ACS Applied Energy Materials
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2025
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IF 5.5
Wen-jing Yao,Sheng Liao,Hao-yi Fu,Wen-yi Xu,Meng Xu,Dan Zhao,Chao Chen
The hydrophilic property of the catalytic interface has been seldom focused on particularly, although many green and sustainable catalysis transformations involve water. Addressing the issue, we prepared Dy–Ni–P catalysts for the 5-hydroxymethylfurfural oxidation reaction (HMFOR) to 2,5-furandicarboxylic acid (2,5-FDCA) in this work. The catalysts were clarified as (DyPO4)m/Ni2P composites with molar ratio m within 0.08–0.28 by ICP-OES, XRD, XPS, and HRTEM characterizations. The catalytic performance of samples was comprehensively analyzed by the HPLC technique, 1H NMR spectra, and various electrochemical tests, indicating that the introduction of DyPO4 in a proper amount (m = 0.16) would significantly enhance the catalytic efficiency versus singular Ni2P in terms of 2,5-FDCA yield (91 vs 26%), selectivity (99 vs 47%), and Faradaic Efficiency (F.E.: 98 vs 70%). The enhancements were accompanied by improved kinetic features such as the Tafel slope (53 vs 95 mV dec–1) and intrinsic activity (3.3 vs 1.7 mA cm–2). The boosting endowment (DyPO4)m/Ni2P stands among the top members of reported Ni-based HMFOR catalysts. The promoter effect of DyPO4 was further investigated by H2O-TPD, contact angle, zeta potential, OCP, and EIS measurements. It was testified that the nonhydrophilic Ni2P surface would be converted to a hydrophilic composite interface with the introduction of DyPO4; in line with the essential change, transfer of reactants and activation of water were obviously intensified with the lowered charge transfer resistance along the catalytic interface, which was responsible for the enhanced catalytic behavior of (DyPO4)m/Ni2P versus Ni2P. The above discovery made the topic regarding water indicate that the hydrophilic property of the catalytic interface played a significant role in facilitating heterogeneous catalysis transformations involving water; exampled by the current (DyPO4)m/Ni2P for HMFOR, rare-earth phosphate could be referred to as an outstanding hydrophilic promoter to innovate excellent catalysts for technology-important chemical engineering involving water.
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Journal of Environmental Sciences
·
2024
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IF 5.9
Kaini Ma,Kai Li,Ping Ning,Jiayu Feng,Jiacheng Bao,Lei Shi,Xiangyu Wang,Xin Sun
This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25, 50, 85, 200, and 300, used for the removal of H 2 S in low-temperature, low-oxygen environments. The impact of different Si/Al ratios on the adsorption oxidative performance of Cu 30 /HZSM-5–85 adsorbents was investigated. According to the performance test results, Cu 30 /HZSM-5–85 exhibited the highest breakthrough capacity, reaching 231.75 mg H 2 S/g sorbent . Cu/HZSM-5 sorbent maintains a strong ability to remove H 2 S even under humid conditions and shows excellent water resistance. XRD , BET, and XPS results revealed that CuO is the primary active species, with Cu 30 /HZSM-5–85 having the largest surface area and highest CuO content, providing more active sites for H 2 S adsorption. H 2 -TPR and O 2 -TPD results confirmed that Cu 30 /HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity, contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process. With notable characteristics such as a large surface area, high desulfurization efficiency, and water resistance, Cu 30 /HZSM-5–85 sorbents hold significant importance for industrial applications.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Yangyang Wen,Jie Li,Weiwei Gong,Zhenjia Yu,Hailin Wang,Shiyi Lu,Hongyan Li,Jing Wang,Baoguo Sun
Precise on-site monitoring of alkylresorcinols, a vital biomarker, is crucial for verifying whole wheat foods and accurately quantifying the whole wheat content in various consumer and industrial products. Herein, for the first time, we introduce a novel ratiometric fluorescence sensor (CDs@ZIF-8/CdTe@MIP) for ultrasensitive and selective detection of alkylresorcinols. 5-Heneicosylresorcinol (C21:0 AR), the primary alkylresorcinol homologue in whole wheat grains, was selected as the target analyte. This analyte was specifically and selectively recognized by the incorporation of a molecularly imprinted polymer (MIP) layer. Within this nanoreactor, blue-emitting carbon dots embedded in zeolitic imidazolate framework-8 (CDs@ZIF-8) and orange-emitting CdTe quantum dots served as the self-calibration signal and response signal, respectively. Exploiting a photoinduced electron transfer effect between CdTe and C21:0 AR, the established fluorescence sensor exhibited remarkable sensing performance, offering wide linear responses in 0.005–1 μg·mL–1 and 1–80 μg·mL–1 concentration ranges, and achieving a low detection limit of 1.14 ng·mL–1. The proposed assay effectively detected C21:0 AR in real samples, including 8 whole wheat foods and 19 whole wheat grains, demonstrating good recoveries and relative standard deviation. Furthermore, an intelligent sensing platform was established by integrating CDs@ZIF-8/CdTe@MIP with a smartphone-assisted device, thus validating the feasibility of visual and on-site monitoring of C21:0 AR. Because of its rapid response, portability, cost-effectiveness, superior sensitivity, and high selectivity, the proposed sensor serves as a reliable method for the analysis of C21:0 AR, thus having substantial potential for on-site monitoring of whole wheat foods.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Xiangfei Ding,Youbing Zhu,Ketao Shi,Zhen Xu,Jian Chen,Zengxi Li,Hui Wang
ZSM-5 zeolite is extensively employed for hydrocarbons cracking to generate light olefins, and its acidity is closely related to the activity and product distribution. In this work, Al-Sn bimetallic ZSM-5 was prepared via a “one-pot” route. Characterizations, including XRD, UV–Vis, XPS, revealed that Sn species were mainly embedded into the zeolite framework as tetrahedral Sn (IV). Moreover, the Sn atoms promoted the formation of Lewis acid sites and reduced the Brønsted acid amount, which effectively inhibited occurrence of side reactions ( e.g. , aromatization, hydrogen transfer) and improved the selectivity of light olefins in n-hexane cracking. Light olefins yield over HZ5[100,200] (Si/Al = 100, Si/Sn = 200) reached 33.4 % due to the appropriate acid property, in comparison with only 15.4 % for HZ5[50,∞] (Si/Al = 50, Si/Sn=∞) containing system. Through optimization of reaction conditions, better catalytic performance (n-hexane conversion of 91.6 % and light olefins yield of 37.6 %) was obtained over HZ5[100,200] under 575 °C with WHSV of 2 h −1 .
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Heliyon
·
2024
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IF 3.4
Changhong Wu,Jie Yang,Chenxiao Ye,Hui Wu,Wenxi Shu,Rongrong Li,Sihan Wang,Yi Lu,Haitao Chen,Zewei Zhang,Qinghua Yao
Background 5-Fluorouracil (5-Fu), a prominent chemotherapeutic agent for colorectal cancer (CRC) treatment, is often associated with gastrointestinal toxicities, particularly diarrhea. Our previous study demonstrated that berberine (BBR) ameliorates 5-Fu-induced intestinal mucosal injury by modulating the gut microbiota in rats. Nevertheless, the precise molecular mechanism underlying BBR's protective effect on intestinal mucosa remains elusive, and its impact on the anti-tumor efficacy of 5-Fu warrants further investigation. Methods The effect of BBR on 5-Fu-induced intestinal mucosal injury was investigated using a tumor-bearing murine model, employing H&E staining, 16 S rDNA sequencing, transcriptome sequencing, Western blot analysis, cell experiments and constructing a pseudo-germ-free tumor xenograft model. Result Our findings demonstrate that BBR alleviates intestinal mucosal damage, reduces the levels of inflammatory factors (IL-6, TNF-α, and IL-1β), and inhibits epithelial cell apoptosis in 5-Fu-treated mice without compromising 5-Fu's anti-tumor efficacy. Moreover, 16 S rDNA sequencing indicated that BBR significantly increases the abundance of Akkermansia and decreases the abundance of pathogenic bacteria Escherichia/Shigella at the genus level. Mechanistically, transcriptome sequencing and Western blot analysis confirmed that BBR upregulates PI3K/AKT/mTOR expression in the intestinal mucosa. However, this effect was not observed in tumor tissues. Notably, BBR did not demonstrate a direct protective effect on 5-Fu-treated CCD841 and SW480 cells. Additionally, BBR had no effect on the PI3K/AKT/mTOR pathway in the intestinal tissue of the 5-Fu-treated mouse model with a depleted gut microbiota. Conclusion This study indicates that BBR alleviates 5-Fu-induced intestinal mucosal injury by modulating the gut microbiota and regulating the PI3K/AKT/mTOR signaling pathway without compromising the anti-tumor efficacy of 5-Fu.
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Clean Energy
·
2025
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IF 3.7
Jiang Zhenhua,Xia Wei,Zhang Yanli,Wang Xinrui,Dong Mingyuan,Chen Kun,Liu Dong,Lu Baowang
This study aims to compare the catalytic performance of ZSM-5 and SAPO-34 zeolite catalysts in the conversion of ethanol. Through experiments conducted at different temperatures (773 K and 673 K), it was found that SAPO-34 initially exhibits superior propylene selectivity compared to ZSM-5. However, the propylene yield on SAPO-34 gradually decreases, while the ethylene yield increases with time on stream. density functional theory calculations were employed for the investigation of reaction mechanism. The results indicate that the SAPO-34 catalyst surface favors propylene desorption, which beneficial for its initial high propylene selectivity. Nevertheless, the smaller pore structure of SAPO-34 limits the effective diffusion of products, leading to product accumulation within the pores and potentially causing catalyst coking and deactivation. By combining the experimental results with theoretical calculation, this study not only explored the selectivity difference between SAPO-34 and H-ZSM-5 in ethanol conversion reaction, but also revealed the influence of different molecular sieve catalyst structures on product distribution and catalyst stability.
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Journal of Water Process Engineering
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2024
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IF 6.3
Jing Li,Suxia Ma,Nuo Xu
The pursuit of carbon peaking and carbon neutrality goals necessitates flexible operation and deep peaking of coal-fired units, thus placing heightened demands on nitrogen oxide (NO X ) emission control. Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), should be fully leveraged, and the high-value synthesis of zeolite represents a viable utilization method. In this context, fly ash-based zeolite was prepared as a catalyst to facilitate the generation of active oxides from H 2 O 2 , combined with alkali solution absorption, to achieve efficient denitrification. This approach effectively transforms ‘waste to pollution’ mitigation. The optimal synthesis conditions for FA-ZSM-5 zeolite were established using the alkali fusion hydrothermal synthesis method, with fly ash as the raw material. The specified conditions were NaOH/FA = 1.2, SiO 2 /Al 2 O 3 = 40, H 2 O/Al 2 O 3 = 1325, TPAOH/Al 2 O 3 = 10, ZSM-5-seed addition of 5 %, and a hydrothermal temperature and time of 140 °C for 24 h. Experimental parameters were meticulously investigated to ascertain their impact on nitric oxide (NO) removal efficiency. The highest removal efficiency was achieved under specific conditions: a reaction temperature of 140 °C, an H 2 O 2 concentration of 6 %, a catalyst dose of 0.3 g, an NO concentration of 600 mg/m 3 , and an SO 2 concentration of 1000 mg/m 3 . Finally, analysis of the catalytic oxidation mechanism revealed that H 2 O 2 , when catalyzed by FA-ZSM-5 zeolite, generates ·OH radicals with strong oxidizing properties, thereby facilitating the oxidative removal of NO.
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Chem Catalysis
·
2024
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IF 11.5
Bin Chen,Shui Yang,Longmei Shang,Yiling Wu,Youting Wang,Jian Tian,Jiale Huang,Xiaodong Zhang,Qingbiao Li,Guowu Zhan
Biomass resources can be converted to biochemicals via the catalytic pyrolysis process, but conventional catalysts often suffer from severe deactivation due to coke formation. Here, a ternary Ni/bio-Z5 catalyst was constructed by integrating ZSM-5 and Ni components on a porous bio-SiO2 platform derived from rice husk. The Ni/bio-Z5 achieved 76% aromatic selectivity for the catalytic pyrolysis of soybean oil, corresponding to a space-time yield as high as 154.8 garom · h−1 · gcata−1. It is confirmed that the bio-SiO2 platform shortened the surface diffusion path of aromatics by co-diffusion, which then inhibited coke formation and significantly improved the catalyst stability. Moreover, the atomically dispersed Ni on ZSM-5 effectively promotes the aromatization of C2=-C6= by enhancing adsorption and acting as an oligomerization center for isoalkyl carbenium ions. The coupling of deoxygenation and aromatization reactions promotes the enhancement of aromatic selectivity through the formation of methyl-substituted cyclopentenone that can be readily converted to aromatics.
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BIORESOURCE TECHNOLOGY
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2019
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IF 6.669
Caidi Jin,Ming Yang,Shuang E,Jianglong Liu,Shen Zhang,Xiaoliang Zhang,Kuichuan Sheng,Ximing Zhang
One-step fractionation with concentrated formic acid at elevated temperatures with short retention time was investigated for corn stover valorization. Crude pulp (CP) with high purity of cellulose and FA-lignin (FAL) with high guaiacyl content were fractionated through one-step mild pretreatment. Formylation reaction on both CP and FAL fractions occurred during the pretreatment and improved the hydrophobicity and thermal stability of CPs and FALs. The presence of formyl group on CPs significantly inhibited the enzymatic hydrolysis efficiency for sugar production, however, the formylated cellulose showed super high reactivity and selectivity for HMF production through catalysis by maleic acid and aluminum chloride in acetonitrile-water co-solvent system. In addition, the fractionated FAL fraction exhibited a loose structure which is prominent for its further catalytic conversion into chemicals and energy.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
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IF 3.8
Ne Ni,Ying Ouyang,Jianqiang Liu,Enhui Xing,Yibin Luo,Xingtian Shu
It was the thermostability and acidity of P precursors that influenced the interaction between P species and framework Al to determine the hydrothermal stability of P modified ZSM-5. With H3PO2 and NH4H2PO2 as P precursors, the P–Al interactions of P modified ZSM-5 samples calcined under different temperatures were systematically investigated by X-ray fluorescence, X-ray photoelectron spectroscopy, 27Al, and 31P MAS NMR spectroscopy, and temperature-programmed desorption of NH3 (NH3-TPD). With H3PO2 as the precursor, lower calcination temperature favored less self-polymerization of P species; however, obvious loss of phosphorus was observed during hydrothermal treatment. Conversely, higher calcination temperature tended to result in excessive interaction between P and framework Al for dealumination. Therefore, moderate interactions between P and framework Al were obtained over H3PO2 modified ZSM-5 calcined at 350 °C, which contributed to weaken the self-polymerization of P species. Compared with H3PO2, neutral NH4H2PO2 generated a relatively weaker P-zeolite interaction, which was less affected by the calcination temperature.
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ADVANCED POWDER TECHNOLOGY
·
2024
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IF 4.2
Han Hao,Tiantian Ren,Cuilu Quan,Wei Guo,Jing Wang
Pharmaceutical cocrystal is an emerging strategy not only to improve physicochemical properties, but also to generate synergistic effects. In this work, a novel cocrystal composed by 5-fluorouracil (5-FU) and sarcosine (SAR) was successfully assembled by wet powder grinding method. The cocrystal was characterized by single crystal X-ray diffraction (SCXRD), powder X-ray diffraction (PXRD), differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR) and Raman spectra. The differences of 1 H NMR spectroscopy between 5-FU/SAR physical mixture (PM) and cocrystal hinted the existence of supramolecular interactions between 5-FU and SAR in solid and solution. Bioavailability of cocrystal was increased than 5-FU. Most importantly, the weak interactions between 5-FU and SAR in cocrystal solution induced the superior cellar inhibition activity on 4T1 and BEL-7402 cells compared than 5-FU and PM. Cocrystal can interfere with the stability of methionine cycle and tetrahydrofolate (FH 4 ) level through the SAR-Gly-Met pathway, enhance the inhibition of thymidylate synthase (TS) compared to 5-FU, thereby interfering with cell cycle and inducing cell apoptosis. The results provided the novel strategy to develop the cocrystal drugs using bioactive amino acids as precursors to enhance the efficacy.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zhen-Qiang Yu,Yao-Xin Xiao,Dong Liang,Che Zhao,Zhen Huang,Gang-Qi Cheng,Rui Shan,Hao-Ran Yuan,Yong Chen
The chemical upgrade of the waste polyester coating on the surface of aluminum cans to value-added products can not only decrease the release of toxic substances, but also improve the quality of aluminum in the recycling process. In this study, different types of zeolite molecular sieve catalysts loaded with Ni, Mo and Co were synthesized, and utilized in the rapid catalytic pyrolysis of polyester coating. Among them, the Ni/ZSM-5 achieved the maximum aromatic compounds yield of 68.43 % at 600 ℃. A series of characterization results demonstrated that the embedding of transition metals (like Ni) could promote the cyclization and aromatization of products through deoxidation and dehydrogenation reactions by changing the pore structure and increasing total acid content (Brønsted and Lewis acids) of the ZSM-5 molecular sieve. Meanwhile, the thermodynamics of polyester coating during catalytic pyrolysis was studied by thermogravimetric method. The average activation energy of Ni/ZSM-5 catalytic pyrolysis of polyester coating is 238.65 kJ/mol. Furthermore, even after being reused for over 5 cycles, the catalyst can still maintain a relatively high yield of aromatic compounds (exceeding 60 %). Finally, the mechanism for aromatic compounds formation from Ni-modified ZSM-5 in-situ catalyzed polyester coating pyrolysis was proposed. This work provided useful ideas for the subsequent treatment of solid wastes.
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