APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jinjing Qiu,Qi Chen,Cheng Liu,Yueling Chen,Jionghua Wu,Kaiqiang Jing,Jimmy C. Yu,Ling Wu,Xianzhi Fu
Defect engineering and single atom incorporation can provide more active sites to modulate the surface electronic structure of a catalyst and to activate reactant molecules. Herein, a series of Ru-anchored DUT-67(Zr) MOFs with explicit defect sites have been prepared for photocatalytic nitrogen reduction. It is characterized that Ru/DUT-67(Zr) possesses uniformly dispersed Ru single atoms and unsaturated Zr. Typically, 1.0 %Ru/DUT-67(Zr) shows best performance with a NH 4 + yield of 61.1 μmol·g −1 ·h −1 , which is approximately 6-folds higher than that of defective DUT-67(Zr) without Ru single atom (DUT-L), while pristine DUT-67(Zr) exhibits a lack of the photocatalytic N 2 reduction activity. The observed enhancement can be attributed to the introduction of Ru and unsaturated Zr sites induced by irradiation. Both of them can work together act as active centers to absorb and activate dinitrogen molecule. Furthermore, benefited from the electronic channel (Ru-S) between Ru and DUT-67(Zr), the separation of photogenerated carriers has been greatly improved, contributing to the collaborative conversion of activated N 2 to NH 3 . This study provides a new insight for designing a dual active sites photocatalyst with unsaturated coordinated sites and the single atoms by the coordinately interaction of functionalized linker.
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
COMPOSITES PART B-ENGINEERING
·
2023
·
IF 13.1
Yang Lyu,Yuan Cheng,Guangdong Zhao,Mengyu Wang,Guiqing Chen,Xinghong Zhang,Wenbo Han
The SiBCN(Zr) ceramics were synthesized via a polymer-derived ceramics route. Using this precursor, the precursor impregnation pyrolysis process prepared the C f /SiBCNZr composites with low density (1.89 g/cm 3 ). Compared to C f /SiBCN, the C f /SiBCNZr composites exhibit reliable thermal stability and ablation resistance in a wide temperature range. A dense oxide layer dominated by ZrO 2 and SiO 2 formed in situ on the surface of C f/ SiBCNZr, effectively preventing outside oxygen and further ablation. The introduced Zr is evenly distributed in SiBCN ceramics, which enables it to give full play to the ablation resistance of Zr at higher oxygen acetylene torch temperatures. This work enriches the fundamental understanding and offers engineering guidance for lightweight ultra-high temperature ceramic matrix composites .
研究领域:
材料科学
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航空航天工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Yuanming Zhou,Shuxin Li,Shuangxing Zhu,Ruizhi Liu,Zhenxiao Tang,Maozhong Yi,Ke Peng
To investigate the influence of (Ta,Zr)C on the ablation resistance of C/C composites, C/C-(Ta 0.5 Zr 0.5 )C-SiC, C/C-(Ta 0.33 Zr 0.67 )C-SiC, and C/C-(Ta 0.2 Zr 0.8 )C-SiC were prepared with different Zr/Ta ratios through high-solid-loading slurry impregnation combined with precursor infiltration and pyrolysis. The flexural performance and ablation resistance both improved with an increasing Zr/Ta ratio. Compared to C/C-(Ta 0.5 Zr 0.5 )C-SiC and C/C-(Ta 0.33 Zr 0.67 )C-SiC, the flexural strength of C/C-(Ta 0.2 Zr 0.8 )C-SiC increased by 74.17 % and 24.29 %, respectively. The mass ablation rate was reduced by 74.33 % and 81.02 %, while the linear ablation rate was reduced by 98.60 % and 97.65 % after 120 s of ablation, respectively. The variations in Zr/Ta ratios affected the formation, integrity, and performance of the microstructure, which was composed of a Zr-rich oxide skeleton combined with Ta-rich oxide binder within the Ta-Zr-O oxide layer on the composite surface, ultimately enhancing the overall ablation resistance of these composites.
研究领域:
材料科学
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航空航天工程
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1845-1855
·
IF 2.372
Wang Tao,Hu Aiyun,Xu Guangzhi,Liu Chen,Wang Haijun,Xia Yongmei
Furfural (FAL) is one of the most important biomass-derived platform compounds. The catalytic transformation of FAL was investigated with three porous Zr–thiophenedicarboxylate hybrids for the production of furfuryl alcohol (FOL). Three Zr-based catalysts, including DUT-67(Zr), DUT-68(Zr) and DUT-69(Zr) were synthesized through a facile assembly of 2,5-thiophenedicarboxylate acid with ZrCl 4 using the acetic acid as a modulator under hydrothermal conditions. These catalysts were also characterized using FT-IR, XRD, SEM, TEM, N 2 adsorption–desorption, XPS and TG. The specific surface area of the DUT-69(Zr) is smaller than that of the DUT-68(Zr) and slightly larger than that of the DUT-67(Zr), but it has a relatively large pore volume and pore diameter. Although all three catalysts showed excellent catalytic activity towards the catalytic transfer hydrogenation of FAL into FOL, the DUT-69(Zr) material has slightly higher catalytic activity than the other two catalysts. Besides, considering the cost of catalyst preparation, the DUT-69(Zr) material was used as the optimal catalyst and studied in detail. A high FOL yield of 92.2% at 95.9% FAL conversion was achieved at 120 °C for 4 h over DUT-69(Zr). Meanwhile, the DUT-69(Zr) could be reused more than six times with a minor decrease in catalytic activity. Finally, a plausible mechanism for catalytic transfer hydrogenation of carbonyl compounds to produce corresponding alcohols was presented based on the results of the experiments and previous reports. Graphical Abstract
研究领域:
化学
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材料科学
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催化反应
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DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2021
·Vol. 40
·期 8
·918-924
·
IF 6
Jisheng Xu,Chengxiang Shi,Shuguang Zhang,Qiancheng Zheng,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Comprehensive Summary Non-oxidative ethane dehydrogenation is a promising route to produce ethene. Herein, PtSn supported catalysts were investigated to achieve better ethane dehydrogenation performance by introduction of different Zr promoters, i.e. , framework Zr and ZrO 2 , to mesoporous MCM-41. In-situ XRD, TEM and CO chemisorption show that aggregation of metal particles and phase segregation of Pt 3 Sn to Pt and PtSn 3 at high temperature occur for PtSn/M, leading to bad ethane dehydrogenation activity. Strong interaction between ZrO 2 and PtSn species, as proved by XPS, results in restrained metal particles, which promotes the initial reactivity. However, Pt phase generated on surface is disadvantageous for the desorption of produced ethene as indicated by CO-IR and C 3 H 6 -TPD, and pyridine-IR and NH 3 -TPD indicate strong acidity generated. Both deactivate the catalyst rapidly by deep dehydrogenation and coking. Moderate interaction between PtSn species and Si-O-Zr with much weaker acidity is formed when framework Zr is incorporated into MCM-41, which benefits the dispersion of metal particles, formation of Pt 3 Sn/Pt species and stabilization of metal species from phase segregation. Outstanding initial ethane conversion and ethene selectivity of ca. 99% were achieved for the optimal PtSn/ZrM, which is more coking-tolerant and stable by generating graphitic carbon mainly on support instead of active metals.
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
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Liyu Chen,Jiaxin Yang,Yifan Zhang,Shaohua Wu,Youjian Yang,Wenju Tao,Jiangyu Yu,Zhaowen Wang
The electrochemical behavior of Zr(IV) on a molybdenum (Mo) electrode in a KF-AlF 3 -Al 2 O 3 -ZrO 2 molten salt system was studied using cyclic voltammetry (CV), square-wave voltammetry (SWV) and chronopotentiometry (CP). The reduction process of Zr(IV) was found to follow a two-step, two-electron transfer mechanism: Zr(IV)+2e − →Zr(II) and Zr(II)+2e − →Zr(0). The reduction process was quasi-reversible and controlled by diffusion. Al-Zr alloys were successfully obtained on Mo and liquid aluminum electrodes by potentiostatic electrodeposition . Flower-like AlZr 3 and irregular granular Al 3 Zr were obtained on the Mo electrode, which were mainly attributed to the electrochemical co-reduction of Al(III) and Zr(IV) in the molten salt. Three Al-Zr alloy phases, Al 3 Zr , Al 3 Zr 2, and Al 2 Zr, were obtained on the liquid aluminum electrode, among which Al 3 Zr was dominant in the product, followed by Al 3 Zr 2 .
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Wei Sun,Shijie Shao,Jun Pan,Yangyang Wang,Hangqi Xia,Xiaohui Gao,Hao Zhang,Qiguang Dai,Li Wang,Xingyi Wang
Ce-Ti-Zr mixed oxide catalysts prepared by sol-gel method were used in catalytic combustion of CH 2 Cl 2 . The characterization reveals that the incorporation of Ce and Zr into TiO 2 anatase or Ti and Zr into CeO 2 fluorite promotes hydroxyl groups, Lewis acidity and surface oxygen through the formation of Ti-O-Zr, Ti-O-Ce and Ce-O-Zr species. Ce-Ti-Zr catalysts show high activity for CH 2 Cl 2 oxidation with the rate of 5.66 × 10 −3 –6.45 × 10 −3 μmol s −1 m −2 at 250 °C and high stability for 50 h. The substitution of surface oxygen for Cl maintains the availability of Ti-OH and thus promotes Cl removal as HCl, which is verified by a great increase in the stable activity of physically closely contacted mixture of separated CeO 2 and TiO 2 or Ti 9 Zr 1 particles. In situ FT-IR shows that CH 2 Cl 2 interacts with Ti-OH to form -O-CH 2 -O-, which is quickly rearranged into formate. Finally, formate is oxidized with surface oxygen into CO or CO 2 .
研究领域:
催化
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yanghuan Huang,Haocheng Zhang,Lou Gao,Tianlan Yan,Yueer Yan,Yahong Zhang,Yi Tang
A series of Zr–Al-MWW zeolites with different Zr state and layer-stacking structure are successfully synthesized via direct grafting zirconocene dichloride onto the external silanols of three kinds of MWW zeolites, i.e. MCM-22 with multilayered structure, ITQ-2 (through layer delaminated route) and OL-MWW (by direct hydrothermal synthesis) with oligolayered structure. The structure, porosity and state of grafted Zr species are distinctly different among the three Zr–Al-MWW zeolites. Zr-OL-MWW possesses the highest content of single Zr atoms with an ideal micro-meso-macro pore system, while Zr-MCM-22 and Zr-ITQ-2 contain two kinds of Zr species (ZrO 2 clusters and single Zr atoms) coexisting in various proportions. The high dispersion of single Zr atoms on OL-MWW can be assigned to the large amount of external silanols of OL-MWW. The as-prepared three bi-functional Zr–Al-MWW zeolites are used for the cascade Meerwein-Ponndorf-Verley (MPV) reduction and etherification (ETH) reaction. Among them, Zr-OL-MWW shows dramatically higher conversion of cinnamaldehyde and yield of 1-cinnamyl 2-propyl ether than Zr-MCM-22 and Zr-ITQ-2, owing to the higher catalytic activity of Lewis acid centers from single Zr atoms, as well as more integrated framework Al sites as Brønsted acid centers with good accessibility. This study offers a simple and efficient strategy to construct Lewis-Brønsted acidic zeolites with exposed heteroatom sites and integrated framework structure, which will provide especial potential in the catalytic conversion of macromolecules.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Fan Xiao,Xiaoyu Hu,Yingbo Chen,Yufeng Zhang
Four different thin-film nanocomposite (TFN) membranes were prepared by adding different concentrations of porous Zr-metal-organic frameworks (MOFs) (UiO-66 and UiO-66-NH2) to piperazine aqueous solution (aqueous phase) or 1,3,5-benzenetricarbonyl trichloride-n-hexane solution (organic phase) by interfacial polymerization. The main purpose is to study the specific effects of different addition methods and addition amounts of nanoparticles on the structure and performance of the TFN membranes by interfacial polymerization. All four TFN membranes exhibited a higher water permeability while maintaining high salt rejection compared to thin-film composite membrane. On the one hand, the TFN membranes behave differently, which are prepared by adding the same kind of nanoparticles to the aqueous phase or organic phase, respectively. The TFN membrane prepared by adding 0.2 w/v% UiO-66 to the organic phase had a high water flux of 87.86 L m–2 h–1, compared to 46.31 L m–2 h–1 of the membrane prepared by adding 0.3 w/v% UiO-66 in the aqueous phase. This is due to the fact that UiO-66 greatly slows the interfacial polymerization rate when UiO-66 is added to the organic phase, resulting in a thinner and wider-aperture polyamide thin-film layer, reducing the water transmission resistance during filtration. Therefore, it is more economical by adding nanoparticles to organic phase than aqueous phase under the same filtering effect. On the other hand, different nanoparticles can also cause differences in performance and structure of the TFN membranes even in the same preparation manner. TFN membrane with UiO-66-NH2 in the aqueous phase has higher water permeance than the one with UiO-66 in the aqueous phase, owing to the good hydrophilicity of the amino group, which improves the water dispersibility of UiO-66-NH2 so that the TFN membrane is more uniform. In addition, UiO-66-NH2 slows down the process of interface polymerization, making the membrane more porous. The monomers in the aqueous phase and organic phase can be adsorbed in the pores of Zr-MOFs, which makes the interfacial polymerization occur both in the pores and on the surface of the pores. Thus, the compatibility between the polyamide and MOFs was enhanced and less defects were formed in the thin-film layer, resulting in a high salt rejection even when the concentration of Zr-MOFs increased. This is the first time to explain that polyamide membrane has not obvious salt rejection attenuation with increasing porous material content using pore adsorption reaction monomer principle. Also, the Zr-MOFs-based TFN membrane exhibited good heat resistance and antifouling property. This work shows that porous Zr-MOFs nanomaterials have significant advantages in the development of nanofiltration membranes with high water flux and rejection.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Lei Chen,Huan Wang,Xiaohong Cao,Yue Feng,Zhibing Zhang,Youqun Wang,Yunhai Liu
A simple hydrothermal method was adopted to synthesize different inorganic-organic hybrid materials (Zr -x ), including zirconium ethylenediamine tetramethylene phosphine (Zr-EDTMP), 2-phosphobutane-1,2,4-zirconium tricarboxylate (Zr-PBTC), odium creatine phosphate zirconium phosphate (Zr-CP), and creatinol zirconium phosphate (Zr–COP). Various characterizations were utilized to explore the physical and chemical properties of materials. The applications of Zr -x in removing U(Ⅵ) were studied comprehensively. The effects of solution's pH value, contact time, initial concentration of U(Ⅵ), and temperature on adsorption were examined. Besides, the desorption, reusability, as well as adsorptive selectivity were investigated. The present study revealed that the U(Ⅵ) adsorption on Zr-EDTMP was in accordance with Sips isothermal model with the greatest adsorption capacity (317.4 mg/g) and the superior adsorptive selectivity for U(Ⅵ). Zr-EDTMP is a potentially high-efficient adsorbent for extracting U(Ⅵ) from radioactive wastewater .
研究领域:
环境科学
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材料科学
·
核化学
✓ 已验证
产品关联
DOI
高影响因子
RADIOCHIMICA ACTA
·
2021
·Vol. 109
·期 10
·759-771
·
IF 1.44
You-qun Wang,Huan Wang,Yue Feng,Zhi-bin Zhang,Xiao-hong Cao,Yun-hai Liu
In this work, diethylenetriamine pentamethylenephosphonic acid (DTPMP) was ultilized into preparing of Zr(IV) organophosphates hybrids (Zr-DTPMP- x , x was the molar ratio of Zr(IV)/DTPMP in the synthetic process, x = 0.5, 1, 2, and 3) using a hydrothermal method. The physical and chemical properties of Zr-DTPMP- x were characterized by SEM&EDS, FT-IR, XRD, Zeta potential, XPS, TGA and contact angle analysis. Moreover, the adsorptive performances of Zr-DTPMP- x for U(VI) were investigated. The adsorption results showed that the optimum molar ratio of Zr(IV) to phosphine, pH, equilibrium time, and dosage was 0.5, 4.0, 180 min, and 10 mg, respectively. Besides, the adsorption of U(VI) was in accordance with the pseudo-second-order kinetic model and Sips isothermal model. Moreover, the adsorption capacity determined by Sips isothermal model was 181.34 mg g −1 for Zr-DTPMP-0.5. Furthermore, the adsorptive selectivity of Zr-DTPMP-0.5 for U(VI) was superior than the others. Zr-DTPMP-0.5 may be a powerful candidate for diminishing the contamination of U(VI).
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Xiong-Fei Zhang,Zhongguo Wang,Yi Feng,Yuxia Zhong,Jiaqiang Liao,Yaquan Wang,Jianfeng Yao
Metal organic frameworks (MOFs) have recently emerged as promising candidates for efficient removal of sulfur-containing compounds (SCCs) from liquid fuels. In this study, adsorptive desulfurization (ADS) is performed by adsorbing thiophene (TP) and benzothiophene (BT) from model fuels over pristine and functionalized UiO-66 (Zr). The introduction of amino ( NH 2 ) and carboxylic ( COOH) groups reduces the porosity of UiO-66. However, the adsorption capacities of functionalized UiO-66 improved remarkably. Especially for the adsorbent functionalized with amino moieties (UiO-66-NH 2 ), its maximum adsorption capacities for TP (29.5 mg S/g) and BT (35.7 mg S/g) are 1.7 and 1.8 times to that of bare UiO-66. The superior performance of UiO-66-NH 2 is ascribed to the higher availability of hydrogen-bond donor sites in the surface and the favorable interactions between H atoms of NH 2 and sulfur species. UiO-66-COOH is beneficial for the adsorption of SCCs than that of pristine UiO-66 because of the existence of acid-base interactions. Moreover, the reusability of UiO-66-NH 2 is confirmed by regenerating it via a simple solvent washing.
研究领域:
化学工程
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材料科学
✓ 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）