ACS Nano
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2026
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IF 16
Xuan Zhao,Ruilong Shao,Yiruo Yu,Zhiwen Hu,Yiting Jiang,Yilan Zhou,Zibiao Zhong,Jinping Zhou
Sepsis is a life-threatening inflammatory syndrome caused by bacterial infections, with limited therapeutic options in critical care. Lipopolysaccharide (LPS) from Gram-negative bacteria triggers sepsis by activating toll-like receptor 4 (TLR4) through myeloid differentiation protein-2 (MD-2) binding. The phosphate groups in LPS serve as key recognition elements for this interaction. This study developed a zirconium/cerium (Zr/Ce) dual-metal nanozyme with phosphatase activity that catalyzes LPS dephosphorylation, disrupting LPS–TLR4 binding to inhibit NF-κB signaling and reduce inflammation. The nanozyme incorporated l-arginine and tannic acid (TA) to enhance the LPS binding capacity, while TA modification improved the antioxidant capability, constructing a multifunctional TA-Zr/Ce nanozyme. Results show that the nanozyme effectively catalyzes LPS dephosphorylation and suppresses inflammatory cytokine release from macrophages. In septic mice, TA-Zr/Ce treatment improved organ function, reduced systemic inflammation, and increased survival rates while promoting anti-inflammatory M2 macrophage polarization. Furthermore, this study constructed a regenerated cellulose microsphere (RCM)-based hemoperfusion system for loading nanozymes and efficiently removing LPS from blood, demonstrating strong clinical translation potential. Therefore, this research provides additional approaches and tools for the clinical management of sepsis.
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INORGANIC CHEMISTRY
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2026
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IF 4.6
Ling Wang,Mei Yan,Min Li,Zheng-Yu Yang,Xian Li,Wenfeng Zhou,Ru-Ling Tang
Zirconium/hafnium fluorides have recently garnered considerable interest as potential optical materials, owing to their short ultraviolet (UV) cutoff edges. Transforming centrosymmetric (CS) structures into noncentrosymmetric (NCS) analogues through cationic regulation has proven to be an effective approach for the development of nonlinear-optical (NLO) materials. Herein, various Zr/Hf-based fluorides with different alkali-metal cations, including K8M5F28(H2O) (M = Zr(1), Hf(2)), CsNaHfF6 (3), and LiK10M6F35(H2O)2 (M = Zr(4), Hf(5)), were synthesized. 1–3 belong to centrosymmetric space groups, whereas 4 and 5, incorporating the Li+ cation with a small radius, exhibit NCS crystal structures. 1 and 2 feature chain-like anionic structures. 3 presents a zero-dimensional (0D) anionic structure constructed from isolated [HfF6]2– octahedra. Compounds 4 and 5 adopt three-dimensional (3D) anionic networks. The introduction of Li+ enhances structural distortion and dipole alignment, resulting in phase-matchable (PM) second-harmonic-generation (SHG) responses. Notably, all compounds exhibit UV absorption edges below 200 nm, confirming superior UV transparency. Overall, these results indicate that alkali-metal regulation is an efficient approach to trigger symmetry breaking while concurrently enabling SHG activity and maintaining short UV absorption edges.
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Advanced Science
·
2026
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IF 14.1
Yanmin Liang,Hongyue Ma,Feier Bai,Jing Zhang,Yan Qi,Bing Shao
The interference of phospholipids in serum poses a critical bottleneck for nontargeted human biomonitoring of chemical hazards. Here, we report a Ti-doping strategy to activate adjacent Zr sites in a bimetallic Zr/Ti metal-organic framework (B-Zr/Ti MOF) for cooperative and efficient phospholipid removal. By precisely engineering the Ti content, the optimal B-Zr/Ti MOF achieves near-complete removal of major phospholipid subclasses while maintaining high recoveries (>50%) for over 500 diverse chemical hazards, even at trace levels (10 ng mL − 1 ). Combined XPS, FT-IR, and DFT calculations reveal that Ti incorporation modulates the local electronic environment, converting adjacent Zr sites into highly active Lewis acid centers that synergistically anchor phosphate headgroups via inner-sphere coordination. When integrated into a nontargeted LC-HRMS workflow, this material dramatically reduces matrix effects and expands detectable feature coverage. This work establishes bimetallic node engineering as a powerful strategy to overcome matrix interference in exposomics and precision biomonitoring.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Gan Ye,Jinghan Wang,Chundi Li,Lei Wu,Jun Zhou,Qiuli Zhang
A solvent-free strategy for the in situ implantation ZrW nanorods within Zr-FDCA was developed. • ZrW-Zr-FDCA retained hierarchical porosity, abundant oxygen vacancies and favorable oil-water wettability. • The optimized catalyst achieved complete oxidation of 1000 ppm sulfur to sulfone at 30 °C within 16 min. • The turnover frequency reaches 365.4 h −1 at 30 °C, which is 3653-fold higher than that of Zr-FDCA. • Tungsten active sites mediate H 2 O 2 activation to produce 1 O 2 as the primary reactive oxygen species. The rational design of highly effective desulfurization catalysts holds great promise for realizing exceptional synergistic catalytic activity toward the production of clean fuels. Herein, we provide a solvent-free strategy for the in situ implantation ZrW 2 O 7 (OH) 2 (H 2 O) 2 (ZrW) nanorods within a metal–organic framework (Zr-FDCA), using renewable organic linkers and Na 2 WO 4 ·2H 2 O as precursors. The resulting ZrW-Zr-FDCA composite retains hierarchical porosity, abundant oxygen vacancies and favorable oil-water wettability, which collectively promote interfacial contact and mass transfer in the biphasic system, thereby significantly enhancing oxidative desulfurization (ODS) performance at room temperature. The optimized catalyst achieves complete oxidation of 1000 ppm sulfur to sulfone at 30 °C within 16 min and maintains 96.7% sulfur removal efficiency over seven consecutive reaction cycles. Its turnover frequency reaches 365.4 h −1 at 30 °C, which is 3653-fold higher than that of Zr-FDCA. Quenching experiment and electron paramagnetic resonance spectroscopy identify W sites as the active centers responsible for H 2 O 2 activation, generating singlet oxygen as the dominant reactive oxygen species driving the ODS process. This work not only expands the one-pot solvent-free approach to encapsulate nanorods within MOFs but also provides an effective route for advancing low-temperature desulfurization. Download: Download high-res image (215KB) Download: Download full-size image
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ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 33
·14733-14742
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IF 7.6
Huang Yao-Bing,Wu Peng-Fei,Zhang Bo-Hao,Liu Qun-Xing,Wu Hao,Fei Teng,Lu Qiang
Selective hydrogenation of the conjugated carbon–carbon double bond (C═C) and carbon–oxygen bond (C═O) is an important reaction in organic synthesis, which not only provides access to key intermediates in natural product synthesis but also serves as a probe reaction for the evaluation of catalyst reactivity. However, the higher activation energy of the C═O bond over the C═C bond renders its reduction more challenging. In this work, we report a tailored zirconium (Zr)-doped zeolite catalyst featuring integrated Lewis and Brønsted acid sites for the selective transfer hydrogenation of the C═O bond of cinnamaldehyde (CAL) followed by etherification to yield 1-cinnamyl 2-propyl ether (CPE). A series of Zr catalysts supported on different zeolites were prepared and characterized. Among them, Zr-doped mesoporous SBA-15 (Zr/SBA-15) exhibited the highest reactivity, achieving complete conversion of CAL and 99% yield of CPE at 140 ° C in 7 h. Mechanistic studies revealed that balanced Lewis/Brønsted acid sites were key to the reaction, where Lewis acid sites primarily catalyzed the transfer hydrogenation of CAL to cinnamyl alcohol (COL), while Brønsted acid sites promoted the subsequent esterification of COL to CPE. The current work not only establishes an efficient one-pot approach for the synthesis of allyl ethers from α,β-unsaturated carbonyl compounds but also provides insights into tuning catalyst reactivity through support modification, which would benefit both fundamental research and industrial production.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2026
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IF 5.9
Litao Zhang,Ping He,Jiang Wu,Naichao Chen,Xingyu Cao,Wenchu Yuan,Zhengyu Liu,Xiao Zhang,Runyao Ma
A Zr/Br-doped core-shell UIO-type MOF optimized for efficient mercury removal. • Synergistic interaction between Zr 4+ and Br − formed dual-functional “oxidation-fixation” active sites. In coal-fired power plants, mercury is released into the atmosphere along with flue gas during the combustion of coal, posing serious threats to both the environment and human health. In this work, a novel core-shell structured Zr/Br dual-doped metal-organic framework adsorbent UIO-type-Zr-Br was successfully synthesized using a multi-step templating strategy with precise control of structural modulation. Through a combined strategy of ZIF-67@ZIF-8 NPs nano-etching and Zr/Br doping, the optimal sample UIO-15 exhibited excellent mercury removal performance, achieving over 98.8% removal efficiency at 120 °C. The UIO-15 adsorbent also demonstrated strong resistance to coal combustion flue gas interference components such as SO 2 (600 ppm) and NO (600 ppm), maintaining nearly 80% efficiency. Furthermore, long-term dynamic tests showed that UIO-15 retained approximately 95% efficiency after 10 h of continuous operation. The Zr 4+ and centers maintained the oxidation state throughout the reaction, indicating the role as structural stabilizers rather than redox-active sites, while Br − participated in the oxidation of elemental mercury Hg 0 to form stable HgBr 2 , which was subsequently immobilized within the MOF framework; Mercury removal was effected by dual-functional oxidation-fixation centers formed via synergistic Zr 4+ -Br - interactions. These findings suggest that UIO-15 is a promising candidate for practical application in mercury removal systems for coal-fired power plants. Download: Download high-res image (363KB) Download: Download full-size image
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Zhengshen Bao,Dehong Xu,Hailong Peng,Changqing Xia,Shixing Wang,Weili Li
Efficient recovery of Au (III) from aqueous wastewater is of great significance for resource utilization and environmental protection. Herein, azine-functionalized Zr-based MOFs (hereinafter referred to as AZA-Zr-MOFs) were prepared via a facile one-pot solvothermal route using 2,2'-diamino-4,4'-(4-amino-1,2,4-triazole-3,5-diyl) dibenzoyl acid as the organic linker. The abundant triazole and amino groups on the MOF surface provide multiple active sites for multi-nitrogen synergistic coordination, thus enhancing the selective capture of Au (III) in aqueous solution. The obtained AZA-Zr-MOFs exhibit a high maximum uptake capacity of 1176 mg/g for Au(III), along with remarkable selectivity and excellent cycling stability (＞90 % efficiency after 5 cycles) over a wide pH range (2.0~9.0). Combined with experimental analyses (X-ray photoelectron spectroscopy (XPS), zeta potential, Fourier transform infrared spectroscopy (FTIR)) and density functional theory (DFT) calculations, the liquid-phase adsorption mechanism of Au (III) is clarified as a synergistic effect of amino-assisted reduction (Au (III)→Au (0)), nitrogen-centered coordination on the MOF surface, and electrostatic interfacial interaction via protonated amino groups. This work provides a feasible preparation method for MOF-based adsorbents and reveals the key role of surface functional groups in the interfacial adsorption of Au (III), which has potential application value for Au (III) recovery from actual aqueous wastewater.
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JOURNAL OF CHROMATOGRAPHY A
·
2026
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IF 4
Haoxuan Song,Yingying Zhang,Keda Guo,Ruobing Jia,Yu Jia,Chenglong Xu,Hong Ye,Qiangqiang Xu,Shengpeng Shi
Magnetic Zr/Ce bimetallic CPs were prepared by a hydrothermal method. • Partial Ce substitution for Zr reduces cost of the bimetallic nodes. • Phthalic acid ligand offers electron-rich aromatic rings for π-π stacking. • DBP uptake reaches 1061–1172 mg/g at 600 mg/L, surpassing most adsorbents. • Magnetic separation enables reuse; capacity drops <5% after five cycles. Phthalate esters (PAEs), as endocrine-disrupting chemicals with reproductive toxicity, pose significant challenges to environmental protection and food safety due to their widespread occurrence and persistence in the environment. In this study, three Zr/Ce bimetallic coordination polymers (CPs) were successfully synthesized via a hydrothermal method combined with a post-modification coprecipitation strategy, using tetrafluoroterephthalic acid (BDC-F₄) and phthalic acid (PA) as mixed ligands. Fe₃O₄ was subsequently deposited in situ to impart magnetic responsiveness to the materials. All three materials exhibited excellent adsorption performance toward dibutyl phthalate (DBP), with adsorption capacities of 1061, 1128, and 1172 mg/g, respectively, at an initial DBP concentration of 600 mg/L, which were higher than the theoretical maximum adsorption capacities of most adsorbents reported in the literature. The adsorption kinetics followed the pseudo-first-order model, while the adsorption isotherms were better described by the Freundlich and Temkin models. Thermodynamic analysis indicated that the adsorption process was spontaneous and exothermic and was predominantly governed by physical adsorption. After five consecutive adsorption–desorption cycles, the average decrease in adsorption capacity was approximately 2.7%, demonstrating excellent structural stability and reusability. This study integrates Zr/Ce bimetallic nodes with mixed-ligand functional regulation, providing a magnetically separable adsorbent design strategy for the efficient and selective removal of PAEs from complex aqueous matrices. Download: Download high-res image (248KB) Download: Download full-size image
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Tao Cheng,Lu Liu,Jia Hui Chen,Pan Wang,Jian Ming Pan
Metal–organic frameworks (MOFs) exhibit a diverse array of applications in the fields of adsorption, catalysis, sensing, and separation. However, the limited water stability of MOFs poses challenges in the separation domain, particularly due to the structural similarities among water-soluble nucleoside compounds, which complicate the selective adsorptive separation of these compounds from complex mixtures. In this study, hydrophilic flower-like zirconium-based MOF nanosheets (Zr-FNSs) were prepared by a one-step hydrothermal method. The investigation focused on their adsorption capacity and the mechanism of action, with respect to various nucleosides. Adsorption experiments were conducted under varying pH conditions to identify the optimal pH and to assess the influence of phosphate number on the adsorption of adenosine compounds. The kinetic adsorption capacities of Zr-FNSs for adenosine monophosphate (AMP), adenosine diphosphate (ADP), and adenosine triphosphate (ATP) were determined to be 254.81, 211.35, and 182.97 μmol g–1, respectively, demonstrating a gradient decrease that may be attributed to increased spatial resistance or a limited number of available adsorption sites. Zr-FNSs have excellent regenerative properties. This work underscores the significance of functional group interactions in the selective adsorption of nucleoside and provides valuable insights for the design of MOF-based adsorbents for the selective separation and purification of nucleoside.
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NEW JOURNAL OF CHEMISTRY
·
2025
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IF 2.5
Hong Zhang,Wenlong Lu,Chen Li,Xinyu Chen,Lei Wang,Hui Wan,Guofeng Guan
In this study, Rh supported on SiO2 was modified with Zr for the first time to investigate its catalytic performance in propylene hydroformylation. The RhZr/SiO2 catalyst exhibits a butyraldehyde selectivity of over 90% along with a 2.7-fold enhancement in propylene conversion compared to the unmodified catalyst, outperforming previously reported Co- and K-promoted systems. XPS characterization, combined with differential charge density calculations and Bader charge analysis, revealed that the introduction of Zr reduced the electron density around Rh, which facilitates CO adsorption on Rh and thereby promotes the formation of more active HRh(CO)x species. This conclusion is further supported by CO adsorption energy calculations. Under optimized reaction conditions (20 mL toluene solvent, 0.4 g RhZr/SiO2 catalyst with ultralow Rh loading of 0.02 wt%, 1.5 g propene, 100 °C, 4 MPa syngas pressure, 4 h), the catalytic system achieved remarkable performance: 75.1% propene conversion, 96.7% butyraldehyde selectivity, and a normal/iso (n/i) ratio of 0.9. Notably, the system exhibited an exceptional intrinsic activity (TOF = 8838 h−1), surpassing all reported ligand-free heterogeneous Rh-based catalysts in recent years. The present work provides an effective strategy for designing modified Rh-based heterogeneous catalysts with ultralow metal loading for hydroformylation applications.
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AICHE JOURNAL
·
2025
·
IF 4
Jia Xiong,Qiang Sun,Hongxia Gao,Zhiwu Liang
Catalytic amine–based solution regeneration has attracted considerable attention due to its potential to reduce energy consumption in carbon dioxide (CO 2 ) separation. However, the limited catalytic activity and cycling stability of catalysts under high–temperature alkaline conditions hinder their industrial application. Herein, zirconium hydrogenphosphate (ZrHP) catalysts, featuring abundant acidic sites, were first utilized for amine solution regeneration. By leveraging its proton donation and acceptance mechanism, efficient monoethanolamine solution regeneration was achieved. The ZrHP–4 catalyst demonstrated a 526% increase in the instantaneous CO 2 desorption rate compared to the non–catalytic test, reducing the relative heat duty by 48%. Moreover, ZrHP–4 exhibited remarkable stability over 10 cycles without requiring regeneration. Density functional theory calculations revealed that ZrHP promotes CO 2 desorption by elongating the C—N bond of carbamate and lowering the proton transfer energy barrier. Therefore, this study offers novel insights into the design and mechanistic understanding of efficient and stable catalysts for amine solution regeneration.
研究领域:
化学工程
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催化科学
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环境科学
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International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 6
·1441-1450
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IF 7.2
Chen Xunlei,Chen Lin,Tian Jiang,Xu Cheng,Liao Jiaxin,Li Tianyu,Wang Jiankun,Feng Jing
Thermal and mechanical properties of yttrium tantalate (YTaO 4 ), a top coat ceramic of thermal barrier coatings (TBCs) for aeroengines, are enhanced by synthesizing Y 1− x Ta 1− x M 2 x O 4 (M = Ti, Zr, Hf; x = 0.06, 0.12, 0.18, 0.24) medium-entropy ceramics (MECs) using a two-step sintering method. In addition, the thermal conductivity, thermal expansion coefficients (TECs), and fracture toughness of MECs were investigated. An X-ray diffraction study revealed that the Y 1− x Ta 1− x M 2 x O 4 MECs were monoclinic, and the Ti, Zr, and Hf doping elements replaced Y and Ta. The variations in atomic weights and ionic radii led to disturbed atomic arrangements and severe lattice distortions, resulting in improving the phonon scattering and reduced thermal conductivity, with Y 1− x Ta 1− x M 2 x O 4 MECs ( x = 0.24) exhibiting the lowest thermal conductivity of 1.23 W·m −1 ·K −1 at 900°C. The introduction of MO 2 increased the configurational entropy and weakened the ionic bonding energy, obtaining high TECs (10.4 × 10 −6 K −1 at 1400°C). The reduction in the monoclinic angle β lowered the ferroelastic domain inversion energy barrier. Moreover, microcracks and crack extension toughening endowed Y 1− x Ta 1− x M 2 x O 4 MECs ( x = 0.24) with the highest fracture toughness of (4.1 ± 0.5) MPa·m 1/2 . The simultaneous improvement of the thermal and mechanical properties of the MO 2 (M = Ti, Zr, Hf) co-doped YTaO 4 MECs can be extended to other materials.
研究领域:
材料科学
·
机械工程
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危险品化学品经营许可证（带存储）