INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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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.
研究领域:
光催化
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材料科学
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能量转换
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环境可持续性
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化学合成
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产品关联
DOI
高影响因子
Science China-Materials
·
2023
·Vol. 67
·期 1
·162-169
·
IF 8.1
Yang Bixia,Zhu Mengyao,Jiang Xingpeng,Shao Wenlei,Wang Zhiqi,Yan Jiawei,Zheng Yanting,Zhuang Zanyong,Yu Yan
The photooxidation of renewable bioderivatives into value-added chemicals is highly significant; however, it typically exhibits low selectivity owing to the challenges in controlling the oxidative species and managing the desirable reaction pathways. In this work, we used the Bi 2 O 2 CO 3 /ZnIn 2 S 4 heterostructure, prepared by a CO 2 -mediated solid–solid phase transition, to catalyze the photooxidation of bioderived 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) with a high selectivity of 98.1% and a yield rate of 882.6 µmol g −1 h −1 . The metal carbonate/oxide heterointerface enables the effective transfer of photoactive electrons and holes, optimizes surface oxygen activation, and facilitates the synergy of ·OOH and holes to selectively convert HMF into DFF. The findings unravel how the tailoring and coupling of the electron–hole pairs and reactive oxygen species on heterostructured materials can promote the usage of renewable feedstocks for sustainable development.
研究领域:
光催化
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环境化学
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材料科学
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绿色化学
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可再生能源
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yu-Feng Qi,Kai-Yao Wang,Yan Sun,Jie Wang,Cheng Wang
The utilization of biomass resources is essential for constructing a carbon neutral society. Electrochemical conversion of biomass-derived platform molecule 5-hydroxymethylfurfural (HMF) to 5-furandicarboxylic acid (FDCA) is a highly promising alternative pathway for the production of valuable biobased oxygenated chemicals, which primarily takes advantage of the on-going development of efficient, robust, and inexpensive catalysts. In the present work, a carbon paper-supported nickel-iron layered double hydroxide (LDH) nanosheet array implanted with abundant cationic vacancies (d-NiFe LDH/CP) is employed as a self-standing electrode for oxidation of HMF to FDCA. A 97.35% conversion of HMF and a 96.8% yield of FDCA could be achieved at 1.48 V, with a faradaic efficiency as high as 84.47% in 1 M KOH electrolyte. More importantly, it also exhibits excellent stability for 10 cycles. The successful introduction of M2+ vacancies was proved by electron paramagnetic resonance spectroscopy. X-ray photoelectron spectroscopy results confirmed that the implanted cationic vacancies would effectively raise the electron density of d-NiFe LDH and tailor the electronic structures of metal sites. This results in a significantly increased active site number and lowered charge transfer resistance that facilitate the electrocatalytic performance improvement. Postreaction characterization indicates that the in situ generated metal (oxy)hydroxides are the active species, and the HMF would be oxidized through both chemical and electrochemical pathways. These interesting findings shed light on the innovation of defect-rich catalysts and their promising application in electrochemical biomass derivative upgrading.
研究领域:
材料科学
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催化化学
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生物质化学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Qianqian Xing,Xiaoliang Jia,Shiyu Jia,Yongqin Qi,Yuqi Wang,Yingxiong Wang,Xianglin Hou
The traditional synthesis methods of cyclopropyl methyl ketone (CPMK) have some disadvantages such as low yield, slow reaction rate and unclear catalytic mechanism. To solve these problems, a new strategy is developed to synthesize CPMK from 5‑chloro-2-pentanone (CPE) using 1,8-diazabicyclo[5.4.0]undec‑7-ene (DBU). Experiment results show that the yield of CPMK reached a maximum of 96.5 % in DBU at 40 °C for 30min. The mechanism study shows that the hydrogen bond between DBU and CPE is the key to drive the deprotonation and cyclization of CPE. The hydrogen bond is formed between the N atom on C = N of DBU and the α-H on the methylene group associated with the carbonyl group on CPE. The catalyst DBU is converted into [DBUH] + Cl − , which can be reclaimed and recycled completely. The density functional theory (DFT) calculation confirmed the existence of molecular hydrogen bonds and proved that the hydrogen bond driving force is the key to the reaction. The hydrogen bond driven mechanism provides a new idea for the basic research of cyclization reaction.
研究领域:
有机化学
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催化反应
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产品关联
DOI
高影响因子
JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2025
·
IF 4.9
Ahmed M. Omer,Eman M. Abd El-Monaem,Heba S. Hassan,Mahmoud A. Elmeligy,Angela Kleinová,Abdelazeem S. Eltaweil,Abolfazl Heydari
pH-sensitive carriers have emerged as an optimal choice for the oral administration of anticancer drugs, exhibiting the desired release performance. This study aims to develop biocomposite beads for the sustained release of the anticancer drug 5-fluorouracil (5-FU). Here, 5-FU was encapsulated within a ZIF-8 metal-organic framework (MOF), which was subsequently impregnated into amino-chitosan beads. The resulting Am-CS@ZIF-8 biocomposite beads were characterized for their chemical structure, surface morphology, elemental composition, crystallinity, surface charges, and mechanical properties utilizing Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), zeta potential analysis, and a texture analyzer, respectively. The developed beads exhibited a textured surface, denser composition, and a positively charged surface with a maximum zeta potential of +12.4 at pH 7.4. In comparison to Am-CS beads, the Am-CS@ZIF-8 biocomposite beads demonstrated superior mechanical properties, achieving a maximum stress value of 5.668 MPa compared to the 1.874 MPa recorded for pure Am-CS beads. pH sensitivity was assessed through the investigation of water uptake behavior at pH 1.2 and pH 7.4. The Am-CS@ZIF-8 biocomposite beads demonstrated a high encapsulation efficiency of approximately 81.6 % for 5-FU. They exhibited pH-responsive release behavior, with only 17 % of the drug released at pH 1.2 after 2 h and a sustained release of 52 % at pH 7.4 over 24 h. The release mechanism was predominantly governed by Fickian diffusion, as closely fitted by the Peppas-Sahlin kinetic model. The formulated carrier confirmed its biodegradability under enzymatic physiological conditions, suggesting its potential applicability as an effective system for the oral delivery of anticancer drugs.
研究领域:
药剂学
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生物材料学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yifei Chen,Xinnan Zhao,Chen Xin,Xiuqin Dong,Hao Gong
This work explored the role of defective sites on the hydroformylation of n-butene through ligand regulation. The investigation examined the effect of modulator properties on defect sites and rhodium loading, and optimized the H 2 BDC/modulator ratio to improve catalyst activity. Atomically dispersed Rh is anchored to these highly dispersed defect sites, effectively preventing aggregation and thereby enhancing hydrogenation ability. Under optimal conditions, the catalyst achieved a conversion of 96.9 %, with an overall aldehyde selectivity of 90 %. DRIFTS analysis provided compelling evidence that Rh(CO) 2 and HRhCO species were formed on 1Rh/MOF-5-HBC, improving CO insertion capability. This study highlights the significance of MOFs as catalyst supports in enhancing performance through defect engineering. The ability of the modulator to induce defect formation was measured by p K a. Meanwhile, it has been discovered that the length differences between the modulator and the MOF organic ligand can have a significant impact on the stability of defective MOFs.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2024
·
IF 5.3
Fengya Ran,Meng He,Shiyong Sun,Rui Lv,Sen Lin,Ke Wang,Yevgeny Aleksandrovich Golubev,Olga Borisovna Kotova,Elena Leonidovna Kotova
Zeolite products synthesized from mineral materials are receiving widespread attention, while there are few reports on the introduction of heteroatom metals from minerals into zeolites. Herein, the effects of different silicon sources, hydrothermal reaction time and the amount of template on the crystallisation of Fe-ZSM-5 were investigated. The morphology and structure of ZSM-5 were characterized by X-ray diffraction (XRD), fourier transform infrared spectroscopy (FT-IR), X-ray electron spectroscopy (XPS) and scanning electron microscopy (SEM). The catalysis of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fe-ZSM-5 was then carried out to evaluate its enzyme-like catalytic performance as a type of nanozyme catalyst. The results showed that Fe-ZSM-5 exhibited peroxidase-like activity, oxidizing TMB into a colored substance in the presence of hydrogen peroxide (H 2 O 2 ). Kinetic analysis implied that, compared with natural horseradish peroxidase (HRP), Fe-ZSM-5 peroxidase mimics exhibit inferior affinity and enzymatic catalytic velocity towards the TMB substrate. However, it exhibited excellent stability under extreme pH, temperature, and ionic strength conditions. This work provides a possible reference for the construction of functional nanozymes using natural mineral resources.
研究领域:
材料科学
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催化化学
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生物医学工程
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产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2024
·
IF 5.3
Yanan Wei,Yunlei Zhang
A novel halloysite (Hal) based acidic catalyst was synthesized by anchoring functional alkyl group and Cr site and catalyzed the selective conversion of mannose to 5-hydroxymethylfurfural (HMF) in NaCl-H 2 O/dimethyl sulfoxide/methyl isobutyl ketone (MIBK) biphasic system. Herein, adjusting the hydrophilicity/hydrophobicity of catalyst by modifying the octyl group can facilitate the HMF yield. The density functional theory (DFT) calculation and in-situ FT-IR results revealed that increasing the hydrophobicity of catalyst surface weakened the interaction between HMF, water molecule and acid sites and inhibited the rehydration of HMF. Moreover, the synergistic effect between Cr and sulfonic group active sites remarkedly promoted the isomerization of mannose to fructose and the dehydration of fructose to HMF, and the 48.1% yield of HMF was obtained. This study provides references for the high value conversion of hemicellulose with the high efficiency reaction system.
研究领域:
生物化学
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催化化学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 28
·6147-6157
·
IF 4.857
Zhaoqi Ye,Yang Zhao,Hongbin Zhang,Yahong Zhang,Yi Tang
Graphical Seed-induced synthesis : Basic mesoporous ZSM-5 with adjustable alkaline-earth metal species have been synthesized by an acid co-hydrolysis and seed-induced method. Its mesostructure together with the high dispersity of basic guest species was realized by this non-classical crystallization process. For zeolite catalysts, the regulation of active site and pore structure plays an important role in the enhancement of their catalytic performance. In this work, a one-pot and organic template-free co-regulation route is proposed to straightforwardly synthesize basic mesoporous ZSM-5 zeolites with adjustable alkaline-earth metal species. The synthesis pathway combines two decisive strategies: 1) the seed-induced interface assembly growth method and 2) the acidic co-hydrolysis/condensation of aluminosilicate species and alkaline-earth metal (e.g., Mg, Ca, Sr, or Ba) sources. It is interesting that the mesoporous structure was self-evolved through particle-attached seed-interfacial crystallization without the assistance of any template. Meanwhile, the incorporation of alkaline-earth metals species is homogeneous and highly dispersed in the solid products during the whole crystallization process, and finally generate the superior basicity. Catalysis tests of the as-synthesized samples displayed their novel performance in the typical base reaction of Knoevenagel condensation, even for bulky substrates owing to the enhanced diffusion arising from the meso/microporous network. This finding opens new possibilities for facile, cost-effective, and environmentally friendly synthesis of mesoporous high-silica zeolites with tunable acid/base properties, and deepens our understanding of the particle-attached crystallization.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Tao Jiang,Fumin Wang,Xubin Zhang,Yi Zhai,Guojun Lv,Yu Shen,Yuzhou Wu
Mesocrystal zeolite with well-defined morphology owns mesoporous channels and single crystal characteristics, which could promote diffusion efficiency, stability and catalytic activity. Thus, we performed the controllable synthesis of ZSM-5 mesocrystal without special additives and complex methods. Selected area electron diffraction (SAED) and fast Fourier transform (FFT) showed diffraction spots regardless of crystallization time, which indicated the well oriented feature of synthesized ZSM-5 zeolites. The crystallization process was further investigated. The oriented particle attachment (OPA) effectively guided the synthesis process of mesocrystals, which followed the nonclassical crystallization mechanism. The crystallinity curve exhibited valley-like shape, which manifested that the crystallization pathway went through three stages: fast precipitation, deconstruction and reorganization. The plausible formation mechanism was proposed, which might be useful for the fabrication of ZSM-5 mesocrystal. The prepared zeolites showed superior catalytic performance in aldol condensation reaction between benzaldehyde and 2-hydroxyacetophenone, obtaining 93% of the conversion.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Shiyou Xing,Pengmei Lv,Che Zhao,Ming Li,Lingmei Yang,Zhongming Wang,Yong Chen,Shijun Liu
Non-H 2 and solvent-free catalytic conversion of waste lipids to liquid hydrocarbons is of great interest because of the associated low-cost, full-safety, and easy-operability. In this work, a solvent-free catalytic process for deoxygenating oleic acid was performed in H 2 and non-H 2 (N 2 , CH 4 , and CO 2 ) media over nano-Ni/HZSM-5. 8-Heptadecene, a primary product obtained at 320 °C in four media, was derived from the straightforward decarboxylation of oleic acid. In non-H 2 medium at 360 °C, the formation of C 8 –C 15 alkanes was enhanced, with yields of ca. 65.05 mol%, 70.71 mol%, and 73.09 mol% for N 2 , CH 4 , and CO 2 , respectively. A low yield of 49.67 mol% C 8 –C 15 alkanes in H 2 medium suggested that the H 2 medium reduced catalytic cracking . This was due to the preferential formation of stable heptadecane from 8-heptadecene in the presence of abundant H 2 . The absence of H 2 favored the cracking of 8-heptadecene. These cracked products were further converted to C 8 –C 15 alkanes, for which a mass supply of hydrogen was mandatory. Gas-phase reactions including methanation , Fisher-Tropsch (F-T) synthesis, and water-gas shift (WGS) reactions between deoxygenated gas products and reaction media provided significant pathways for the hydrogen required for the formation of alkanes. The CH 4 medium also acted as a hydrogen source due to its decomposition, catalyzed by nano-Ni/HZSM-5. Coke was substantially formed in all the four media. It was highlighted that the medium of H 2 favored the formation of aliphatic cokes, whereas the non-H 2 media, particularly the CO 2 medium, facilitated aromatic coke species on account of its weak oxidizability. Additionally, there was a severe loss of loaded Ni nanoparticles under H 2 medium but a slight Ni loss in CO 2 medium, which was proposed to the reason of aromatic cokes formation at the catalyst surface , acting as a trap for the loaded Ni nanoparticles.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
CHEMISTRY & BIODIVERSITY
·
2024
·Vol. 21
·期 6
·e202400150
·
IF 2.3
Long Ren,Yupu Xu,Wenjun Chen,Changsen Zhang
Experiments were conducted in this study on the co-hydropyrolysis of three components of biomass (cellulose, hemicellulose, and lignin) and HDPE by using SR-Pd/Trap-HZ-5 as catalyst. To control the variable, we use the same experiment conditions in co-hydropyrolysis: Si/Al ratio of 50, Pd load 1 %, catalyst to reactant ratio of 1 : 10, 1 MPa, 400 °C, reaction time 1 h. Use XRD, TEM, BET, and NH 3 -TPD to confirm catalyst successful synthesis; use pine sawdust (PW) co-hydropyrolysis with HDPE to analyse catalytic activity; and use GC/MS to characterize the chemical composition of the bio-oil from the co-hydropyrolysis of biomass components and HDPE. The results show that cellulose has a significant synergistic effect with aromatic hydrocarbon production, whose selectivity was 93.3 %; hemicellulose has a synergistic effect; aromatic selectivity can reach 75.1 %; and a negative synergistic effect between lignin and HDPE was shown as the selectivity of aromatic hydrocarbons decreased from 62.1 % to 15.6 %. Graphical
研究领域:
能源与燃料化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）