB (pyridine nucleotide transhydrogenase); (2) knockout of ldhA (lactate dehydrogenase). Finally, transcriptomic analysis under high-5-HT stress revealed a potential 5-HT transporter, YhjX. The resulting strain WW15 produced 15.5 g/L 5-HT and a yield of 0.063 g/g glucose through a two-stage fed-batch fermentation, representing the highest titer and yield reported to date.
研究领域:
生物化学
·
合成生物学
·
微生物学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Luxin Ren,Wangchen Huo,Guiying Li,Wonyong Choi,Taicheng An
Photocatalytic oxidation and micropollutants have both attracted extensive attention in the field of wastewater treatment . However, invalidation mechanism of photocatalytic system and target transformation are still a challenge. Here, we used TiO 2 supported on nickel foam (TiO 2 /NF) and 5-fluorouracil (5-FU) as model photocatalyst and pharmaceutical micropollutant to investigate photocatalytic transformation pathways of 5-FU and inhibition mechanisms of its degradation efficiency reduction. Incredibly, removal efficiency of 5-FU dramatically decreased from 80% to 20% after 120 h continuous operation, owning to the competition for hydroxyl radical ( • OH) between trans-intermediates and 5-FU, accumulated in the solution. Using HR-MS, the produced intermediates during photocatalytic degradation of 5-FU were revealed to be that mono/polyhydroxylated compounds, short-chain oxides and carboxylation ones were main trans-intermediates. Combining ATR-FTIR, SEM-EDS and validation experiments for factors, it was found that the inhibition of 5-FU degradation should be contributed to the competition for • OH in the bulk or preferential consumption of • OH in TiO 2 diffusion layer, by the aforementioned intermediates. The present study provides insights into photocatalytic oxidation of 5-FU and basic information about mechanisms of inhibition on target contaminant removal.
研究领域:
环境科学
·
废水处理
·
药物化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2014
·
IF 1.552
Xingcui Guo,Xicheng Wang,Jing Guan,Xiufang Chen,Zhangfeng Qin,Xindong Mu,Mo Xian
Ru particles were introduced into the zeolite ZSM-5 (MFI) by either a conventional impregnation method or a one-step template-free process. The resultant materials were characterized by X-ray diffraction, N 2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, NH 3 and CO 2 temperature-programmed desorption. The results indicated that the Ru species in ZSM-5 catalysts prepared via the latter approach (designated as Ru/ZSM-5-TF) were highly dispersed in the ZSM-5 framework structure and this material exhibited high catalytic performance during the hydrogenation of D-glucose to D-sorbitol. The conversion of D-glucose was as high as 99.6% with D-sorbitol selectivity reaching 99.2%, exceeding the performance of Ru/ZSM-5 catalysts prepared by the conventional impregnation method with microporous or desilicated ZSM-5 supports. More importantly, this catalyst showed high stability against leaching and poisoning and could be reused several times. The extensive dispersion of the Ru species, strong interaction between the Ru species and the ZSM-5, and the suitable surface acidity-basicity balance of the Ru/ZSM-5-TF were all critical factors leading to excellent catalytic behavior and stability.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
International Journal of Chemical Engineering
·
2014
·
IF 0
Hu Li,Qiuyun Zhang,Song Yang
A series of SO3H-functionalized polymers were prepared and employed as heterogeneous catalysts for one-pot transformation of fructose into 5-ethoxymethylfurfural (EMF) that is considered to be one of potential liquid biofuels. A high EMF yield of 72.8% could be obtained at 110°C for 10 h, and the polymeric acid catalysts could be recycled for five times without significant loss of catalytic performance.
研究领域:
化学工程
·
可再生资源
✓ 已验证
产品关联
DOI
FUEL PROCESSING TECHNOLOGY
·
2016
·
IF 3.847
Haian Xia,Siquan Xu,Xiaopei Yan,Songlin Zuo
It is of great significance to explore and develop a cost-effective and environmentally friendly way to covert cellulosic materials into 5-hydroxymethylfurfural (5-HMF). An inexpensive FePO 4 catalyst, which is insoluble at room temperature but can be partially dissolved and behaves as homogeneous catalyst at elevated temperatures, was used to directly convert cellulose into 5-HMF. The effect of various reaction conditions including reaction temperature, reaction time, cellulose concentration and catalyst amount on the conversion of cellulose and 5-HMF yield was investigated. A 5-HMF yield up to 49.5 mol% was achieved at 160 °C for 60 min with the FePO 4 catalyst, which is comparable to the highest yield of 5-HMF obtained in ionic liquid or homogeneous catalysis reaction systems. Moreover, this unique catalyst is readily separated from the aqueous solution via precipitation after cooling to room temperature since it is insoluble at room temperature. The catalyst can be used over five successive cycles although the amorphous FePO 4 underwent the structural transformation from an amorphous phase into a new crystalline form of FePO 4 , evidenced by XRD, IR, and visible Raman spectroscopic results. The soluble iron species, such as Fe 3 + species, act as Lewis acid sites catalyzing isomerization of glucose to fructose followed by the dehydration of fructose into 5-HMF catalyzed by H + ions.
研究领域:
生物质化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）