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FUEL · 2025 · IF 7.5

Hydroxyl engineering of precipitated silica to construct hierarchically layered ZSM-5 zeolites for efficient methanol-to-propylene

Ke Yan,Yimin Zhang,Xinyu Xu,Yucai Qin,Yi Mei,Yun Zu

Non-classical crystallization pathways have emerged as a pivotal strategy for the synthesis of zeolites with tailored structures, with the initial feed composition being one of the most critical factors influencing this process. As primary raw material for the formation of zeolite networks, the physicochemical properties of Si sources significantly affected structural and acid properties of zeolites via non-classical crystallization pathways. While, the present operating mechanism between each other was still confusing. In this work, the precipitated silica with tunable Si-hydroxyls was home-made using one-step synthesis of fluorosilicic acid and ammonia aqueous in a SK static reactor. Leveraging this tailored silica, a series of hierarchically layered L-ZSM-5 zeolites were successfully prepared by a non-classical crystallization pathway regulated by Si-hydroxyl engineering. The findings revealed a linear positive correlation between the percentage of layered structures and framework single Al distribution of L-ZSM-5 zeolites and the number of silanol nests present in the precipitated silica. Under comparable conditions, the as-prepared hierarchical L-ZSM-5(7/6) zeolite with more layered structures and framework Al located in the straight/sinusoidal channels exhibited excellent propylene selectivity (44.09 %) and reaction lifetime (25 h, WHSV = 6 h −1 ) in methanol-to-propylene reaction. This work elucidates a decisive relationship between Si-hydroxyls engineering and zeolite crystallization, offering novel insights into the synthesis of zeolites with specific structural features through non-classical crystallization pathways.

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CERAMICS INTERNATIONAL · 2024 · IF 5.1

In vitro controlled release of 5-aminosalicylate from ZnAl-NO3(-CO3) layered double hydroxide drug delivery system

Jichao Zhu,Xianli Dong,Kunhao Li,Siyu Tian,Yao Kong,Weitong Chen,Shuping Zhou

In the field of pharmaceutical research and development, the development of nano drug carriers based on intercalation structures has become one of the important development directions. Hydrotalcite (LDHs) and its derivatives have the advantages of low cost, simple synthesis, high drug loading efficiency, good biocompatibility, and easy degradation, and have received widespread attention in the field of biomedicine. Based on this, we synthesized 5-aminosalicylate (5-ASA) intercalated NO 3 based and CO 3 based ZnAl-LDHs drug delivery systems using ion-exchange and chemical co-precipitation methods, respectively. The crystalline structure, morphology, thermal stability, and host-guest interaction were characterized in detail by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), Ultraviolet visible spectroscopy (UV), Scanning electron microscopy (SEM), Thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopic (XPS). The drug loading, drug release behavior and release kinetic of 5-ASA intercalated ZnAl-LDHs were studied. The characterization results indicated that the intercalation mode of the drug and the strength of the host-guest interaction are related to the interlayer anion type and synthesis process of ZnAl-LDHs. The amount of 5-ASA loaded into LDHs from an ion-exchange process was 28.6 and 13.8 wt% for NO 3 − and CO 3 2− based LDHs, respectively, whereas it was 6.9 and 10.4 wt% for co-precipitation process. The modeling kinetics results indicated that the release process of 5-ASA by ZnAl-LDHs intercalated with 5-ASA conforms to the parabolic diffusion model. These results indicated that the drug delivery system was controlled by diffusion of 5-ASA ions into aqueous solution through exchange with phosphate anions.

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Catalysts · 2024 ·Vol. 14 ·期 7 ·397 · IF 3.8

In Situ Growth of Mn-Co3O4 on Mesoporous ZSM-5 Zeolite for Boosting Lean Methane Catalytic Oxidation

Yuxuan Zhang,Ruibo Wei,Lin Yang,Jinming Ge,Feiyang Hu,Tingting Zhang,Fangyin Lu,Haiwang Wang,Jian Qi

The low-temperature oxidation of methane gas in coal mine exhaust gas is important for reducing the greenhouse effect and protecting the environment. Unfortunately, the carbon–hydrogen bonds in methane molecules are highly stable, requiring higher reaction temperatures to achieve effective catalytic oxidation. However, metal oxide-based catalysts face the problem of easy sintering and the deactivation of active components at high temperatures, which is an important challenge that catalysts need to overcome in practical applications. In this work, a series of Mn-Co3O4active components were grown in situ on ZSM-5 zeolite with mesoporous pore structures treated with an alkaline solution via a hydrothermal synthesis method. Due to the presence of polyethylene glycol as a structure-directing agent, manganese can be uniformly doped into the Co3O4lattice. The large specific surface area of ZSM-5 zeolite allows the active component Mn-Co3O4to be uniformly dispersed, effectively preventing the sintering and growth of active component particles during the catalytic reaction process. It is worth mentioning that the Mn-Co3O4/meso-ZSM-5-6.67 catalyst has a methane conversion rate of up to 90% at a space velocity of 36,000 mL·g−1·h−1and a reaction temperature of 363 °C. This is mainly due to the mesoporous ZSM-5 carrier with a high specific surface area, which is conducive to the adsorption and mass transfer of reaction molecules. The active component has an abundance of oxygen vacancies, which is conducive to the activation of reaction molecules and enhances its catalytic activity, which is even higher than that of noble metal-based catalysts. The new ideas for the preparation of metal oxide-based low-temperature methane oxidation catalysts proposed in this work are expected to provide new solutions for low-temperature methane oxidation reactions and promote technological progress in related fields.

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AICHE JOURNAL · 2024 · IF 3.5

Lithium solvent extraction from weak alkaline brine by 2-hydroxy-5-nitro-4-alkoxy-benzophenone and TRPO

Guimei Zhou,Wenjun Yan,Shufan Yan,Dandan Gao,Debin Zeng,Dongdong Li,Dewen Zeng

Solvent extraction of lithium by β-diketones from alkaline brine has been known to be an efficient process. However, its relatively high working pH, consequently the high alkaline consumption and substantial dissolution loss in raffinate, limit its industrial application. Herein, a novel lithium extractant, i.e., 2-hydroxy-5-nitro-4- n -octoxy-benzophenone (referred to as N531), was proposed, which can extract lithium at relatively lower pH with remarkable low alkaline consumption and dissolution loss. Exactly, the pH corresponding to half lithium extraction is 8.5, and the Li/Na separation factor is ~500. The extractant concentration in the raffinate varied from 0.8 to 9.3 mg L −1 , depending on the pH and salinity. An application case was given to extract lithium from the raw brine of Zabuye salt lake, indicating that N531 is a commercially prospective extractant to extract lithium from alkaline brine.

CAS / MDL: 112-40-3 100786-00-3
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Controllable boosting activity on Co4N by Fe substitution for oxygen evolution reaction and efficient 5-hydroxymethylfurfural oxidation

Liyan Wang,Zhaokun Wang,Liang Chu,Mu Yang,Ge Wang

The design of transition metal nitrides with excellent oxygen evolution reaction and 5-hydroxymethylfurfural oxidation reaction (HMFOR) is of great significance to achieve the goal of "carbon peaking and carbon neutrality". Herein, Fe-doped bimetallic nitride Fe x Co 1-x ) 4 N was prepared by a simple electron regulation strategy. The introduction of Fe changes the electronic structure of Co and optimizes the adsorption energies of *OH, reduces the potential barrier for the generation of *OOH as a potential-determining step and thus increases the intrinsic OER activity of Co 4 N. In addition, Fe substitution of some of the Co atoms gives (Fe x Co 1-x ) 4 N a higher electrochemical active surface area, which accelerates the electron transfer efficiency and improves the electrical conductivity. The overpotential for (Fe x Co 1-x ) 4 N-0.9 to reach a current density of 10 mA cm −2 in 1 M KOH is only 271 mV. When in 1 M KOH + 50 mM HMF condition, (Fe x Co 1-x ) 4 N-0.9 requires only 1.37 V to reach a current density of 10 mA cm −2 . This work provides practical guidance for developing bifunctional transition metal electrocatalysts with excellent OER and HMFOR activity.

CAS / MDL: 10026-22-9 7782-61-8
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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Dual-metal synergy unlocking ROS-free catalysis for rapid aerobic oxidation of 5-hydroxymethylfurfural at room temperature

Meiyun Zhang,Penghua Che,Hong Ma,Xin Liu,Shujing Zhang,Yang Luo,Jie Xu

Clean catalytic oxidation has a broad prospect in the modern chemical engineering and energy chemistry fields. However, unexpected over-oxidation and disruptive degradation are frequently induced by excessive reactive oxygen species (ROS). Herein, we reported a new ROS-free approach to effectively drive O 2 to be activated into highly reactive surface peroxo species through enzyme-mimicking mechanism. Benefiting from the dual-metal synergy effect between Cu and Co active sites, ROS (H 2 O 2 and OH • ) is generated in situ while further scavenged completely into surface peroxo species, which gives rise to very high selectivity and extremely high carbon balance. For example, the CuCo/N-C catalyst affords >99.8% conversion and 94.5% selectivity to 2,5-furanedicarboxylic acid at 25 °C for 6 h in the aerobic oxidation of biomass platform 5-hydroxymethylfurfural. Moreover, it achieved exceptional performance in the oxidation of a variety of hydroxyl compounds to organic acids with high yields (89.9%–99.5%) at a mild temperature (25–40 °C). This exploration introduces an innovative clue for emulating enzyme catalysts, thereby enriching our comprehension and advancement of biologically inspired catalytic oxidations.

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ANTIVIRAL RESEARCH · 2024 · IF 4.5

Drug delivery system based on metal-organic framework improved 5-Fluorouracil against spring viremia of carp virus

Liang Zhao,Wei-Ze Wang,Tian-Tian Jiang,Tian-Zi Sun,Bo Liu,Bin Zhu

Spring viremia of carp virus (SVCV), as a high pathogenicity pathogen, has seriously restricts the healthy and sustainable development of cyprinid farming industry. In this study, we selected 5-Fluorouracil (5-Fu) as the drug model based on zeolitic imidazolate framework-8 (ZIF-8) to construct a drug delivery system (5-Fu@ZIF-8), and the anti-SVCV activity was detected in vitro and in vivo . The results showed 5-Fu@ZIF-8 was uniform cubic particle with truncated angle and smooth surface, and the particle size was 90 nm. The anti-SVCV activity in vitro results showed that the highest inhibition rate of 5-Fu was 77.93% at 40 mg/L and the inhibitory concentration at half-maximal activity (IC 50 ) was 20.86 mg/L. For 5-Fu@ZIF-8, the highest inhibition rate was 91.36% at 16 mg/L, and the IC 50 value was 5.85 mg/L. In addition, the cell viability was increased by 18.1% after 5-Fu treatment. Similarly, after 5-Fu@ZIF-8 treatment, the cell viability increased by 27.3%. Correspondingly, in vivo experimental results showed the viral loads reduced by 18.1% on the days 7 and the survival rate increased to 19.4% at 80 mg/L after 5-Fu treatment. For 5-Fu@ZIF-8, the viral loads reduced by 41.2% and the survival rate increased to 54.8%. Mechanistically, 5-Fu inhibits viral replication by regulating p53 expression and promoting early apoptosis in infected cells. All results indicated that 5-Fu@ZIF-8 improved the anti-SVCV activity; it may be a potential strategy to construct a drug-loaded system with ZIF-8 as a carrier for the prevention and treatment of aquatic diseases.

CAS / MDL: 67-68-5 67-56-1
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Molecular Catalysis · 2025 · IF 4.9

Direct oxidation of methane to methanol over copper and zinc synergistic co-modified H-ZSM-5 catalyst

Shengxin An,Shuaibo Zhao,Jingting Jin,Tao He,Yuhao Wang,Na Kong,Jie Zhou,Wenzhi Li

Great expectations have been placed on bimetallic co-modified zeolite for the direct oxidation of methane to methanol. In this work, H-ZSM-5 zeolite was modified with bimetallic copper and zinc via ion-exchange method. Numerous experiments were conducted and the methanol yield of 44,302.70 μmol·g cat −1 ·h −1 was obtained over 1Cu/2Zn-ZSM-5 catalyst. A series of characterization analyses confirmed that the introduction of Zn increased the proportion of active Cu species bound to extra-framework oxygen by altering the electronic state of copper. The bis (μ-oxo) dicopper ligand was identified as the active site for methane oxidation. The possible reasonable reaction pathway was the free radical reaction. This work provides a valuable guidance for the preparation of co-modified zeolite catalysts for the direct oxidation of methane to methanol.

CAS / MDL: 10031-43-3
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2024 · IF 3.7

Cost-effective bifunctional lignin-derived carbon supported tin oxide with efficient production of 5-hydroxymethylfurfural from glucose

Sien Yan,Linhuo Gan,Kui Wang,Kang Sun

5-Hydroxymethylfurfural (5-HMF) is one of the important bio-based platform compounds, and the catalytic conversion of glucose to 5-HMF is a highly desirable approach that is receiving increasing attention. Herein, we reported the synthesis of lignin-derived carbon supported tin oxides (SnO x /LC) catalyst via a two-step hydrothermal-pyrolytic method using wheat straw alkali lignin as a cost-effective carbon source with high carbon content. The key preparation conditions of catalyst and its catalytic conditions for the conversion of glucose to 5-HMF were investigated, respectively. Results show that under the preparation conditions of tin tetrachloride dosage of 3.0 mmol and pyrolysis temperature of 500°C, the optimized catalyst (3.0-SnO x /LC-500) with a high yield of 63.4% exhibits good catalytic performance of 5-HMF yield of 50.1% and reaction selectivity of 86.0% under the optimum conditions of reaction temperature and time of 190°C and 3 h, initial glucose concentration of 10 wt%, 3.0-SnO x /LC-500 dosage of 100 mg in a biphasic solvent system of volume ratio of water to tetrahydrofuran of 1:4. In addition, 3.0-SnO x /LC-500 exerts an excellent reusability in five-cycle experiment. Furthermore, SnO x /LC was characterized in detail using X-ray diffraction patterns (XRD), X-ray Photoelectron Spectroscopy (XPS) Brunauer-Emmett-Teller (BET), ammonia temperature-programmed-desorption (NH 3 -TPD), pyridine adsorption infrared spectroscopy (Py-FTIR), scanning electron microscope (SEM) and thermal gravimetric analysis (TGA). Results indicate that Brønsted acid sites and Lewis acid sites coexist on 3.0-SnO x /LC-500, and more Sn 4+ as well as proper ratio of weak acidity to medium acidity are conductive to its catalytic performance in glucose-to-5-HMF reaction.

CAS / MDL: 50-99-7 67-47-0
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CARBOHYDRATE RESEARCH · 2012 · IF 2.332

Selective dehydration of fructose to 5-hydroxymethylfurfural catalyzed by mesoporous SBA-15-SO3H in ionic liquid BmimCl

Xingcui Guo,Quan Cao,Yijun Jiang,Jing Guan,Xiaoyan Wang,Xindong Mu

Mesoporous SBA-15 materials functionalized with propylsulfonic acid groups (SBA-15-SO 3 H) were synthesized through a conventional one-pot route. It was used as a catalyst for the selective synthesis of 5-hydroxymethylfurfural (HMF) from the dehydration of fructose using BmimCl as solvent. Reaction time, temperature and fructose concentration were investigated during the HMF synthesis procedure. The catalyst SBA-15-SO 3 H exhibits high fructose conversion (near 100%) and HMF selectivity (about 81%) with good stability in the HMF synthesis. It was a suitable catalyst to produce HMF from renewable carbohydrates in potential industrial process.

CAS / MDL: 4420-74-0 78-10-4
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS · 2024 · IF 4.3

Catalytic degradation of Reactive Black 5 through peroxymonosulfate activation with Co organic frameworks combined with graphite oxide

Qian Zhang,Ruo Yu Yin,Zhi Huang,Yan-ying Liu,Jun-ming Hong

The development of high-efficiency catalysts for peroxymonosulfate (PMS) activation is critical for pollutant treatment in environmental applications. In this research, a Co organic framework (CoHHTP) combined with graphene oxide (GO) (CoHHTP/GO) with a 2D structure was prepared for PMS activation to treat the azo dye Reactive Black 5 (RBK5). The combination of CoHHTP and GO via oxygen groups resulted in the high activity of CoHHTP/GO, and almost 100 % performance was achieved within 30 min under various pH, temperature, PMS loading, and catalyst loading conditions. The maximum RBK5 removal efficiency was obtained with a catalyst loading of 3.0 g L −1 , PMS loading of 0.5 mM, temperature of 25 °C, and pH of 6 with a pseudo-first-order kinetics k value of 0.1903 min −1 . The activation energy of the CoHHTP/GO/PMS/RBK5 system was calculated to be 14.34 kJ mol −1 . Meanwhile, radicals and nonradicals, including SO 4 ·− , ·OH, ·O 2 − , and 1 O 2 , were proven to be generated and involved in RBK5 degradation. Moreover, RBK5 degradation pathways were identified through experimental research and density functional theory calculation.

CAS / MDL: 7782-42-5 71-00-1
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CATALYSIS LETTERS · 2024 · IF 2.3

Low-Temperature Plasma Modification of Lignin-Derived Carbon Solid Acid Catalyst for Catalytic Production of 5-HMF

Lv Shijun,Deng Xiaoya,Zhu Peiwen,Ruan Lingyu,Tao Yuheng,Wang Liqun,Zhu Jie,Qing Qing

Sulfonated carbon catalysts exhibit superior catalytic performance for production of biobased chemicals, but the catalyst preparation approaches are still suffered from high corrosion and possible pollution risks. In this paper, lignin extracted from corn stover was used to prepare lignin-based activated carbon, which was then subjected to grafting modification by sulfur dioxide nonthermal plasma method to construct a novel lignin-derived solid acid catalyst (LP-LDSA). The catalytic performances of LP-LDSA were further determined by dehydration of fructose to produce 5-HMF in a biphasic solvent system composed by dimethyl sulfoxide (DMSO) and water. Under the optimal conditions, the 5-HMF yield and reaction selectivity were 88.9% and 89.4%, respectively. This LP-LDSA catalyst also exhibited excellent stability and reusability in five sequential reaction batches. This method has advantages of shorter solid acid preparation duration, lower energy consumption, and higher catalytic stability, presenting an innovative and green method for sulfonation production of solid acid catalyst. Graphical Abstract

CAS / MDL: 64-18-6 67-47-0 123-76-2
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