ENERGY
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2024
·
IF 9
Bingshuo Li,Aorong Ding,Tianhua Yang,Zhuo Wang,Haijun Zhang,Xingping Kai,Rundong Li
Hydrodeoxygenation (HDO) of phenols has significant potential for the synthesis of cycloalkane. In this study, a Ni-based magnetic molecular sieve catalyst, Ni/HZSM-5@SiO 2 @Fe 3 O 4 , was carefully prepared and systematically characterized using various analytical methods. A screening of the HDO reaction conditions was carried out using a typical phenolic compound of 4-ethylphenol. Under the optimal reaction conditions (240 °C, 3 h) with n-dodecane as the solvent, the 6 % Ni/HZSM-5@SiO 2 @Fe 3 O 4 catalyst showed excellent performance, achieving a 4-ethylphenol conversion of 59.3 % and an ethylcyclohexane selectivity of 85.1 %. In comparison to conventional Ni/HZSM-5, the magnetic micromesoporous molecular sieve catalyst exhibited superior catalytic activity, alkane selectivity and recyclability, with a catalyst recovery ratio of 95 %. Furthermore, the effect of liquid-solid mass transfer efficiency on the ethylcyclohexane selectivity considering of the stirring speed was studied, and the selectivity was increased from 81.6 to 85.1 % when the speed was increased from 400 to 600 rpm. This finding was further substantiated by Fluent numerical simulation. To elucidate the HDO pathway of 4-ethylphenol on Ni/HZSM-5@SiO 2 @Fe 3 O 4 , a comprehensive reaction pathway was proposed, providing insights into the catalytic mechanism.
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高影响因子
POLYMER
·
2024
·
IF 4.1
Jing Xu,Pingbo Zhang,Mingming Fan,Pingping Jiang,Shijun Chen,Xunxun Sheng
To improve the weak interaction between poly (butylene adipate‐co‐terephthalate) (PBAT) and poly (lactic acid) (PLA) blends, this study added modified metal-organic frameworks (MOFs) to enhance the interfacial bonding strength between PBAT and PLA. MOF-5 nanoparticles were synthesized by room temperature synthesis and modified with KH-560. PBAT/PLA/KH-560@MOF films were prepared by solvent casting. The microscopic morphology, mechanical properties, thermal properties, hydrophobicity, water vapor transmission rate and antimicrobial properties of the composite films were investigated. The results showed that KH-560@MOF nanoparticles were uniformly dispersed in the polymer matrix of PBAT and PLA, reducing phase interface defects. Mechanical properties of PLA/PBAT improved in the presence of KH-560@MOF. The breaking elongation and tensile strength values were maximized when adding 1 wt% KH-560@MOF. Doping of KH-560@MOF improves hydrophobicity and water vapor transmission rate of films. Zn 2+ in MOF-5 imparts antimicrobial properties to the film, showing antimicrobial activity against both Gram-positive and Gram-negative food-borne pathogens (i.e., E. coli and S.aureus ). This work enriched the design of compatibilizer for the PLA/PBAT blend and provided a novel approach for expanding the application of MOFs.
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高影响因子
Small
·
2025
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IF 12.1
Shufang Zhou,Jintong Xu,Jiayi Wang,Nurimangul Muntiza,Qiliang Deng
The reversible photo-transformation metal–organic framework (MOF) capable of changing properties by surface chemical modification has huge potential in various industrial fields. However, such material is still rare. Herein, a crystalline 3D MOF constructed by 5-boronobenzene-1, 3-dicarboxylic acid, and zinc sulfate (Zn-BBDA) is reported, where the boronic groups are spontaneously change into the hydroxyl groups during the preparation process. The resulted MOF possesses the orderly distributed hydroxyl groups in interlayers. The photo-responsive properties of the resulted MOF are explored. The results indicate that the appearance color and fluorescence emission of the resulted Zn-BBDA can be simultaneously adjusted based on the oxidation-reduction reaction of the hydroxyl group. The transformation degree of the MOF can be quantitatively monitored by fluorescence emission or Red, Green, Blue (RGB) readout. The response mechanism of the resulted Zn-BBDA is revealed. The surface properties of the resulted Zn-BBDA before and after irradiation are also investigated. The present material exhibits a bright future in the field of anti-counterfeiting and antibacterial treatment. The research provides new views in exploring novel photo-response materials.
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PubMed
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
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IF 4.1
Xian-De Zhou,Yong-Hui Tian
Biomass is a natural and renewable carbon resource. One of the possible green approaches to “carbon neutrality” is catalytic conversion of biomass resources into high value-added chemicals. As a result, photocatalytic selective oxidation of the biomass product 5-hydroxymethylfurfural (5-HMF) to 2,5-dicarbonylfuran (DFF) is an ecologically benign and energy efficient method. In this study, 2D g-C 3 N 4 /BiOCl heterostructures composites were prepared by easy ultrasonication-assisted stirring method for the first application of photocatalytic oxidation of 5-HMF to DFF. The physicochemical properties of the synthesized materials were characterized by SEM, XRD, FT-IR, XPS, UV–vis, BET surface area, PL and EPR analysis. The experimental results show that the g-C 3 N 4 /BiOCl composite is superior to pure g-C 3 N 4 and BiOCl in the oxidation of 5-HMF to DFF. The improved photocatalytic performance of the g-C 3 N 4 /BiOCl composites can be attributed to the improved visible light absorption, the creation of compact and intact Z-type heterojunction, increased surface area and enhanced separation efficiency of photogenerated electron-hole pairs. In addition, the photocatalyst has high stability and reusability. A putative photocatalytic process is proposed based on the respective energy band locations of these two semiconductors.
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高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·277
·
IF 4
Yunhan Pu,Huajie Zhang,Yanjun Li,Chuan Yu,Xiaofei Song,Chen Yang,Mingli Fu
The conversion of methane (CH4) to methanol (CH3OH) under mild conditions remains a significant challenge in catalysis. In this study, we introduce a method to adjust the surface valence states of copper species in Cu-ZSM-5 catalysts by annealing under different atmospheres (N2, air, and H2). Among these, the 10% Cu-ZSM-5 catalyst calcined in H2showed outstanding performance, achieving a methanol productivity of 8.08 mmol/(gcat·h) and 91% selectivity at 70 °C and 3 MPa using H2O2as the oxidant. Comprehensive characterization revealed that H2annealing optimized the Cu surface to a lower valence state (predominantly Cu+), enhancing CH4adsorption and promoting H2O2activation to generate ·OH and ·CH3radicals, which drive selective CH3OH formation. In situ DRIFTS and radical trapping experiments further confirmed the critical role of Cu+in facilitating C-H bond cleavage and suppressing overoxidation.
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高影响因子
RENEWABLE ENERGY
·
2024
·
IF 9
Wenli Zhang,Jifei Liu,Hongwei Gu,Cheng Pan,Yifei Long,Qunpeng Cheng,Guozhi Fan
The metal-organic framework materials ZIF-8 and UiO-66-NH 2 , synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH 2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m 2 /g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH 2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH 2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH 2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.
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高影响因子
FUEL
·
2024
·
IF 6.7
Guozhang Chang,Shanshan Dai,Huifen Kang,Jie Li,Yong Liu,Jian Zhang,Qingjie Guo
Limited knowledge regarding the controlled preparation of aromatic hydrocarbons (AHs) via catalytic pyrolysis of individual organic components hinders high yields of lignocellulosic biomass-based AHs. This report describes a systematic investigation of AHs generation following catalytic pyrolysis of organic components referring to cellulose, xylan, and lignin. Results show that in a programmed-heating process (20 °C/min), a (Ca-Fe)/HZSM-5 catalyst promoted the degradation of cellulose, xylan, and lignin with respective increment ratios of 24.56 %, 17.29 % and 19.45 %, and significantly increased the release of benzene during the pyrolysis of cellulose and xylan. In a fast-heating process (20 °C/ms), Ca-Fe alone presented a positive effect on bio-oil yield from cellulose, whereas HZSM-5 and (Ca-Fe)/HZSM-5 afforded high bio-oil yields from all three components. Notably, Ca-Fe and HZSM-5 exhibited synergistic effects on the bio-oil and AHs yields following cellulose pyrolysis, and on AHs yield following xylan pyrolysis. Alcohols, aldehydes, and furans were suitable precursors for generating AHs via pyrolysis of both cellulose and xylan. Lignin conversion to AHs involved various potential reaction pathways, including dehydration-deoxygenation-aromatization and dehydration-hydrodeoxygenation. The orders of (Ca-Fe)/HZSM-5 catalyzed pyrolysis of individual components towards AHs generation were xylan > cellulose > lignin. The presence of Ca-Fe particles inhibited deactivation of HZSM-5 in pyrolysis of a cellulose/xylan/lignin mixture.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Kezhen Qian,Wenmin Tian,Zixu Yang,Jing Xu,Huihua Pan,Lijie Yin,Dezhen Chen
The catalytic upcycling of end-of-life polyethylene by using hierarchical zeolites has garnered attention. Fine-tuning these zeolites’ micromesoporous structure and acidity is crucial for process efficiency, which requires a comprehensive understanding of their impact on polyethylene cracking. The impact of the mesoporosity and acidity of aggregated hierarchical HZSM-5 zeolites on high-density polyethylene (HDPE) vapor cracking was studied. The results indicated that the hierarchical structure enhanced accessibility to internal acid sites, facilitating monomolecular cracking and aromatization. Intercrystalline mesopores additionally heightened the alkylated aromatic yields. The Si/Al ratio shows a positive correlation toward the C5+ aliphatic hydrocarbon cracking, which boosts the formation of C2–C4 olefins and BTEX (benzene, toluene, ethylbenzene, and xylene). However, the presence of mesopores also yielded more heavy aromatics, thus increasing the risk of coking. The role of acid sites spatial distribution was investigated by poisoning the acid sites in micropores via pre-coking. The results indicated that the cracking of HDPE vapor occurred on the external acid of the zeolite, followed by the subsequent C5+ aliphatic hydrocarbon cracking on the mesopore and micropore to form aromatics and C1–C4 products. The formation of BTEX mainly occurred in the micropore, while the heavier aromatics and other alkylated benzenes were formed in the mesopore. The results of this study highlighted the importance of a proper hierarchical structure and acid site distribution in zeolites for effective and stable polyolefin cracking.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Shuxing Zhang,Xiaoshu Ding,Yanji Wang
5-Amino-1-pentanol is an important pharmaceutical intermediate used in the synthesis of anti-inflammatory and anticancer drugs. The direct hydrogenolysis of furfurylamine to 5-amino-1-pentanol has the advantages of a simple process route and high atom utilization. In this paper, for Pt/ZrO2 catalysts, the effects of different Pt loading and calcination temperatures on catalyst activity, selectivity, and surface properties such as Pt nanoparticle size, acidity and alkalinity, and the ratio of Pt0/(Pt0+Pt2+) were investigated. Through the study of the relationship between catalyst preparation conditions, furfurylamine hydrogenolysis reaction performance, and surface properties, it was found that moderate Pt nanoparticle size, higher Pt0/(Pt0+Pt2+) ratio, and more acidic sites favored furfurylamine hydrogenolysis. The higher number of basic sites favors the dispersion of Pt metal. The results of in situ FTIR show that the amino group of furfurylamine is adsorbed on the acidic site of Pt/ZrO2, and the furan ring is adsorbed on Pt nanoparticles, which is beneficial to the hydrogenolysis of furfurylamine.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3033-3052
·
IF 2.8
Huang Guihua,Yang Zizhen,Li Sijia,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In-situ crystallization was used to prepare the composite molecular sieve ZSM-5/MOR (Z/M) successfully, and FeLa-ZSM-5/MOR (FeLa-Z/M) was obtained by loading Fe and La on the surface of the composite molecular sieve by hydrothermal method. The composite molecular sieve combined the water absorption of mordenite (MOR) and the mass transfer performance of ZSM-5, and effectively improved the surface area and porous structure. This zeolite improved the dispersion performance of active sites in Z/M and reduced mutual aggregation between particles, which was conducive to catalytic efficiency. The addition of La increases the number of oxygen vacancies, according to XRD, TEM, XPS, UV-DRS, and other data analyses. Because doping of La stretched the Fe–O bond, reduced the oxygen vacancies’ formation energy, and promoted oxygen vacancies’ formation, which was an essential reason for Fe 3+ reduction and Fe 3 O 4 formation. The addition of La also had a highly dispersed effect on Fe. Under the optimal conditions, with a FeLa mass ratio of 1:1, FeLa-Z/M at 25 mg, H 2 O 2 at 0.5 ml, and a pH of 3, the degradation rate of IC was found to be 97.8% and 99.5% in 5 min and 10 min respectively. Analysis of the reaction indicated that the catalyst followed a first-order reaction kinetic. Free radical quenching experiments confirmed that the main free radicals in the FeLa-Z/M Fenton-like system were hydroxyl radicals (·OH), suggesting a possible catalytic mechanism. Furthermore, the synthesized FeLa-Z/M catalyst exhibited superior performance compared to other methods of IC removal, demonstrating high reusability and efficient degradation even after multiple uses. Graphical abstract
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yijun Luo,Wenxin Yang,Jincheng Liu,Wei Cai,Zewei Liao,Xiaoyan Xiang,Bingjie Li,Yanxiong Fang
The concurrent production of renewable hydrogen and valorization of biomass represents a promising strategy to tackle energy sustainability and environmental concerns. However, designing efficient bifunctional photocatalytic systems capable of driving both reactions remains a significant challenge. This study introduces a Z-scheme heterojunction composed of graphitic carbon nitride (g-C 3 N 4 ) and titanium dioxide (TiO 2 ), synthesized through a combined hydrothermal and self-assembly approach, for simultaneous photocatalytic H 2 evolution and selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF). The heterostructure establishes an internal electric field that directs photogenerated electrons to g-C 3 N 4 and holes to TiO 2 , thereby facilitating effective charge-carrier separation while preserving their strong redox potentials . Structural analyses confirm the uniform growth of TiO 2 nanorods with reduced diameter of less than 10 nm on g-C 3 N 4 nanosheets, which enhances light harvesting and exposes abundant reactive sites. Under optimized conditions, the composite exhibited exceptional performance, achieving H 2 and DFF production rates of 481.9 μmol g −1 h −1 , respectively, with 92.8 % DFF selectivity. This represents a 3.8-fold enhancement in activity compared to pristine g-C 3 N 4 . The improved efficiency is attributed to the Z-scheme charge-transfer pathway, which mitigates recombination losses and optimizes the utilization of electrons and holes for respective reduction and oxidation reactions. This work provides a scalable framework for integrating green hydrogen generation with biomass refining, advancing the development of multifunctional photocatalysts for sustainable energy and chemical synthesis.
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高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Yanjuan Yang,Yuhuan Li,Liang Deng,Shangzhi Xie,Chuang Gao,Zixu Yang,Jing Xu
The production of 5-hydroxymethylfurfural (5-HMF) from saccharide conversion has fallen short of industrial expectations due to low reaction efficiency and high costs. Herein, we fabricated a series of LaPO4 catalysts with controlled crystal structures and tuned acidity via a facile hydrothermal method. The hexagonal LaPO4-120 catalyst exhibited a high glucose conversion of 99.9% and a remarkable 5-HMF yield of 90.1% at 150 °C for 60 min. Additionally, the hexagonal LaPO4-120 catalyst showed promising activities in converting various saccharides including fructose, glucose, cellobiose, sucrose, and inulin. A series of characterization studies and DFT calculations revealed that the hexagonal LaPO4-120 catalyst possessed low-coordination La sites and abundant zeolitic water stored in the open and oxygen-lined channels, which provided Lewis acid sites and a dynamically local Brønsted acid environment to respectively facilitate glucose isomerization and the subsequent dehydration. A plausible reaction mechanism involving a synergetic proton transfer via hydrogen bonding is proposed. This study offers insights for the design of low-cost and heterogeneous catalysts with finely tuned Lewis and Brønsted acid sites for 5-HMF production.
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高影响因子
危险品化学品经营许可证（带存储）