NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 8
·3573-3580
·
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
·
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
·
2025
·
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
·
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
Marine Drugs
·
2015
·Vol. 13
·期 6
·3360-3367
·
IF 2.853
Ying Fu,Ping Wu,Jinghua Xue,Hanxiang Li,Xiaoyi Wei
Two new quinone sesquiterpenes named myrothecols G and H (1and2), a pair of C-1′ diastereomers of 13-hydroxyl penicilliumin A, were isolated from the mycelia solid cultures ofMyrotheciumsp. SC0265. Their structures, including the absolute configurations, were established on the basis of the spectroscopic data combining with the theoretical conformational analysis. The cytotoxic activities of1and2were tested against a panel of human tumor cell lines.
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CERAMICS INTERNATIONAL
·
2026
·
IF 6
Runduo Teng,Changhao Feng,Yanting Wang,Wenjun Tu,Tianyu Lan,Qiyuan Fu,Jingyu Long
N-butanol is widely used in fields such as chemical engineering and pharmaceutical synthesis; therefore, trace-level, highly sensitive detection of n-butanol is of great significance. In this study, an n-butanol gas sensor based on silver (Ag)-decorated yttrium ferrite (YFeO 3 ) nanotubes was fabricated using the electrospinning followed by the impregnation method. Compared with the pure YFeO 3 , the Ag-decorated YFeO 3 nanotubes exhibited an enhanced response of 162.06 toward 10 ppm n-butanol. This remarkable gas-sensing performance is primarily attributed to the synergistic effects of the mixed-valence states of iron, abundant surface oxygen vacancies, and the Ag spillover effect. Moreover, it exhibits excellent long-term stability and a detection limit as low as 76.5 ppb. These results indicate that Ag-decorated YFeO 3 nanotubes hold significant potential for trace n-butanol detection.
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Nature Catalysis
·
2026
·
IF 48.3
Ding Liang,Yao Ze-Cheng,Tang Tang,Wan Xin,Liu Xiaozhi,Jiang Zhe,Fu Jiaju,Shi Zhuo-Qi,Tai Jing,Lyu Zhen-Hua,Dong Jichen,Li Qing,Su Dong,Shui Jianglan,Hu Jin-Song,Wan Li-Jun
High-performance cathode catalysts are essential for proton-exchange membrane fuel cells. Intermetallic nanocrystals are promising candidates but suffer from intrinsic activity–durability trade-offs because their comprehensive catalytic properties are determined by several intertwined structural factors that cannot be optimized independently by existing synthesis techniques. The challenge lies in the inherent thermodynamic and kinetic constraints during synthesis. Here we develop a decoupled synthesis strategy that leverages block-copolymer micelle confinement, which enables the customized synthesis of libraries of intermetallic nanocrystals, simultaneously achieving ultra-small size, ultra-high ordering degree, tailorable loading density, narrow size distribution, compositional uniformity, and broad compositional and substrate universality. The developed Pt 3 Co intermetallic nanocrystal/Ketjenblack catalyst achieves a rated power density of 1.08 W cm −2 and 92% rated power retention after 30,000 cycles under light-duty-vehicle conditions and 900 h of stable operation at 10 A. It also delivered a 70.2% cell efficiency without degradation and 98.4% specific power retention after 90,000 cycles of heavy-duty-vehicle applications. This performance led us to project a lifetime of 240,000 h.
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Materials
·
2026
·Vol. 19
·期 18
·3966
·
IF 3.7
Zhe Tong,Xinghao Song,Wenxing Lei,Yajun Zhang,Jiaojiao Li,Li Zhao
The incorporation of various types of fillers is critical to enhancing the starved oil lubrication performance of PEEK matrix composites. In this work, PEEK composites reinforced with h-BN and SCFs were fabricated via a hot-pressing method, and the friction and wear behaviors under dry sliding and starved oil lubrication were systematically investigated. Surface oil wettability and Vickers hardness were characterized, and tribological tests were conducted on a ball-on-disk reciprocating tribometer. Worn surface topography and wear mechanisms were elucidated through laser scanning confocal microscopy and scanning electron microscopy. The results show that h-BN effectively reduces the friction coefficient through its solid lubrication effect, while SCFs significantly improve the hardness and load-bearing capacity of the PEEK matrix. Under dry sliding conditions, the PEEK composite containing h-BN and SCFs achieves the lowest wear rate of 10.3 × 10−5mm3/(N·m), which is 74.6% lower than that of pure PEEK, indicating a synergistic anti-wear effect. Under starved oil lubrication, PEEK/h-BN maintains the smoothest and lowest friction, and the presence of SCFs further improves wear resistance of PEEK composites despite a slight increase in friction. In addition, the fillers’ incorporation reduces the surface oil wettability of the PEEK composites; the dominant wear mechanism hence transforms from severe adhesive wear and plastic deformation in pure PEEK to mild abrasive wear.
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Nature Communications
·
2026
·
IF 18.1
Fang Geqian,Alhajjar Nour,Yu Wenjun,Marinova Maya,Ben Tayeb Karima,Lin Jian,Roland Thomas,Simon Pardis,De Waele Vincent,Ordomsky Vitaly V.,Khodakov Andrei Y.
Selective photocatalytic oxidation of methane to liquid oxygenates under ambient conditions remains challenging due to the inert C–H bond and propensity for over-oxidation. Controlling carrier transfer and reactive oxygen species is therefore essential to the selective methane photooxidation. Ultrasmall zirconium metal–organic framework (UiO-66-H) nanocrystals in situ grown on titania form a heterojunction that promotes efficient charge separation and tunes the interfacial band alignment. Comprehensive experiments and characterization reveal that this heterojunction precisely regulates • OH and • OOH generation, enabling controlled, radical-mediated oxidation of methane with a competitive oxygenate yield and nearly 100% selectivity at room temperature using air as an oxidant. In this work, ultrasmall metal–organic framework–semiconductor heterojunctions with a built-in electric field provide an effective route for developing efficient, low-cost photocatalysts for methane chemical valorization under mild, solar-driven conditions.
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PubMed
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ACS ES&T Engineering
·
2026
·
IF 6.3
Xu Pan,Jiangkun Xie,Mingze Jiao,Liang Shan,Hongyuan Qi,Wenjun Huang,Zan Qu,Naiqiang Yan,Haomiao Xu
Methane selective catalytic reduction (CH4-SCR) represents a promising strategy for nitrogen oxides (NOx) abatement, yet its practical application is hindered by catalyst deactivation in the presence of water, caused by competitive adsorption on acid sites and irreversible hydroxylation of active metal species. In this study, we developed a dual-functional In@H-Beta/Fe2O3 catalyst through sequential ion-exchange and impregnation. This architecture confines indium species within the channels of H-Beta zeolite, while Fe2O3 nanoparticles are dispersed on the external surface, creating a synergistic system featuring a hydrophobic layer and strong Fe–O–In interfacial interactions. Under 5% H2O conditions, the optimized catalyst achieves 85% NOx conversion (vs 40% for conventional In@H-Beta). The enhanced water resistance is attributed to two factors: first, Fe2O3 establishes a physical barrier that protects acid sites and stabilizes InO+ active sites via Fe–O–In bonding, thereby inhibiting hydroxylation; second, strong interfacial Fe–O–In interactions further stabilize InO+ active sites against aqueous deactivation. Additionally, the Fe2+/Fe3+ redox cycle is proposed to facilitate O2 activation. In situ DRIFTS studies under 5% H2O confirm effective CH4 activation, as indicated by markedly more intense C–H stretching bands compared with In@H-Beta. The reaction pathway involves NO activation over Brønsted acid sites to form nitrate species, and CH4 activation on InO+ sites generating methyl radicals, which subsequently participate in NOx reduction. This work offers a new design strategy for developing highly active and water-tolerant CH4-SCR catalysts suitable for industrial flue gas treatment.
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ACS Catalysis
·
2026
·
IF 13.6
Jun-Bin He,Lian Wu,Wenli Yuan,Hai-Xue Pan,Binju Wang,Gong-Li Tang
Achieving highly regioselective C–H bond functionalization at the bridgehead carbon of a single molecule is a fascinating, yet formidable challenge. BcmD, a P450 enzyme, catalyzes the regioselective hydroxylation at the sp3-hybridized bridgehead carbon of the bicyclo[4.2.2]piperazinedione ring scaffold during bicyclomycin biosynthesis. Herein, we provide mechanistic details of BcmD to understand its substrate binding and the origin of its regioselectivity. The high-resolution structure of SoBcmD from Streptomyces ossamyceticus in complex with its natural substrate, together with site-directed mutagenesis and computational simulations, reveals that the precise substrate positioning, enabled by specific hydrogen-bonding and hydrophobic interactions with crucial residues, determines the regioselectivity. Intriguingly, we identify SoBcmD as a peroxygenase that could utilize H2O2 as an oxidant to catalyze regioselective hydroxylation. Mechanistic analysis indicates that H2O2 activation in SoBcmD involves a homolytic cleavage process, mediated by a hydrogen-bonding network comprising residues T277, A273, and the substrate. Furthermore, structure-based channel analysis and mutagenesis demonstrate that the I157V mutant exhibits significantly enhanced peroxygenase activity. These findings advance our understanding of regioselectivity control in BcmD and provide valuable guidance for engineering P450 peroxygenases for the C–H bond activation at the chemically challenging bridgehead carbon sites.
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