Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Ye Runping,Ma Lixuan,Mao Jianing,Wang Xinyao,Hong Xiaoling,Gallo Alessandro,Ma Yanfu,Luo Wenhao,Wang Baojun,Zhang Riguang,Duyar Melis Seher,Jiang Zheng,Liu Jian
CO 2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-O V -Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kg cat −1 ·h −1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO 2 with abundant oxygen vacancies can facilitate H 2 dissociation energetically and thus improve CO 2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.
研究领域:
催化
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化学工程
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材料科学
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环境科学
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高影响因子
MICROCHIMICA ACTA
·
2026
·Vol. 193
·期 4
·239
·
IF 5.4
Li Guangyan,Cheng Xiu,Zhu Minnan,Tian Yayang,Chen Linfeng
To address the need for rapid detection of profenofos (PFF) residues, we developed a self-cascaded colorimetric sensor using the bifunctional nanozyme Ce-UiO-66@His, prepared by doping histidine (His) into Ce-UiO-66. The introduction of His optimized the valence state distribution of cerium and increased the concentration of oxygen vacancies, thereby endowing Ce-UiO-66@His with enhanced phosphatase-like and laccase-like activities. Crucially, these two enzymes can efficiently catalyze in sequence under the same catalytic conditions, thereby achieving an integrated self-cascaded catalytic reaction of PFF. Specifically, the phosphatase-like activity hydrolyzes PFF to generate 4-bromo-2-chlorophenol, which is then oxidized by the laccase-like activity and coupled with 4-aminoantipyrine to form a red quinone-imine dye with strong absorbance. This self-cascaded, dual-recognition system provides exceptional selectivity and high sensitivity for PFF, with a detection limit of 0.71 µg/mL. Furthermore, by integrating smartphones and RGB recognition, a portable photo-colorimetric method was developed that realizes rapid and visual quantification of PFF. This work not only presents a new strategy for rapid monitoring of PFF residues but also offers insights into designing efficient biomimetic self-cascaded sensing systems. Graphical abstract
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LANGMUIR
·
2025
·
IF 3.9
Chao Zhang,Changhua Li,Xiaoxia Huang,Jing Zhang,Xiaoyu Mao,Wei Ren,Yi He
The long-term corrosion resistance of metal coatings remains a persistent challenge. Single nanofillers often fail to address this issue comprehensively. Herein, siloxene (S) was employed as a substrate to construct a composite structure integrating polyaniline (PANI) and Ce-MOF. The PANI structure imparts passive corrosion protection to the coating, while the pH-responsive Ce-MOF structure endows the coating with efficient self-healing capability. In addition, the fibrous PANI and the unique flexible structure of Ce-MOF endow the two-dimensional S sheets with good load-bearing capacity, thus enabling the composite coating to exhibit enhanced mechanical properties, which include adhesion strength, tensile performance, and wear resistance. It is found through research that the |Z|0.01 Hz of the composite coating increases by 1.5 orders of magnitude in the initial stage of immersion, and the tip current value decreases by more than 80% after being immersed for 20 days. A more than 80% decrease in wear rate is observed in the composite coating, and the adhesion, tensile strength, and tensile modulus of the coating are significantly improved. This study offers significant perspectives on the development of versatile nanofillers for epoxy coatings and establishes an application strategy for S materials in metal coating systems.
研究领域:
材料科学
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腐蚀工程
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高分子科学
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纳米技术
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表面工程
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CARBON
·
2023
·
IF 10.9
Qingyuan Zhao,Wenjie Zhao,Yinghao Wu
The limited interfacial combination between CF and polymer matrix caused by the chemical inertness of CF surface greatly restricts the protective capability of carbon fiber reinforced polymer coatings (CFRPCs), which could not effectively resist the impact of external forces, especially in the severe and complicated ocean environment (like deep-sea area and splash zone). Hence, it is the crux to enhance the interface compatibility and interface strength between fiber and resin. Based on the reliable compatibility between imidazole and epoxy as well as the corrosion inhibition effects of cerium-based compounds, a kind of bi-functional metal-organic framework (MOF) called the cerium-imidazole framework (Ce-MI) was constructed on the CFs surface via in-situ growth method to improve the interface compatibility and interface strength of fiber and resin and further increase protective performance of epoxy (EP) coating under the simulated deep-sea area and splash zone . After 168 h immersion under alternating hydrostatic pressure, CF@Ce-MI/EP coating displayed impressive impermeability and anti-corrosion performance, and the interfaces of fiber/epoxy adhered firmly. After the erosion wear test, the volume loss and mass loss of CF@Ce-MI/EP were decreased by 23.77% and 14.80%, respectively, compared with CF/EP. Finally, we discussed the protective mechanism of composite coating to reveal the different processes of interface failure caused by the high pressure and the impact of solid particles , respectively.
研究领域:
材料科学
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化学工程
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APPLIED SURFACE SCIENCE
·
2026
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IF 6.6
Jialong Shi,Haijie Chen,Sijia Chen,Xiaolong Liu,Dapeng Feng,Zhiwen Zheng,Dan Qiao
The development of advanced lubrication technologies is essential for enhancing energy efficiency, reducing environmental impact, and improving mechanical durability. In this study, a high-performance lubrication system tailored for diamond-like carbon (DLC) coatings is designed, employing graphene oxide-functionalized cerium-based metal–organic framework (GO@Ce-MOF) composites as nano-additive in an aqueous polyethylene glycol (PEG) solution. The GO@Ce-MOF hybrids were synthesized via electrostatic self-assembly, demonstrating outstanding tribological characteristics with an exceptionally low coefficient of friction (COF ≈ 0.004) and minimal wear on DLC substrates. Post-friction analysis confirmed that the structural integrity of the DLC coating remained unimpaired, with wear predominantly localized on the opposing steel balls. A bilayer tribofilm, approximately 45.5 nm thick and composed of metal oxides and amorphous carbon, formed on the steel surface, facilitating a transition to carbon/carbon friction interfaces. The rod-like architecture of the cerium-based metal–organic framework (Ce-MOF), encapsulated by layered graphene oxide (GO), synergistically contributed to reduced rolling friction and provided carbonaceous precursors for in situ tribofilm formation. This solid–liquid lubrication synergy enabled superlubricity and near-zero wear. The findings demonstrate a novel strategy for promoting in situ growth of carbonaceous tribofilms on dual friction interfaces, offering transformative potential for sustainable lubrication of advanced coating materials.
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MOLECULES
·
2026
·Vol. 31
·期 4
·740
·
IF 5.1
Quan Xiang,Linzhu Zhang,Lu Chen,Ruowen Liang,Renkun Huang,Guiyang Yan
Catalytic systems that couple pollutant degradation with hydrogen evolution have attracted significant attention due to their potential to simultaneously address environmental and energy issues. In this study, an S-scheme heterojunction composed of lamellar polymeric carbon nitride (PCN) anchored with a rod-like cerium metal–organic framework (Ce-MOF) was successfully synthesized via a facile one-step oxidation method, enabling efficient visible-light-driven photocatalytic hydrogen evolution and simultaneous tetracycline degradation. The optimized PCN/Ce-MOF composite delivers a hydrogen production rate of 495.7 μmol g−1h−1and achieves a tetracycline removal efficiency of 78%. Such excellent performance is attributed to the charge transfer mechanism of the S-scheme heterojunction in the PCN-Ce-MOF composite during the reaction process, while retaining the intrinsic redox capabilities of both materials. Meanwhile, mechanistic studies reveal that tetracycline can effectively capture holes during its efficient degradation, inhibit electron–hole recombination, and promote proton reduction to generate hydrogen. This investigation provides valuable insights for the rational design of S-scheme heterojunction photocatalysts, aiming to achieve efficient and stable photocatalytic hydrogen production and synergistic degradation of organic pollutants.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
·
IF 6.3
Zhuohan Zhang,Zhichao Yu,Lian Cong,Lixiang Ma,Yuan Li,Zhaoyang Liu,Yaokun Fu,Lu Zhang
MgH 2 exhibits significant potential as promising candidates for next-generation hydrogen storage solutions, owing to excellent hydrogen storage capacity. However, its high thermodynamic stability and kinetic barriers result in sluggish dehydrogenation kinetics and high dehydrogenation temperatures. Herein, oxygen vacancy (O V )-rich CeO 2 @C effectively weakens the Mg–H bond energy, which is manifested as the elongation of the Mg–H bond. Moreover, the O V -rich CeO 2 @C reacts with H 2 to form CeH 2.73 , which enhances hydrogen diffusion within the Mg/MgH 2 system. Meanwhile, the formation of CeH 2.73 promotes the formation of O V within the MgH 2 -CeO 2 @C, further facilitating the dehydrogenation of MgH 2 . Thereby, the synergistic effect of the O V -rich CeO 2 @C and CeH 2.73 lower the dehydrogenation temperature of MgH 2 and enhance kinetic performance. The MgH 2 -CeO 2 @C-3h behaves the most optimal dehydrogenation performance, achieving a release of 4.88 wt% H 2 within 10 min at 350 ℃. The initial dehydrogenation temperature of the MgH 2 -CeO 2 @C-3h is reduced to 274 ℃, and the dehydrogenation activation energy ( E a ) is lowered to 99.13 kJ mol –1 , compared to 327 ℃ and 160.7 kJ mol –1 for pristine MgH 2 . This work provides new insights into designing O V -rich metal oxide catalysts for MgH 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiaojie He,Yuhong Xu,Wei Wang,Bo Hu,Zijie Wang,Xin Yang,Yu Wang,Liwei Yang
A series of hierarchical micro/nano Ce-based composites were derived from Ce-MOF via thermal treatment in N 2 atmosphere. Different from conventional complete decomposed materials, forming cerium oxide in air, Ce-MOF that calcinated in N 2 at lower temperatures (400 °C or 500 °C) showed a partial thermal decomposition with high percent content of Ce(III). Even though the complete decomposed products held higher surface areas, the partial decomposed samples exhibited extremely higher phosphate uptake, with working capacity 2–4 times higher than that of ceria. The results implied a predominant effect of different valence states on phosphate removal by Ce-based materials, in which Ce(III) species were demonstrated playing the major role to form binding with phosphate. The maximum adsorption capacity (189.4 mg/g) was achieved by Ce-MOF-500(S) with wide applicable scope of pH ranging from 2 to 12 and great selectivity for phosphate in the presence of competing anions. Remarkably, Ce-MOF-500(S) described obvious enhanced phosphate adsorption ability under alkaline condition. This was due to the fact that the hydrolyzed Ce(III) species brought more active sites in the form of hydroxyl groups for ligand exchange with phosphate. Furthermore, based on the analysis of FTIR, XPS, XRD and zeta potential, electrostatic attraction, ligand exchange and surface precipitation were confirmed as the main adsorption mechanisms for partial decomposed samples, while electrostatic attraction was the main mechanism for complete decomposed samples.
研究领域:
环境科学
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材料科学
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ANALYST
·
2022
·Vol. 147
·期 23
·5355-5362
·
IF 5.227
Yi Xia,Jiaxin Zhou,Yanying Liu,Yutong Liu,Ke Huang,Huimin Yu,Xue Jiang,Xiaoli Xiong
Due to their high catalytic activity, stability and low cost, nanozymes with oxidase-like activity have attracted widespread interest in the fields of analytical detection and colorimetric sensing. To further promote the catalytic activity and the sensitivity of dopamine (DA) sensing, herein, a mixed valence Ce-MOF (MVCM) with enhanced oxidase-like activity was synthesized by the dielectric barrier discharge (DBD) microplasma method. Compared with hydrothermal synthesis, the prepared MVCM synthesized using a microplasma showed a higher catalytic activity, which benefits from a low Ce3+/Ce4+ ratio. Due to the spontaneous redox properties of Ce3+/Ce4+ in a MVCM, the MVCM-based colorimetric sensing of dopamine was established and showed a limit of detection of 0.74 μM over a linear range of 5–100 μM with high selectivity and stability and has been applied for the detection of dopamine in sweat. The proposed study provides an effective synthesis method for nanozymes with enhanced activity and shows great promise in widespread analytical and sensing applications.
研究领域:
材料科学
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分析化学
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生物传感
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Redox Biology
·
2026
·
IF 16.2
Yaping Chen,Kaichen Zeng,Yunxin Ye,Xinyi Sun,Ling Yan,Ziya Lao,Yifan Wu,Tao Luo,Li Yang,Lvhua Guo
In situ integration creates an electronically coupled Ce MOF-CD nanozyme. • Interfacial electron transfer regulates the Ce 3+ /Ce 4+ redox balance. • pH-dependent catalysis switches from ROS generation to superoxide removal. • Ce MOF-CD reduces inflammation and accelerates MRSA-infected wound healing. Infected wounds require therapeutic materials that can control bacterial infection without aggravating oxidative tissue damage. Here, glutathione-derived carbon dots (GSH-CDs) were introduced during the formation of a cerium metal-organic framework (Ce MOF) through an in situ integration strategy to construct a carbon-dot-integrated Ce MOF nanozyme (Ce MOF-CD). Electronic-structure analyses supported interfacial electron redistribution from GSH-CDs toward Ce MOF, accompanied by changes in the local electronic environment and Ce 3+ /Ce 4+ distribution of the Ce active centers. Ce MOF-CD exhibited a distinct pH-dependent redox catalytic preference, with oxidase-like catalysis favored under acidic conditions and superoxide dismutase-like activity becoming more pronounced near neutrality. Accordingly, Ce MOF-CD markedly reduced the viability of MRSA and E. coli and disrupted established biofilms under acidic conditions. Under near-neutral cellular conditions, it reduced intracellular oxidative stress, attenuated inflammatory activation, and promoted repair-associated macrophage polarization. In an MRSA-infected wound model, Ce MOF-CD reduced bacterial burden and local inflammation, promoted tissue reconstruction, and accelerated wound closure with favorable biosafety. Overall, GSH-CDs-mediated interfacial electronic regulation modulates the pH-dependent redox catalytic behavior of Ce MOF, enabling antibacterial activity to be coordinated with oxidative-stress regulation during infected wound healing. Download: Download high-res image (393KB) Download: Download full-size image
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MICROCHIMICA ACTA
·
2026
·Vol. 193
·期 7
·455
·
IF 5.4
Zhao Zhenghong,Xu Yue,Xu Shuzhen,Zhang Lianming,Li Jianping
The detection of carbohydrate antigen 19 − 9 (CA19-9), a critical serum marker for gastrointestinal malignancies, is particularly challenging because of its typically low concentration and substantial matrix interference, creating a critical demand for improved detection technologies. Herein, we rationally designed and synthesized a nanozyme with dual-ligand cerium-organic framework (Ce-MOF-BN) nanozyme for glycosyl-imprinted colorimetric biosensing via a one-pot method. The crystalline porous framework is densely functionalized on its surface with spatially accessible amino and boronic acid groups, enabling the recognition and oriented immobilization of imprinting templates. A well-defined core–shell molecularly imprinted composite was successfully fabricated through the systematic optimization of the ligand ratio. The composite exhibits intrinsic oxidase-like activity without requiring H 2 O 2 , and the molecularly imprinted polymer (MIP) shell supplies specific cavities for the highly selective recognition of CA19-9. Under optimized assay conditions, the sensor achieves the quantitative detection of CA19-9 across a broad linear range of 0.0001–100 U/mL, with a limit of detection as low as 2.7 × 10 − 5 U/mL. This work provides valuable insights for designing next-generation high performance biomimetic sensing materials and advancing their clinical diagnostic applications. Graphical The alternative text for this image may have been generated using AI.
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高影响因子
RARE METALS
·
2024
·
IF 9.6
Hu Xiao-Jie,Sun Yu-Han,Liu Ling-Yue,Mao Dan-Jun,Zheng Shou-Rong
Monochloroacetic acid (MCAA) is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water. In this study, a series of CeO 2 -supported Pd catalysts (Pd/MCeO 2 ) were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC (Ce-MOF), and the liquid-phase catalytic hydrodechlorination of MCAA was explored using these catalysts. For comparison, Pd/CeO 2 catalysts were additionally synthesized using the conventional impregnation method. The characterization results reveal that the catalysts exhibit strong metal–support interaction, leading to high Pd dispersion and Pd n + content. Additionally, the calcination temperature significantly influences catalytic performance, with the catalyst calcined at 500 °C (Pd/MCeO 2 -500) demonstrating the highest catalytic activity and achieving complete dechlorination of MCAA within 50 min. Furthermore, it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir–Hinshelwood model. Accordingly, low reaction pH is favorable for the catalytic hydrodechlorination of MCAA, enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface. Theoretical results suggest that the presence of Pd n + efficiently facilitates MCAA adsorption and C–Cl cleavage, thus significantly enhancing the liquid-phase catalytic hydrodechlorination. Graphical abstract
研究领域:
环境科学
·
催化化学
·
材料科学
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高影响因子
危险品化学品经营许可证（带存储）