Journal of Materials Chemistry A
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2024
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IF 10.7
Yuhui Huang,Yehan Tao,Qingqing Wang,Jian Du,Jinwen Hu,Jie Lu,Yanna Lv,Haisong Wang
To develop an industrial zeolite-based catalyst for efficient furfural production, the acidity, pore structure, and electronic properties of H-β zeolite were modulated by synergistic deatomization and atomic implantation treatments. The dealumination effectively decreased the intrinsic aluminum-related Lewis and Brosted acid sites, thus decreasing the occurrence of unwanted side reactions. Meanwhile, the removed skeleton aluminum can create voids for the following atomic implantation of introducing higher valent-state niobium species, which would provide new kinds of catalytic active sites, increase the average pore size by distorting the zeolite skeleton, and enhance the interaction with reactant molecules by acting as more electron deficient centers. In a single-phase water/γ-valerolactone reaction system, the optimum catalyst can efficiently convert both xylan and xylose with a conversion of 100 % at a medium temperature of 130 ℃ within 3 hours. Compared with the furfural yield over untreated H-β (12.7%), the yield over deAlβ/Nb(20%) catalyst was greatly enhanced by 54% with xylose as raw material. The catalyst can be recovered by simple cleaning and thermal regeneration and then reused. The proposed post-treatment strategy could maintain the integrity of the zeolite structure, ensure uniform and stable metal dispersion under harsh conditions, manage the complexity and cost of the preparation process, and most importantly, optimize the catalytic performance. Addressing these issues is essential for improving the efficiency and practical application of industrial zeolite catalysts by this general approach and benefiting industrial furfural production.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2011
·Vol. 49
·期 12
·2755-2760
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IF 3.894
Jing Xu,Yuhong Ma,Jingyi Xie,F.J. Xu,Wantai Yang
A universal photoassisted pathway to functionalize polymeric surfaces is presented by transferring the inert surface sp 3 C H bonds into reactive groups, such as SO 3 H, NH 2 , SH, and COOH. The proposed method uses acetone as photoinitiator and different phenols with a para substituent XR as the reactants. Acetone excited by UV irradiation acts as a pair of scissors cutting both the surface C H bonds of the polymer substrate and the O H bonds of phenol, leading to the formation of carbon-centered surface chain free radicals and oxygen-centered phenoxy free radicals. By coupling of these two radicals, a variety of functional X groups with an R spacer from XR species of different phenol reactants were readily bonded to the polymeric surfaces, where phenol reactants included 4-hydroxylbenzene sulfonic acid for SO 3 H, p -aminophenol and tyramine for NH 2 , 4-hydroxythiophenol for SH, and tyrosine for COOH. © 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2011
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 47
·e56255
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IF 2.7
Jin Yang,Yixuan Hou,Yingzheng Hong,Yingbang Yao
Since thermally conductive fillers easily aggregate when introduced into polymer matrix, it is essential to apply a modifier to enhance the dispersion of the filler. In current study, the surface of boron nitride (h-BN) is firstly modified by employing a double modification process and then added into sulfonated polyetheretherketone (SPEEK) to form the composite materials. Four different kinds of samples of double-modified h-BN were obtained. Ultimately, the XXX@h-BN/SPEEK (XXX denoted as modifier, i.e. PDA, VTMS, TEOS, and APS) flexible film with the horizontally oriented XXX@h-BN was produced by heating the mixture under an external electric field. The test results indicate that the thermally conductive filler PDA@h-BN (PDA: polydopamine), which was prepared by modifying OH@h-BN with PDA, loaded into SPEEK, and electrically oriented, shows the best overall performances. With a high tensile strength of 43.24 MPa and good flexibility, PDA@h-BN/SPEEK flexible film exhibits an in-plane thermal conductivity of 2.3 Wm −1 K −1 at a filling ratio of 10 wt%. The sample may be bent at a steep angle without breaking down and can recover to original shape bearing its high degree of flexibility.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Ruijie Ma,Huimin Gao,Jinpeng Zhang,Jieying Jing,Wen-Ying Li
Photocatalytic reduction of CO 2 to formic acid (HCOOH) offers a sustainable pathway for carbon utilization, yet its efficiency is fundamentally limited by poor CO 2 adsorption and rapid electron-hole recombination in conventional photocatalysts. To address this challenge, a series of Pd-loaded hydrogenated TiO 2 catalysts (x wt%Pd/H-TiO 2 ) were developed through a synergistic hydrogen reduction-impregnation strategy, aiming to regulate the electron density of Pd active sites and enhance interfacial charge separation. Systematic characterization revealed that increasing Pd loading (0.6–1.4 wt%) effectively trapped photogenerated electrons, suppressing recombination losses and elevating electron density at Pd sites. Combined with optimized CO 2 adsorption capacity (0.178 mmol·g −1 ) and accelerated charge transfer, the 1.0 wt%Pd/H-TiO 2 catalyst achieved a HCOOH production rate of 14.14 mmol·g cat −1 ·h −1 under mild conditions (30 °C, 2.0 MPa, 4.57 mW·cm −2 ), outperforming most reported TiO 2 -based systems. Mechanistic studies further demonstrated a strong correlation between Pd-induced electronic effects and multi-electron CO 2 activation kinetics. This work provides a scalable catalyst design paradigm for balancing charge dynamics and surface reactivity in photocatalytic CO 2 valorization.
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Journal of the American Chemical Society
·
2024
·
IF 14.4
Liu Lin,Yunming Xu,Yiting Han,Ruikun Xu,Tongyue Wang,Zemin Sun,Zhenhua Yan
A deep understanding of the mechanism for the spin-magnetic effect on O–H cleavage is crucial for the development of new catalysts for water oxidation. Herein, we designed and synthesized the crystalline Fe-DABDT and Co-DABDT (DABDT = 2,5-diaminobenzene-1,4-dithiol) and optimized an effective magnetic moment to explore the role of the spin-magnetic effect in the regulation of water oxidation activity. It can be found that the OER activity of the catalyst is positively correlated with its effective magnetic moment. Under the external magnetic field, Fe-DABDT with more spin single electrons has a stronger spin-magnetic response to water oxidation than Fe/Co-DABDT and Co-DABDT. The increase in OER current of Fe-DABDT is nearly 2 times higher than that of Co-DABDT. Experimental and density functional theory studies show that magnetized Fe sites could realize nucleophilic reaction, accelerate the polarization of electron spin states, and promote the polar decomposition of O–H and the formation of the O–O bond. This study provides mechanistic insight into the spin-magnetic effect of oxygen evolution reaction and further understanding of the spin origin of catalytic activity, which is expected to improve the energy efficiency of hydrogen production.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 8
·3573-3580
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IF 2.7
Ruidong Li,Bo Zhao,Ganggang Chang,Shanchao Ke,Minjie Chen,Didi Dong,Chun Pu,Xiaoyu Yang
In the current investigation, the base-metal hollow multifunctional catalyst, Pd–IL@H-UiO-66-NH2, was fabricated utilizing a hydrothermal method followed by etching and supporting processes. The results of the effort demonstrate that Pd–IL@H-UiO-66-NH2 displays significantly enhanced activity and product selectivity in catalysis of the one-pot Knoevenagel condensation–hydrogenation reaction, as well as a high level of generality in promoting hydrogenation reactions of unsaturated hydrocarbons. The excellent properties of Pd–IL@H-UiO-66-NH2 are ascribed to its rationally designed spatial distribution of catalytically active sites within its hierarchical structure, which is comprised of surface wrinkles that increase hydrophobicity and exposure of the active sites, and hollow structures that serve as nanoreactors to enrich substrate interactions and improve mass transfer. Furthermore, the catalytic stability of Pd–IL@H-UiO-66-NH2 was shown to be largely maintained after its use in five successive catalytic cycles. The stability of the new tandem catalyst benefits from strong confinement effects associated with its hollow structure and electronic interactions between the Pd and ILs that effectively restrict leaching and aggregation of Pd nanoparticles (NPs).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yanan Huang,Wenjing Xie,Jia Li,Jixing Liu,Hao Chen
Oxidative desulfurization (ODS) is one of the most promising processes for producing clean fuels to meet the requirements for the clean use of fossil fuels. In this study, a MoS2/h-BN heterojunction was synthesized using the chemical vapor deposition method, leading to a modified electronic structure at the surface. X-ray photoelectron spectroscopy, electron paramagnetic resonance, and electrochemical impedance spectroscopy suggested the occurrence of interfacial electronic reorganization and enhanced charge transfer efficiency due to the formation of a well-defined heterojunction. Hydrogenation temperature-programmed reduction revealed a strong interaction between h-BN and MoS2, which contributed to the highly efficient performance of the heterojunction for ODS applications. As a result, although h-BN showed very low ODS activity, its catalytic activity was enhanced so much and even comparable to that of pure MoS2 after loading with only 1.7 wt % MoS2 on h-BN to construct MoS2/h-BN heterojunctions.
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Nano-Micro Letters
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2022
·Vol. 14
·期 1
·1-12
·
IF 23.655
Yang Peng,Zha Jiajia,Gao Guoyun,Zheng Long,Huang Haoxin,Xia Yunpeng,Xu Songcen,Xiong Tengfei,Zhang Zhuomin,Yang Zhengbao,Chen Ye,Ki Dong-Keun,Liou Juin J.,Liao Wugang,Tan Chaoliang
The growth of high-quality single-crystalline Te nanobelts is reported by introducing atomically flat hexagonal boron nitride (h-BN) nanoflakes into the chemical vapor deposition system as the growth substrate.
The field-effect transistor based on Te grown on h-BN exhibits an ultrahigh hole mobility up to 1370 cm 2 V −1 s −1 at room temperature.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Hui Zhao,Xin-Pu Fu,Wei-Wei Wang,Jin-Cheng Liu,Chun-Jiang Jia
Despite the supported Au demonstrating superior activity in catalyzing various reactions, their stubborn and widespread deactivation issue has long remained unsolved. Therefore, the challenge in current investigations of Au-based catalysts could be divided into two aspects: uncovering the authentic molecular induction for the deactivated evolution and fabricating interfacial structures combining efficiency and stability. In this work, by incorporating NiO x (H) adjacent to small active Au 1 /Au n species, the as-formed 0.5Au-5NiO x (H)/CeO 2 catalyst simultaneously achieved high reactivity ( r = 5.23 mmol CO ·g Au −1 ·s −1 ) toward the water-gas shift (WGS) reaction and remarkable long-term stability with time-on-stream of 100 h at 250 °C, significantly surpassing the reference Au/CeO 2 counterpart as well as the other oxides-supported Au catalysts reported previously. Comprehensive in-situ characterizations and DFT calculations revealed that the CO molecules, rather than H 2 , H 2 O, or CO 2 molecules, are the dominant molecular driver for Au aggregation, correspondingly inducing the degraded catalytic efficiency. Specifically, on the one hand, the strong CO−Au coordination degraded the ejection barrier of Au atoms from Au-Au coordination; on the other hand, the −OH groups as intermediates from H 2 O dissociation, participating in the stabilization of Au species upon the surface, were dynamically consumed by CO molecules. For these regards, the adjacent Ni adatoms promote the sufficient generation of stable −OH groups for stabilizing Au atoms under WGS reaction. As a result, the corresponding Au−Au ejection and Au−O diffusion barriers of as-formed Au n −O(H)−Ni/CeO 2 combinations are significantly enlarged, which thereby boosts the structural stability in the CO-containing atmospheres.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2025
·Vol. 26
·期 18
·9016
·
IF 4.9
Xiulin Zhang,Yang He,Xiaolu Zhang,Ziyi Liang,Wendong Wang,Zhenyu Da,Jianyi Lv,Meng Guo,Xueyun Huo,Xin Liu,Jing Lu,Lixue Cao,Xiaoyan Du,Zhongming Ge,Zhenwen Chen,Xuancheng Lu,Jianzhong Zhang,Changlong Li
Helicobacter pylori(H. pylori) is a well-known pathogen associated with chronic gastric infection, progressing from gastritis to gastric adenocarcinoma, but the dynamic phenotypic and molecular characteristics of gastric epithelial cells during sustained infection remain unclear. We established a chronic infection model using the human gastric epithelial cell line GES-1, exposed toH. pylorior its lysate across 30 generations, dynamically assessing cell proliferation, migration, invasion, apoptosis, autophagy, and epithelial–mesenchymal transition (EMT) markers, with RNA sequencing for transcriptomic changes and a Mongolian gerbil model to validate chronic pathological progression. AcuteH. pyloriexposure induced pronounced morphological changes; suppressed proliferation, migration, and invasion; triggered apoptosis; and blocked autophagic flux, while long-term stimulation reversed these effects. EMT markers showed progressive loss of epithelial characteristics with chronic infection. RNA sequencing revealed a dynamic shift from inflammation-driven apoptosis to adaptive survival mechanisms. In vivo, prolonged infection induced dynamic TLR expression alongside progressive gastric pathology, including atrophy and dysplasia. Our study provides new molecular evidence for dynamic cellular and immunological adaptations of gastric epithelial cells under chronicH. pyloriinfection, highlighting critical intervention windows for preventing gastric carcinogenesis.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Yong Zhou,Jiamei Liu,Xudong Zhao,Bin Yang,Bing Li,Xiaoyang Liu
Because of their unique electrical and magnetic properties, the perovskite multiferroic materials exhibit significant potential in spintronic device applications. However, synthesizing room-temperature multiferroic materials with robust magneto-electric coupling effects remains a major challenge. In this work, Yb 3 + , with an ionic radius slightly smaller than Y 3+ , was selected for A -site doping in the h -YMnO 3 , which has a high ferroelectric transition temperature (T C ∼ 900 K) and a low antiferromagnetic transition temperature (T N ≤ 70 K). This similar ionic radius allows Yb to substitute the Y site effectively while introducing distinct electronic states, thereby optimizing the structure and multiferroic properties of h -YMnO 3 without significantly altering the crystal structure. A series of Yb-doped Y 1- x Yb x MnO 3 ( x = 0, 0.1, 0.2, 0.3, 0.4, 0.5 and 1) materials were synthesized via conventional solid-phase reaction. The effects of Yb doping on the structure, magnetism, and ferroelectricity of h -YMnO 3 were studied. X-ray diffraction (XRD) and corresponding XRD refining results show that as Y 3+ is replaced by Yb 3+ with smaller radii, the cell parameters and cell volume of Y 1- x Yb x MnO 3 decrease, the cell is compressed, and the lattice structure of Y 0.5 Yb 0.5 MnO 3 obtained under the condition of Yb semi-doping changes significantly. Subsequent magnetic and room-temperature ferroelectric test results show that the Y 1- x Yb x MnO 3 series samples have anti-ferromagnetic ground states. In particular, the proper inclination of Mn 3+ ions in the double perovskite structure of Y 0.5 Yb 0.5 MnO 3 generates strong Dzyaloshinskii-Moriya (DM) interactions, resulting in relatively strong antiferromagnetism. The antiferromagnetic Neel temperature (T N ) from 37 K to 41 K. Yb 3+ -induced inclined ferroelectricity enables Y 0.8 Yb 0.2 MnO 3 to achieve the highest ferroelectric polarization of 0.030 µC cm −2 , which is 180 % greater than that of h -YMnO 3 . The results demonstrate that Yb doping plays a crucial role in regulating the structure and multiferroic properties of h -YMnO 3 , offering a novel strategy for developing room-temperature multiferroic materials with robust magneto-electric coupling.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Yujia Xie,Fengyong Zhang,Pingle Liu,Fang Hao,Hean Luo
Direct functionalization of saturated C–H bonds by metalloporphyrin catalysts is among the topical and challenging areas within the chemical industry and synthetic chemistry. In this work, supported CoD(p-Cl)PPCl metalloporphyrin catalysts were prepared and characterized. It has been found that the CoD(p-Cl)PPCl/ZnO catalyst shows better catalytic activity than the supported catalyst (ZrO2, MCM-41, kaolin, Zr(OH)2, and boehmite (BM)) in cyclohexane oxidation with dioxygen. The effects of the reaction pressure, reaction temperature, and reaction time on the catalytic activity were considered by the supported CoD(p-Cl)PPCl/ZnO catalyst. The CoD(p-Cl)PPCl/ZnO catalyst can be facilely recovered and was recycled up to seven times without a significant decrease in catalytic performance. The average cyclohexane conversion and selectivity to KA oil are 10.98% and 84.34%, respectively, and the turnover number is 2.10 × 107.
研究领域:
催化化学
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有机合成
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工业化学
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材料化学
·
绿色化学
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