Journal of Materials Chemistry A
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2024
·Vol. 12
·期 10
·5875-5884
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IF 10.7
Hui Guo,Yifeng Li,Lulu Jiang,Yenan Sha,Shihang Guo,Donglin Han
Proton conducting oxides are attracting increasing attention due to their promising application as electrolytes in solid-state electrochemical devices for energy conversion and chemical production, including protonic ceramic fuel cells, electrolyzers and membrane reactors. BaZrO3 and Ba(Zr,Ce)O3 substituted by acceptor dopants are currently the most promising proton conductors. In principle, replacing Zr or Ce with one kind of trivalent element (e.g., Y or Yb) can generate oxygen vacancies, which are necessary for the hydration reaction to introduce charge carriers of protons. However, it is commonly recognized that substituting Zr or Ce with Y and Yb simultaneously leads to high performance of the devices, but the reason is not clear. In this work, we studied the transport properties of four different compositional classes: BaZr0.8−xCexY0.2O3−δ (BZCY20), BaZr0.8Y0.2−xYbxO3−δ (BZYYb), BaZr0.1Ce0.7Y0.2−xYbxO3−δ (BZCYYb) and BaCe0.8Y0.2−xYbxO3−δ (BCYYb), at 600, 650 and 700 °C. For BZCY20, the ionic conductivity decreases on replacing Zr in BZY20 with x = 0.1 of Ce, increases with increasing Ce content within x = 0.1–0.5, and decreases on further increasing Ce content from x = 0.5 to 0.8. The ionic transport number increases with increasing Ce content. The ionic conductivity, partial conductivity of oxide ions and hole conductivity of BZCYYb and BCYYb increase with increasing Yb content. Since the increment of hole conductivity is larger, the ionic transport number decreases. For BZYYb, the ionic conductivity decreases and the hole conductivity increases with increasing Yb content, leading to decreasing ionic transport number. Both the high ionic conductivity and transport number are vital factors governing the performance of protonic ceramic cells (PCCs). Therefore, the improved performance of PCCs by adding both Y and Yb into the electrolyte cannot be explained from the viewpoint of electrical properties of the electrolytes. Thereby, we summarized our recent series of studies on the chemical compatibility between the electrolyte and NiO negatrode substrate, and suggested that the loss of dopant was suppressed by partly replacing Y with Yb. The high ionic conduction of the electrolyte can be maintained after co-sintering at high temperature to fabricate PCCs. This might be the real reason for the high performance of the devices using Y and Yb co-substituted electrolytes, prepared by the co-sintering method.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
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IF 4.3
Xue Ye,Chenxi Bai,Peipei Zhang,Fuyuan Han,Junyu Xia,Xinhua Gao,Wenlin Xu,Lisheng Guo,Jie Li
Metallic atoms within metal–organic framework (MOF) materials exhibit a distinctive and adaptable coordination structure. The three-dimensional (3D) pore configuration of MOFs enables the complete exposure of metal active sites, rendering them prevalent in various catalytic reactions. In this study, zinc (Zn) atoms within Zn-based MOF materials, characterized by an abundance of valence electrons, are utilized for the transesterification of dimethyl carbonate (DMC). Additionally, the introduction of zirconium (Zr) effectively addresses the susceptibility of the MOFs’ crystal structure to dissolution in organic solvents. The formulated catalyst, Zn-10%Zr-MOF(300), demonstrates remarkable catalytic performance with 91.5% DMC selectivity, 61.9% propylene carbonate (PC) conversion, and 56.6% DMC yield. Impressively, the catalyst maintains its high performance over five cycles. Results indicate that Zr interacts with Zn, forming new coordination bonds and enhancing the catalyst crystal structure stability. Moreover, electron transfer intensifies the alkalinity of the active Zn atoms, enhancing the overall catalyst performance. This research informs the development of transesterification heterogeneous catalysts and broadens the application scope of MOF catalysts.
研究领域:
材料科学
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催化
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化学工程
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产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Zarfashan Shahid,Bairong Fu,Saima Rehman,Zia Ahmad,Jiping Chen,Xianbo Lu
Bisphenol compounds, including BPA and BPS, are significant pollutants found in the environment, food, and daily necessities. They pose various adverse effects, including estrogenic, immunotoxic, metabolic, and reproductive toxicity, which severely threaten human health and ecological safety. Achieving simultaneous rapid detection of BPA and BPS is still very challenging due to their similar structures and co-existence in actual samples at ultratrace level. This study addresses the problem of developing an effective method for the rapid detection of BPA and BPS simultaneously. A new electrochemical nanosensor based on ionic liquid (IL) coupled Zr-MOF@GO was developed for ultrasensitive real-time detection of BPA and BPS. The Zr-MOF@GO/IL nanocomposite features a custom-built structure with an ordered framework, abundant pores, and highly coupled interfaces. The experimental findings demonstrate that the introduction of IL enhances the conductivity and dispersibility of the nanocomposite, improves the absorption capability for target bisphenols, and significantly improves the detection limit and linear range of the Zr-MOF@GO based electrochemical sensor. The sensor demonstrated wide linear ranges with detection limits of 5.5 nmol/L for BPA and 7.1 nmol/L for BPS (S/N = 3), respectively. Comparative studies revealed that the detection limits of the Zr-MOF@GO/IL-based sensor improved by an order of magnitude compared to the Zr-MOF@GO-based sensor. Additionally, the sensor exhibited superior analytical performance regarding reproducibility, stability, and selectivity. This study investigated the capability and synergy of IL coupled high-valent stable transition metal Zr IV -based MOFs in electrochemical sensing for the first time. This development sets a new benchmark in non-enzymatic electrochemical sensing, establishing the Zr-MOF@GO/IL-based sensor as a promising platform for the individual or simultaneous rapid detection of bisphenols in actual samples.
研究领域:
环境科学
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分析化学
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材料科学
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纳米技术
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Liam John France,Wan Li,Yanke Zhang,Wentao Mu,Zhihang Chen,Junjun Shi,Qiang Zeng,Xuehui Li
A series of Fe-Zr mixed-metal oxides were prepared and examined for the simultaneous reduction of NO and SO 2 with CO. The catalyst containing 40 mol% exhibited near-complete conversion of both pollutants at a minimum temperature of 350 °C and a GHSV of 90,000 h −1 . The addition of Fe 3+ to ZrO 2 decreased the crystallinity of the latter phase and significantly enhanced surface area. Concentrations of 30 mol% or greater produced segregated FeO x phases, which affected catalytic performance in distinctly different ways: supported Fe 3+ (30 mol%) possessed similar activity to doped Fe 3+ ; α-Fe 2 O 3 (50 mol%) inhibited activity due to its’ lower reducibility; an amorphous phase (40 mol%) promoted iron-weighted areal activity. A complete identification of the ambiguous component was not successfully established, but the obtained properties revealed that it exhibited weaker interaction with the support and had a size greater than that of oligomeric-Fe 2 O 3 yet smaller than 3 nm.
研究领域:
催化
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环境科学
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化学工程
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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Jiale Han,Fang Li,Mengyuan Zhao,Meimei Guo,Yunhang Liu,Xiangxing Guo,Qiwen Ran,Zhankui Wang,Hongyuan Zhao
In this work, a novel electrochemical sensor was designed based on Zr-based metal–organic framework (UIO-66) nanoparticles embellished single-wall carbon nanotube networks (SCN) for the detection of methyl parathion (MP). The synergistic combination of SCN and UIO-66 nanoparticles could fully exert each advantage to boost the MP electrochemical sensing analysis performance. SCN with one-dimensional hollow nanostructures formed three-dimensional interconnected carbon conductive networks, which possessed excellent conductive properties and acceptable specific surface area, enabling efficient transport of electrons and ions. UIO-66 nanoparticles with Zr-OH groups contributes and porous structure to the good affinity for phosphate groups on MP molecules, which enhanced the selective recognition and enrichment capability of sensing electrode towards MP. Under the multifunctional integration of SCN and UIO-66 nanoparticles, the SCN@UIO-66/GCE sensor could present satisfactory MP electrochemical detection performance (LOD: 8.05 nM, linear MP concentration range: 0.01–10 μM). The satisfactory practical property was realized at the SCN@UIO-66/GCE sensor with satisfactory recovery rates of 98.28–101.95 % and low RSD of 1.23–3.01 % for the electrochemical detection of MP in orange juice and lettuce samples.
研究领域:
分析化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Xiao Yang,Zhuwei Yang,Linsen Li,Zhao Jiang,Guangxu Cheng
Dry methane reforming (DRM) represents a highly promising approach to greenhouse gas conversion (CO 2 and CH 4 ) to valuable byproducts. However, severe carbon deposition and catalyst deactivation inhibit large-scale applications. The work designed new catalysts with a yolk-shell structure using the water-in-oil microemulsion method. The catalysts were composed of a yolk-shell structure, with Ni-M as the active point and silica as the shell. The catalytic performance evaluation indicates that the Ni-M @SiO 2 catalysts show higher CH 4 and CO 2 conversion compared with the Ni@SiO 2 and conventional catalysts at 750 ℃, suggesting the yolk-shell structure and added M species enhance the DRM activity. The XRD, HRTEM, XPS, BET, H 2 -TPR, and CO 2 -TPD analysis confirmed the existence of yolk-shell configuration and evident electronic effect among Ni, M species, and SiO 2 . The long term measurements indicate that the added M species also bring higher carbon deposition tolerance for DRM, where Ni-Ce@SiO 2 and Ni-Zr@SiO 2 exhibit good structural and catalytic stability for DRM over 100 h. Through XRD, TEM, and TGA characterizations of the exhausted catalysts, it is determined that the coke deposition resistance of the catalyst is improved as a result of increased oxygen mobility and enhanced Ni dispersion on the catalytic surface, both of which are enhanced by the added Ce species. The structural analysis of the spent catalysts indicates that the tolerance of carbon deposition is improved by the yolk-shell samples. This study can offer valuable insights for the development of Ni-based catalysts with exceptional carbon deposition capability for DRM.
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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DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·894-905
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IF 6.119
Jihui Yao,Yuzi Rong,Zeyan Gao,Xiaohua Tang,Fei Zha,Haifeng Tian,Yue Chang,Xiaojun Guo
To introduce a hierarchical porous structure into SAPO-34 zeolites and adjust their acid properties and crystalline size, a series of Zr-modified SAPO-34 zeolites (Zrx-SAPO-34 (x = 0.25, 0.50 and 0.75)) with hierarchical porous structure were synthesized by hydrothermal crystallization using palygorskite as a silicon and partial aluminum source, morpholine and tetraethylammonium hydroxide as organic structure directing agents and UiO-66 as a co-template agent. The obtained catalysts were characterized via XRD, SEM, TEM, EDX, N2-adsorption–desorption, NH3-TPD, FTIR, Py-IR, XRF, 29Si MAS NMR and TG analyses. The catalytic performance of Zrx-SAPO-34 in the methanol-to-olefin (MTO) transformation was investigated in a fixed bed reactor. The introduction of a hierarchical porous structure effectively enhanced the diffusion and mass transfer of the reactants/products, prolonging the catalytic lifetime. Additionally, the optimization of the acidity dramatically improved the selectivity for light olefins. Under the reaction conditions wherein the reaction temperature was 400 °C, the feed of WHSV was 2.0 h−1, the mass of the catalyst was 0.5 g and at atmospheric pressure, the Zr0.50-SAPO-34 zeolites exhibited optimum catalytic performance, where the methanol conversion was 100%, the light olefin selectivity was 98.66% and the catalytic lifetime was more than 1500 min.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 41
·19432-19438
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IF 3.591
Fangyuan He,Heyi Zhang,Xiaonan Li,Jie Yang,Wenqing Ma,Hong Zhang
In this study, for the first time, we selected a size-matched polyoxometalate α-Mo8O26, and successfully prepared Mo8-UiO-66(Zr) as a catalyst with double active sites for extractive and catalytic oxidative desulfurization systems (ECODS). UiO-66(Zr) can encapsulate Mo8O26 in the cage and avoid its leaching, while the sulfur compounds can also enter the cage to approach the sites. As a result, in the presence of H2O2 as an oxidant, the catalyst exhibited extraordinary oxidative desulfurization performance towards benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT). It only takes 10 min for the desulfurization efficiency to reach 100%. The catalyst can be reused for at least 4 times without significant loss in the desulfurization activity. Also, the possible reaction mechanisms of the catalytic oxidation process have also been proposed.
研究领域:
化学
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催化科学
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能源与燃料
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产品关联
DOI
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
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2025
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IF 6.6
Jianmei Li,Yuting Yin,Haiyu Li,Zongyao Zhao,Mengqin Xiang,Yong Tang,Qi Sun
The escalating economic and ethical concerns associated with camel meat adulteration using cheaper horsemeat necessitate the development of rapid, on-site detection technologies that overcome the limitations of conventional laboratory-based methods. In this study, a portable electrochemical DNA biosensor was fabricated by integrating a polydopamine (PDA)-modified screen-printed carbon electrode (SPCE) with a nucleic acid-functionalized UIO-66(Zr) metal-organic framework (MOF). The PDA coating facilitated stable, covalent immobilization of DNA capture probes through Schiff base reactions, while the UIO-66(Zr) MOF functioned as a high-capacity signal amplifier owing to its large surface area and intrinsic redox activity. This synergistic architecture enabled ultrasensitive detection, achieving a limit of 3.57 pmol/L for horsemeat DNA and 0.5 g/kg adulteration in camel meat blends—significantly surpassing the performance of existing detection methods. The biosensor exhibited excellent specificity by distinguishing single-base mismatches, along with high reproducibility (RSD = 4.12%), operational stability over 15 days, and accurate recovery rates ranging from 91.7% to 112.4% in spiked samples. Its disposable electrode format, cost-effectiveness, and compatibility with portable potentiostats underscore its strong potential for on-site meat authentication. Overall, this work provides a practical and scalable solution to combat meat fraud in resource-limited settings and establishes a versatile MOF-electrode nanoassembly platform for advanced food safety monitoring.
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Huanjing Chen,Wanqiao Bai,Hongmei Chai,Loujun Gao
To achieve the rapid and sensitive detection of trace methyl parathion (MP) in river water and edible agricultural products, the catalytic composite material zirconium hydroxide (Zr(OH)4)/zeolite imidazolate framework-90 (ZIF-90) was prepared by a one-step synthesis method. The composite was further incorporated with a conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hydrogel to prepare a modified electrode. Then, an electrochemical sensing method based on the PEDOT:PSS/Zr(OH)4/ZIF-90 composite was successfully established for the analysis and detection of MP. The component ratio of the composite material, modification amount and pH value of the detection substrate were optimized. The electrochemical properties of the composite modified electrode were evaluated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV) techniques, and the results confirmed that it had good electrochemical properties. The electrochemical response of the established sensing method to MP showed a good linear relationship in the concentration range of 1–250 µmol L−1, and its detection limit and sensitivity reached 0.74 µmol L−1 and 0.09 µA µmol−1 L−1, respectively. The interference of common coexisting ions on the detection performance of the PEDOT:PSS/Zr(OH)4/ZIF-90 modified electrode was further investigated, and it was applied for the quantitative analysis of MP in actual river water and apple samples. The electrochemical sensing method developed in this work provides a new way for the efficient detection of MP residues in environmental water and agricultural products.
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DOI
高影响因子
Journal of Natural Gas Chemistry
·
2012
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IF 1.348
Lincai Peng,Junping Zhuang,Lu Lin
Effects of Zr/Ti molar ratio in SO 2− 4 /ZrO 2 -TiO 2 solid acid catalyst calcined at different temperatures on its surface properties and catalytic activity were thoroughly investigated in this paper. The physicochemical characteristics of prepared samples were determined by N2 adsorptiondesorption, XRD, NH3-TPD and XPS techniques, respectively. It was found that the crystallization temperature of the samples increased after the combination of ZrO 2 and TiO 2 ; and phase transformations from the anatase to the rutile of TiO 2 species and the tetragonal to the monoclinic of ZrO 2 species were effectively suppressed at higher temperature. The sample with a Zr/Ti molar ratio of 3/1 calcined at 450 °C showed the highest surface area and the most acid sites among all the tested samples. The acid site densities of samples were relatively closed to each other if they were calcined at the same temperature, however, decreased with the calcination temperature. The result indicates that the sulfur content in samples is a crucial factor to control the acid site density. Calcining the sample at 650 °C and higher temperatures resulted in a significant desorption of sulfate ion on the samples. The synthesized samples were evaluated as a potential catalyst for glucose conversion under the near-critical methanol conditions (200 °C/4 MPa). The results suggested that the relatively weaker acid sites of the catalyst were more favorable for the accumulation of methyl glucosides, while the moderate acid sites were responsible for the formation of methyl levulinate. The catalytic activity for methyl levulinate production almost increases linearly with the catalyst acid site density. The catalyst deactivation is due to the loss of sulfate ion and the two catalysts with Zr/Ti molar ratios of 3/1 and 1/3 could effectively alleviate the deactivation caused by sulfate solution in the reaction medium and can be reused after calcination with the reuse rate of over 90% in terms of the methyl levulinate selectivity.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2025
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IF 5.2
Fangfang Yang,Xueyan Wang,Jialu Li,Zhanfeng Li,Zonghua Wang
In recent years, the ultrasonic removal of organic pollutants has attracted a great deal of attention. In this study, a novel MOF-based sonocatalyst with bimetallic center was formed by doping Zr atoms into the MX@MIL-125(Ti), aiming to improve the ultrasonic removal performance of organic pollutants. The successfully prepared MX@MIL-125(Ti/Zr) showed a porous structure with abundant grooves and channels (average pore size of 21.8 nm, and specific surface area of 36.910 m 2 /g), and significantly had a higher quantum yield (13.24 %) than MIL-125(Ti) and MX@MIL-125(Ti), thereby producing more OH and O 2 − free radicals under ultrasonic irradiation. The experimental results showed that the MX@MIL-125(Ti/Zr) had good sonocatalytic activity and could effectively deal with small-molecule dyes and macro-molecule microplastics under ultrasonic conditions, where the removal efficiency achieved approximately 95 % for Rhodamine B (within 12 min) and approximately 90 % for micro-polyethylene (within 4 h in the presence of persulfate). In addition, a possible degradation-dominant mechanism was proposed to explain the MX@MIL-125(Ti/Zr)-mediated sonocatalytic removal, where the existence of Zr atoms could help sono-excited electrons generate and transfer onto the conductive MXene, thereby facilitating more charge carriers to create reactive free radicals. Therefore, the study would provide a green and feasible approach for the industrial treatment of organic pollutants in water bodies.
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）