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
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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
·
环境科学
·
材料科学
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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
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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
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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
BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Lishi Yan,Ruoshui Ma,Huaixin Wei,Liangzhi Li,Bin Zou,Yiwen Xu
The production of 5-hydroxymethylfurfural (5-HMF) from cellulose catalyzed by a series of transition metal chlorides (i.e. FeCl 3 , RuCl 3 , VCl 3 , TiCl 3 , MoCl 3 and CrCl 3 ) was studied in biphasic system. RuCl 3 was the most efficient catalyst among these transition metal chlorides for 5-HMF production, and resulted in both the highest yield of 83.3% and selectivity of 87.5% in NaCl-aqueous/butanol biphasic system. XRD analysis and FTIR spectroscopy were applied to further characterize the RuCl 3 catalyzed cellulose slurries to reveal the catalytic reaction mechanism. Results demonstrated that RuCl 3 enhanced the decrystallization and cleavage of C O C bonds in cellulose, promoted the subsequent dehydration of glucose into 5-HMF, while suppressed the glucose retro -aldol reaction to byproduct lactic acid. In addition, with the assistance of NaCl-aqueous/butanol biphasic system, 5-HMF further degradation was limited and thusly maintained a desired 5-HMF yield. This proposed approach provides an efficient strategy for one-pot conversion of cellulose into 5-HMF.
研究领域:
化学工程
·
可再生资源转化
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yu Zhou,Ning Li,Caiping Ma,Xiaohua Shen,Xiaofeng Li,Baojun Wang,Lixia Ling
Ga-ZSM-5 zeolite has excellent performance for methanol to aromatics (MTA) reactions, but introducing Ga metal into ZSM-5 zeolite leads to a complex acid species. The present study investigated the effect of Ga metal content on the acid amount and MTA reaction products in the hydrothermal synthesis of Ga-ZSM-5 zeolite. Lewis acid mainly formed at a Ga/Al ratio below 2.0, and at a Ga/Al ratio higher than 2.0, framework Ga species formed, increasing Brønsted acid content. Ga 2.0 -ZSM-5 zeolite exhibited the lowest B/L acid ratio (0.48), excellent BTX selectivity (40.26%), and the highest H 2 selectivity (8.93%). This finding indicates the most pronounced synergistic hydrogenation of Brønsted and Lewis acids. Ga 3.0 -ZSM-5 produced more xylene with more Brønsted acid compared to Ga 1.0 -ZSM-5, although they both had the same B/L acid ratio. The alterations in acidic species at different content of Ga metal appear to be conducive to the regulation of acidity in Ga-ZSM-5 zeolites.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2021
·Vol. 13
·期 13
·2096
·
IF 4.329
Ke Ke,Hairui Ji,Xiaoning Shen,Fangong Kong,Bo Li
5-hydroxymethylfurfural (HMF) obtained from biomass is an important platform chemical for the next generation of plastics and biofuel production. Although industrialized, the high yield of HMF in aqueous systems was rarely achieved. The main problem is that HMF tends to form byproducts when co-adsorbed with water at acid sites. In this study, the pressure was reduced to improve the maximum yield of HMF from 9.3 to 35.2% (at 190 °C in 60 min) in a glucose aqueous solution. The mechanism here involved water boiling as caused by pressure reduction, which in turn promoted the desorption of HMF from the solid catalyst, thereby inhibiting the side reaction of HMF. Furthermore, the solid catalysts could be reused three times without a significant loss of their catalytic activity. Overall, this work provides an effective strategy to improve the yield of HMF in water over heterogeneous catalysts in practice.Keywords:glucose;5-hydroxylmethyfurfural;aqueous phase;heterogeneous catalysts;pressure reduction
研究领域:
化学工程
·
生物化工
·
可再生能源
✓ 已验证
DOI
PubMed
高影响因子
Processes
·
2025
·Vol. 13
·期 5
·1440
·
IF 2.8
Tongtong Zhang,Sijia Wang,Xingyuan Li,Yupeng Du,Jiajun Hu,Shi Jiang,Yu Guo
Room-temperature complete oxidation of formaldehyde (HCHO) is an important orientation of research programs, yet challenges remain. The development of efficient catalysts with high activity and excellent stability is of great significance for such practical application. Inspired by this whole catalytic process, we, therefore, chose HZSM-5 zeolite with abundant acidic sites as catalyst support and lactic acid (LA) as modifier to regulate the properties. The use of LA simultaneously enhances the hydroxyls density and increases the dispersion of Pt nanoparticles, which are better than the reference catalyst prepared via direct wetness impregnation method. Most satisfying of all, the lactic acid-modified HZSM-5-supported Pt catalyst demonstrates a remarkable reaction performance for room-temperature HCHO oxidation at a high concentration HCHO of 80 ppm and a large space velocity of 360,000 mL/g/h (especially with a low Pt loading of 0.5%). In addition, a 120 h test further confirms the favorable stability of the designed catalyst. This pre-modified strategy using organic acid might provide potential approach in the construction of efficient zeolite-supported catalysts.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 12
·1120
·
IF 4
Peng Yang,Hualei Hu,Yong Yang,Guojun Lan,Soliman I. El-Hout,Qianquan Fang,Guowen Lu,Chunlin Chen,Jian Zhang
The nano-metal oxide-catalyzed oxidation of 5-hydroxymethylfurfural (HMF) with sodium hypochlorite (NaClO) is an effective and mild technique for synthesizing 2,5-furanediformic acid (FDCA). However, the rapid and large-scale separation of nanocatalysts remains a major challenge. In this study, we developed a magnetic and recyclable copper oxide-based catalyst supported on the mechanochemically synthesized Fe3O4. Benefiting from the introduction of the Fe3O4carrier and cetyltrimethylammonium bromide (CTAB) surfactant, the CuO-CTAB/Fe3O4catalyst owns smaller CuO particle sizes, which endows it with excellent catalytic activity in the oxidation of HMF, achieving a high FDCA yield of 90.3%. Furthermore, the rapid magnetic separation of the catalyst effectively inhibits the excessive conversion of FDCA. The recovered catalyst can be reused for at least five cycles without significant loss of catalytic performance, confirming the promising application prospect of the CuO-CTAB/Fe3O4catalyst.
✓ 已验证
产品关联
DOI
高影响因子
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