PHYSICAL REVIEW B
·
2026
·Vol. 113
·期 8
·085117
·
IF 3.9
Ruifeng Tian,Jie Chen,Feng Wu,Jiayi Guan,Zhiyan Shao,Wei Wu,Mingwei Ma,Zhiwei Hu,Haoyu Zheng,Pengda Ye,Yuxiang Chen,Hua Zhang,Yanfeng Guo,Meiling Jin,Jiabin Qiao,Fan Yang,Xiang Li
Materials tunable between heavy-fermion metals and antiferromagnetic insulators near quantum criticality are promising candidates for exploring unconventional superconductivity, yet such a behavior is rare in transition metal oxides. Here, we report the high-pressure synthesis and characterization of two Pb-based $A$-site ordered perovskites, ${\mathrm{PbCu}}_{3}{\mathrm{Ru}}_{4}{\mathrm{O}}_{12}$ and ${\mathrm{PbCu}}_{3}{\mathrm{Ti}}_{4}{\mathrm{O}}_{12}$, which are characterized as a heavy-fermion metal and an antiferromagnetic insulator, respectively. Systematic $B$-site substitution in ${\mathrm{PbCu}}_{3}{\mathrm{Ru}}_{4\ensuremath{-}x}{\mathrm{Ti}}_{x}{\mathrm{O}}_{12}$ ($x=0\ensuremath{-}4$) reveals a continuous evolution of electronic and magnetic properties, with intermediate compositions exhibiting divergent low-temperature specific heat, indicative of proximity to a quantum critical point. The experimental observation supported by density functional theory calculations reveal that ${\mathrm{PbCu}}_{3}{\mathrm{Ru}}_{4}{\mathrm{O}}_{12}$ exhibits more enhanced effective mass than ${\mathrm{CaCu}}_{3}{\mathrm{Ru}}_{4}{\mathrm{O}}_{12}$, attributed to its enhanced Fermi-level density of states and narrower bandwidth, driven by the elongated Ru-O bonds and the covalent character of ${\mathrm{Pb}}^{2+}$. These results establish ${\mathrm{PbCu}}_{3}{\mathrm{Ru}}_{4\ensuremath{-}x}{\mathrm{Ti}}_{x}{\mathrm{O}}_{12}$ as a rare platform to study quantum criticality and strong correlations in transition-metal oxides and demonstrate that combine $A$-site and $B$-site tuning provides an effective route to tailor electronic and magnetic properties.
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Journal of Water Chemistry and Technology
·
2023
·Vol. 45
·期 2
·164-175
·
IF 0.6
Jing Meng,Geng Cong,Guan Yinyan,Gao Weichun,Ming Hao,Li Dan,Wang Nan,Liu Shiyue,Jiang Wei,Liang Jiyan,Wang Xueying
Abstract The sol-gel approach was utilized to make a copper-doped Ti/SnO 2 -Sb anode for electrochemical oxidation of norfloxacin (NOR). Sycanning electron microscopy (SEM), energy dispersive spectrometry (EDS), X-ray diffraction (XRD), linear scan voltammograms (LSV), and cyclic voltammetry (CV) were used to examine the anode’s surface morphology and electrochemical characteristics. The results show that the doped metal makes the anode coating denser and smoother, which is more conducive to resistance to electrochemical corrosion. The electrochemical degradation of NOR utilizing the constructed anode was examined in relation to reaction circumstances such as current density, pH value, and initial NOR concentration. Within the selected range of reaction conditions, the removal rate of NOR using Ti/SnO 2 –Sb–Cu electrode was significantly higher than that of blank electrode. The following were the shifting trends: NOR removal efficiencies grew with applied current density and initial NOR concentration, and reduced with increasing pH value. Water samples with different reaction times were taken and tested by UV-Vis spectrum. As can be seen from the results, with the progress of the reaction, the intensity of the characteristic peak decreased, indicating that NOR is degraded gradually. The electrochemical degradation pathways of NOR were studied using liquid chromatography coupled with mass spectrometry (LC-MS). Six intermediates were detected and a possible reaction pathway for the degradation of NOR by electrochemical oxidation was proposed.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2023
·
IF 8.7
Wei Wang,Xiangyu Jin,He Huang,Shuang Hu,Can Wu,Hebing Wang,Yiwu Pan,Changqing Hong,Xinghong Zhang
Ablative thermal protection systems are considered to be one of the most promising means of protection for spacecraft re-entry, but challenges remain. Herein, efficient Ti-Si binary modified carbon fiber reinforced phenolic aerogel nanocomposites (C f /TS-PR) were originally designed based on a multi-stage construction strategy. The C f /TS-PR exhibited desirable mechanical strength , good thermal insulation with a minimum thermal conductivity of 0.0756 W/(m·K), remarkable thermal stability and outstanding ablation resistance, benefiting from the features of TiO 2 and the special structure of TiO 2 -SiO 2 coating. The linear ablation rates are as low as 0.004 and 0.003 mm/s at the heat flow of 1.0 and 1.5 MW/m 2 , respectively. The mass loss rates are as low as 0.006 and 0.009 g/s at the heat flow of 1.0 and 1.5 MW/m 2 , respectively. These results indicate that the C f /TS-PR nanocomposites can be a reliable thermal protection material for the future high-temperature service environment of ultra-high-speed vehicles and neutral rockets.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3517-3525
·
IF 4
Shihui Wang,Zhoujun He,Ling Wu,Deling Wang,Ruiru Si,Xiyao Liu,Ruowen Liang
Due to their explicit structure, metal–organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)–NH2 (denoted as MTi), UiO-66(Zr)–NH2 (denoted as UZr) and MIL-68(In)–NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface –N⋯Ti– coordination species. The coordination–photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.
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Catalysts
·
2023
·Vol. 13
·期 6
·971
·
IF 3.9
Chunjie Shi,Xiaofeng Yu,Wei Wang,Haibing Wu,Ai Zhang,Shengjin Liu
The catalytic activity and cyclic catalysis of different methyl benzoates were studied by using a series of Lewis solid acid catalysts. The iron-supported zirconium/titanium solid acid catalysts were characterized using FTIR, SEM, XRD, and BET. The details of catalytic activity and cyclic catalysis verified that the catalyst catalyzed the reactions of 31 benzoic acids with different substituents and methanol. In addition, the mechanism was revealed according to the microstructure, acid strength, and specific surface area of the catalysts, and the yields of methyl benzoates by the GC-MS. Zr ions had significant effects on the catalytic activity of the catalyst. A certain proportion of Fe and Ti ions additionally enhanced the catalytic activity of the catalyst, with the catalyst-specific composition of Fe:Zr:Ti = 2:1:1 showing optimal catalytic activity. A variety of substituents in the benzene ring, such as the electron-withdrawing group, the electron-donating group, large steric hindrance, and the position of the group on the benzene ring, had regular effects on the catalytic activity of the methyl benzoates. An increase in the catalyst activity occurred owing to the increases in the catalyst surface and the number of acid sites after the Fe ion was added. The catalytic activity remained unchanged after the facile recycling method was performed.Keywords:zirconium/titanium solid acid;iron-supported;methyl benzoate compounds
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AICHE JOURNAL
·
2022
·Vol. 69
·期 5
·e17999
·
IF 4.167
Dong Lin,Yang Xu,Xiuhui Zheng,Wei Sheng,Zhenyi Liu,Yinglong Yan,Yu Cao,Yibin Liu,Xiang Feng,De Chen,Chaohe Yang
Regulating the microenvironment of active sites is crucial to boost the performance of direct propene epoxidation with H 2 and O 2 . Herein, the enhanced surface transfer of H 2 O 2 intermediates was first achieved by sodium-decorated Au-Ti bifunctional active sites. Combined with multi-techniques (e.g., operando UV–vis–NIR system, DFT studies and quantitative model calculations), it is found that the sodium-decorated silanols (Si-ONa species) on the TS-1 support enhance the formation of Ti-OOH intermediates by restraining H 2 O 2 decomposition. In addition, sodium-decorated silanols improves the desorption of propylene oxide, suppressing its ring-opening and formation for the carbonaceous deposits. Moreover, the sodium-decorated Au nanoparticles with smaller diameter and higher electron density further strengthen O 2 adsorption and boost the H 2 O 2 formation. This work not only provides fundamental understandings on the microenvironment of Au-Ti bifunctional catalysts but also sheds new light on enhancing the performance by boosting the surface molecular transfer.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Lijun Guo,Liming Zhao,Yuling Tang,Jianfei Zhou,Bi Shi
Efficient degradation of organic contaminants by oxidative radicals remains a challenge due to invalid consumption of radicals and easy generation of secondary halogenated pollutants. In this work, an efficient and recyclable bimetallic biochar (Cr-Ti/BC) was developed through peroxydisulfate (PDS) activation via nonradical pathway for sulfamethoxazole (SMX) degradation. The Cr-Ti/BC exhibited excellent catalytic activity for 99.9 % of SMX removal with a high k obs of 0.13 min −1 , and negligible inhibitory effects were observed under various pH condition. The activation mechanisms were (i) metastable reactive intermediates (Cr-Ti/BC-PDS) formation via an interaction between Cr-Ti/BC and PDS on the active defective sites (e.g., OH/C O C, COOH, C O, nitric oxides, graphitic N, and pyridinic N), and (ii) 1 O 2 generation through electron transfer between Cr-Ti/BC-PDS intermediates and dissolved oxygen. The high reusability and strong stability of Cr-Ti/BC also verified the outstanding advantage of the Cr-Ti/BC during practical application. This study not only is the first study the catalytic performance of Cr and Ti co-doped biochar for PDS activation, but also successfully provides a promising strategy to induce a nonradical pathway for PDS activation, which is of great significance for the subsequent method design, and thus paving the path for exploiting advanced oxidation systems in practical application for organic contaminant removal toward polluted site remediation.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Zijun Yang,Qiang Yu,Hua Wang,Qingfeng Ge,Xinli Zhu
Ketonization of propionic acid has been investigated on Lewis acidic TS-1 and Ti-Beta zeolites to understand the reaction mechanism and effects of pore topology and hydrophobicity. Characterizations showed that TS-1 and Ti-Beta (Si/Ti = 40) exhibited a similar acidity whereas TS-1 was more hydrophobic than the silanol-rich Ti-Beta. TS-1 showed higher activity, selectivity, stability and was more resistance to H 2 O than Ti-Beta. A combination of infrared spectroscopic, isotopic and kinetic studies showed that the molecularly adsorbed monodentate propionic acid is the most abundant reactive intermediate, and C-C coupling is the rate-determining step. The mechanism of ketonization of propionic acid at isolated tetrahedral Ti centers can be described by a Langmuir-Hinshelwood model. The turnover rate on TS-1-40 is ∼ 1.3 times higher than that on Ti-Beta-40, which is consistent with the lower fitted free activation energy, i.e., the energy difference between C-C coupling transition state and two co-adsorbed propionic acids at a Ti center. The slightly lower activation enthalpy on Ti-Beta-40 than TS-1-40 is over-compensated by much larger entropy penalty, due to more silanol groups and hydrogen bonded propionic acids in close proximity to the Ti center for Ti-Beta-40, which impose additional steric hindrance to bulkier C-C coupling complex at transition state and outweigh the difference of steric hindrance of pore confinement between MFI and BEA frameworks. This work provides insight into the ketonization mechanism on Lewis acidic zeolites, and indicates that moderate pore size with hydrophobic property promotes ketonization of carboxylic acid at isolated tetrahedral Ti centers confined in zeolites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jing Li,Guo Lin,Fangguan Tan,Likang Fu,Biao Zeng,Shixing Wang,Tu Hu,Libo Zhang
In the context of industrialization and severe wastewater pollution, mercury ions pose a major threat due to their high toxicity. However, traditional adsorbents and common metal-organic framework (MOF) materials have limited effectiveness. This study focuses on combining magnetic materials with functionalized titanium-based MOF composite (SNN-MIL-125(Ti)@Fe 3 O 4 ) to improve mercury ion adsorption. Through comprehensive characterization and analysis, the adsorption performance and mechanism of the material were studied. The optimal adsorption of the material was achieved at pH 5, exhibiting a pseudo-second-order adsorption model and the Hill theoretical capacity of 668.98 mg/g. Hill and Tempkin models confirmed the presence of chemical and physical adsorption sites on the material surface. Thermodynamic experiments showed a spontaneous endothermic process. Despite the presence of interfering ions, the material exhibited high selectivity for mercury ions . After four cycles, adsorption performance decreased by only 8%, indicating excellent reusability. Nitrogen- and sulfur-containing functional groups played a key role in mercury ion adsorption. In conclusion, SNN-MIL-125(Ti)@Fe 3 O 4 , as a magnetic MOF adsorption material, showed potential for effective remediation of mercury-contaminated wastewater. This study contributes to the development of efficient adsorption materials and enhances the understanding of their mechanism.
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CRYSTAL GROWTH & DESIGN
·
2023
·
IF 3.8
Caiyun Liu,Huihui Niu,Dexin Wang,Yanshu Liu,Amir Said,Guo Wang,Chen-Ho Tung,Yifeng Wang
Selective oxidation utilizing sunlight and O2 is a cost-effective technique for converting organic raw materials into value-added products. We present a novel Bi-doped Ti-oxide cluster (TOC), Ti19Bi2, for the selective conversion of benzyl alcohols to benzaldehydes under sunlight irradiation. It is prepared as single crystals and precisely characterized by single-crystal X-ray diffraction. A structure–activity study is performed by combining experiments and density functional theory. Bi mainly contributes to the LUMO + 1 of Ti19Bi2, with a minor effect on the band gap energy. Bi doping causes the accumulation of photogenerated electrons at Bi sites, resulting in potent reducing power and high O2 activation ability, promoting charge separation and interfacial charge transfer. The Ti19Bi2 solar system showed good activity, selectivity, substrate scope, and catalyst recyclability in the selective oxidation of benzyl alcohols. It outperforms reference TOCs free of Bi, such as Ti8O8Bz16 (Bz = benzoate) and commercial TiO2 P25. Additionally, Ti19Bi2 is effective in photocatalytic CO2/epoxide cycloaddition and dye degradation reactions.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 27
·7885-7895
·
IF 4.478
Zhang Xiaoya,Feng Quanshou,Xie Zehu,Xu Fuxing,Yan Yinghua,Ding Chuanfan
In this work, on the basis of an immobilized metal ion affinity chromatography enrichment strategy, a new kind of covalent organic framework (COF) material for enrichment of phosphorylated peptides and exosomes was successfully prepared in a facile method, and Ti 4+ and Nb 5+ were used as dual-functional ions (denoted as COF-S–S-COOH-Ti 4+ /Nb 5+ ). With the advantage of unbiased enrichment towards phosphopeptides, COF-S–S-COOH-Ti 4+ /Nb 5+ shows ultra-high selectivity (maximum molar ratio of β -casein: BSA is 1:20,000) and low limit of detection (0.2 fmol). In addition, the material has an excellent phosphopeptide loading capacity (100 μg/mg) and reusability (at least seven times). Furthermore, applying the material to the actual sample, 4 phosphopeptides were selectively extracted from the serum of renal carcinoma patients. At the same time, exosomes with an intact structure in the serum of renal carcinoma patients were successfully isolated rapidly using this strategy. All experiments have shown that COF-S–S-COOH-Ti 4+ /Nb 5+ exhibits exciting potential in practical applications. Graphical abstract
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Zhicheng Zhang,Chao Xu,Xudong Xiong,Chen Wang,Qi Zhang,Zhao Fan,Yongqian Wang
The application of CdS in pollutant degradation was limited due to the rapid compounding of photogenerated carriers. A ternary Au@NH 2 -MIL-125(Ti)/CdS (5Au@40NMT/CdS) composite catalyst was synthesized with a two-step method and methylene blue (MB) was used as simulate contaminants to evaluate its photocatalytic performance under simulated visible light. The compounding of NH 2 -MIL-125 and the loading of Au nanoparticles significantly enhanced the photodegradation performance of the composite catalyst. Compared with pure CdS, the ternary composite catalyst exhibited higher degradation efficiency (93.3 %) and higher degradation rate (9 times that of CdS)within 30 min, which was attributed to the high specific surface area and the synergistic effect of the three components that accelerated the carrier separation and broadened the photoresponse range. In addition, superoxide radical (·O 2 - ) was identified as the main active species in the MB degradation process by the electron spin resonance (ESR) technique. This work was expected to give a strategy for the fabrication and design of CdS/MOF composite catalysts in the field of pollutant degradation.
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