ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Xiaoxiao Wang,Yanmei Yang,Zhiqing Zhou,Yuling Zhong,Miaomiao Qin,Weiqing Wang,Weifeng Li,Bo Tang
5-hydroxymethylfurfural (HMF) is one of the most promising biomass-based chemicals that is used to produce many kinds of important compounds. Especially, the selective conversion of HMF to 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), an important chemical feedstock, has high industrial significance but is technically challenging. In this study, we present a high-performance photocatalyst for selective oxidation of HMF to HMFCA. By integrating an ultrasmall amount of palladium (Pd) nanoclusters (1.12‰ in weight) on defective hexagonal boron nitride nanosheets (Pd/defective h-BN nanosheets (dh-BNs)), outstanding photocatalytic performance can be achieved, resulting in up to a 95% HMF conversion ratio with an 82% HMFCA selectivity. The performance is considerably higher than that of pristine dh-BNs and Pd on defect-free h-BNs. More importantly, this Pd/dh-BNs catalyst maintains a high catalytic activity after eight cycles, demonstrating robust catalytic stability. Density functional theory calculations indicate that Pd/dh-BNs can lower the energy barrier for HMF oxidation and facilitate the desorption of HMFCA, which contributes to the high selectivity catalytic performance. This study not only introduces a promising photocatalyst for sustainable chemical transformations but can also provide valuable insights into the design of advanced photocatalytic material for biorefinery applications.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
·
IF 5.7
Jinye Huang,Xuan Xuan,Dongmei Xu,Yuezhong Wen
The regulation solutions and mechanisms of reducing pesticide phytotoxicity to nontarget plants are not well-defined and detailed. Here, we have proposed a new detoxification strategy to control the toxic effects of herbicide imazethapyr (IM) induced in wheat seedlings from the perspective of the plasma membrane (PM) H+-ATPase. We found that the changes in PM H+-ATPase activity have a regulatory effect on the phytotoxic effects induced by IM in plants. Treatment with PM H+-ATPase activators restored the reduced auxin content and photosynthetic efficiency caused by IM, thereby promoting plant growth. Application of a PM H+-ATPase inhibitor further reduced phosphorus content and significantly increased 2,4-dihydroxy-7-methoxy-2H,1,4-benzoxazin-3(4H)one (DIMBOA) and jasmonic acid levels. These effects indicate that auxin and DIMBOA may regulate plant growth trends and detoxification effects mediated by PM H+-ATPase. This work opens a new strategy for regulating herbicide toxicity to nontarget plants from the PM H+-ATPase.
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Small
·
2025
·
IF 12.1
Ruiqi Guo,Shujuan Wang,Minqi Sheng,Xingli Zou,Mingzhi Zhang,Guangcheng Li,Yi Cao,Zhenglong Fan,Jinxin Chen,Wenxiang Zhu,Fan Liao,Tianjiao Ling,Hao Ren,Fan Lv,Zhenhui Kang
Iridium (Ir) is recognized to have extremely high catalytic activity in the hydrogen evolution reaction (HER). However, there are still technical challenges in maximizing the utilization of Ir atoms in the catalytic reaction process through dimensional regulation strategies. Herein, an innovative strategy is utilized to fabricate porous phosphorus-doped iridium (P-Ir) with a 2D structure, specifically the reduction of 1T phase-IrO 2 (1T-IrO 2 ) nanosheets using phosphine gas. The optimized P-Ir achieves an overpotential of 17.2 mV (vs RHE without i R-correction) in 0.5 m H 2 SO 4 during the HER process, outperforming benchmark Pt/C (27.0 mV) and most reported Ir-based electrocatalysts. During the long-term stability tests, P-Ir maintains stable operation for more than 100 h at both −10 and −100 mA cm −2 , respectively. Moreover, the HER activity and transient potential scanning results of Ir-based phosphides prove that doping P atoms in the Ir lattice promotes the reaction kinetic rate and charge transport capacity during hydrogen evolution. Theoretical calculations reveal that P atoms doping weakens the adsorption energy of H intermediates (H*) by regulating the d -band center of the Ir sites. Simultaneously, the desorption process of H* is also facilitated by forming a special bridged-H* bond structure, eventually accelerating the HER kinetics.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Xinyuan Yan,Juan Chai,Luohao Yuan,Hongfeng Yin
Glutathione (GSH), as an significant intracellular antioxidant, plays a vital role in preserving the balance of cellular redox homeostasis. The accurate and sensitive detection of GSH is essential for understanding the cellular redox status and for the diagnosis and treatment of many diseases. Herein, a core–shell structure composed of glucose oxidase (GOx), platinum (Pt) nanoparticles and a zeolitic imidazolate framework (ZIF-8) shell was constructed. Pt NPs in the core–shell showed high peroxidase-like catalytic activity. The as-prepared Pt-GOx@H-ZIF-8 can be utilized for colorimetric detection of GSH, exhibiting a broad linear range from 0.5 to 90 μM, and a low limit of detection (LOD) of 0.4 μM. Pt-GOx@H-ZIF-8 showed excellent sensitivity, selectivity and stability towards glutathione detection, making it a promising candidate for intracellular antioxidants.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
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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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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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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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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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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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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