JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·Vol. 45
·期 15
·117640
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IF 6.2
Li Xu,Wei Liao,Xiaosong Zhou,Yongqiang Tan
The influences of Cr 3 C 2 addition on phase formation, microstructures and mechanical properties of (Zr,Ti,Nb,Ta,Hf)C prepared from binary carbides mixtures by spark plasma sintering were studied. The introduction of 4/3 mol.% Cr 3 C 2 significantly lowered the minimum temperature for uniform high-entropy phase (Zr,Ti,Nb,Ta,Hf)C from 2200 °C for to 1900 °C. The lower solubility limit of Cr in (Zr,Ti,Nb,Ta,Hf,Cr)C results in excessive Cr 3 C 2 -based carbides, which tends to segregate along grain boundaries at higher sintering temperatures while locate at triple junctions at lower sintering temperatures . High mechanical strength of 599 MPa were obtained when 4/3 mol.% Cr 2 C 3 was added and sintered at 1900 °C. The fine grain size and Cr 3 C 2 -based carbides are responsible for the high mechanical properties. More Cr 2 C 3 addition results in lower mechanical properties due to excessive Cr 3 C 2 -based carbides.
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高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Yongli Chang,Weiling Liu,Yang Chen,Yong Zhang,Ruoyu Li,Xiaoyang Xu,Yu Tang,Lizhi Wu,Huibo Zhao,Li Tan
Tuning metal-support interactions in catalysts represents a promising strategy for optimizing the catalytic activity of CO 2 hydrogenation. Here, CuZnZr ternary catalysts with varied interfacial structures were fabricated by altering the metal loading sequence to elucidate the interactions between different counterparts. Compared to reference catalysts with different interfaces (Cu-ZnZr, Zn-CuZr and Zr-CuZn), CuZnZr synthesized via the coprecipitation method (CZZ) displays the highest catalytic performance, achieving a CO 2 conversion rate of 13.3 %, methanol selectivity of 71.3 %, and a STY of 12.2 mmol MeOH ·g cat -1 ·h -1 under optimal conditions. Extensive characterization results indicate that this exceptional activity originates from the synergistic optimization of both structure and reaction mechanism, driven by the interface confinement effect (ICE) enabled by abundant interfacial sites. Specifically, the surface of CZZ shows high density of highly dispersed Cu 0 nanoparticles and rich oxygen vacancy sites, which is beneficial to the activation of H 2 and the adsorption of CO 2 . In-situ DRIFTS further revealed that, compared to reference catalysts, CO 2 hydrogenation on CZZ follows both the HCOO* and COOH* pathways, leading to a substantial improvement in overall catalytic activity. In summary, this study provides a deeper understanding of the ICE and their impacts on catalytic performance, offering a valuable theoretical insight for the design of high-performance catalysts in future research.
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Wenwen Lin,Siyu Yao,Hao Chen,Shenglai Li,Yang Xia,Yuan Yao,Jing Li,Dangguo Cheng,Jie Fu
Electrochemical nitrogen reduction reaction (NRR) to produce ammonia under ambient conditions is considered as a promising approach to tackle the energy-intensive Haber-Bosch process, but the low Faradaic efficiency and yield of NH 3 are still a challenge. Herein, a carbon-vacancies enriched mesoporous g-C 3 N 4 is developed by an in situ Zr doping strategy. The in situ mesoporous-forming mechanism is deeply understood by TPSR to reveal the functions of Zr dopant that pulls C from the precursor of C 3 N 4 , resulting the formation of homogeneous mesopores with about 57% of the one C-defective s-triazine ring in C 3 N 4 . Due to the defect sites obtained in metal doping synthesis, the RuAu bimetallic supported catalyst (RuAu 3 /0.3Zr-C 3 N 4 ) exhibits effective NRR performance with a Faraday efficiency of 11.54% and an NH 3 yield of 5.28 μg h −1 mg −1 cat. at −0.1 V (RHE), which is nearly 10 times higher than that of RuAu 3 /C 3 N 4 catalyst. This work proposes a simple and template–free preparation method for the high defect density mesoporous C 3 N 4 , and provides new possibilities of a wide application of mesopore g-C 3 N 4 .
研究领域:
材料科学
·
电催化
·
环境科学
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Caiyun Han,Jing Xie,Xize Min
Due to the non-degradable of heavy metal, adsorption has been extensively applied to abatement it. Most studies were focused on uptake metal ions via electrostatic attraction and ion exchange, and load molecule H 3 AsO 4 from strongly acidic wastewater was still challenging. To solve the problem, bimetallic La–Zr MOFs was facilely fabricated in this work, and the fcu topology structure of La-Zr MOFs was remained well under the investigate crystallization time and crystallization temperature. However, the crystallinity of the obtained La-Zr MOFs was influenced by the synthesized factors. The obtained La–Zr MOFs was employed as adsorbent to removal Cr(VI) and As(V), and the performance was evaluated by the batch experiment. The result indicated that the adsorption performance of Cr(VI) and As(V) was positively correlated with the crystallinity , and the optimal sample was 1LaUN 12 . From the XPS characterization, it was found that H 3 AsO 4 was successfully uptake over 1LaUN 12 surface, and the maximum monolayer adsorption capacity was 83.40 mgH 3 AsO 4 /g via ligand exchange and coordination reactions with La−OH and Zr−OH. In addition, the sample 1LaUN 12 also exhibited the excellent Cr(VI) load performance, and the maximum monolayer adsorption capacity of Cr(VI) was 222.5 mg/g. Above 40% Cr(VI) was reduced to Cr(III) by amino groups, and immobilized over the surface of 1LaUN 12 . Eventually, 1LaUN 12 displayed a good structural stability in the acidic medium, which was in favor of removing Cr(VI) and As(V) efficiently from strongly acidic solutions.
研究领域:
环境科学
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材料科学
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CERAMICS INTERNATIONAL
·
2026
·
IF 6
Siqi Guo,Wei Feng,Qingyuan Wang,Ruichong Chen
Advanced tritium breeder materials with high lithium density, robust mechanical strength, and fine grain size are prerequisites for the safe and efficient operation of fusion blankets. While Li 2 TiO 3 -Li 4 SiO 4 biphasic ceramics have been developed to balance the trade-offs between single-phase breeders, achieving rigorous control over microstructure stability at elevated temperatures remains a challenge. In this work, a dual-optimization strategy combining solid solution strengthening and biphasic compositing was proposed. Novel Li 2 (Ti,Zr)O 3 -Li 4 SiO 4 ceramic pebbles with various phase ratios (Ti/Si atomic ratio = 1:0.5, 1:1, and 1:2) were successfully prepared for the first time. The introduction of Zr into the Li2TiO3 lattice serves as a grain growth inhibitor, while the Li 4 SiO 4 phase enhances sinterability. The results indicate that pure-phase and well-crystallized powders can be obtained at 700 °C. Interestingly, the addition of Li 4 SiO 4 was found to hinder the phase transition of Li 2 (Ti,Zr)O 3 effectively. Benefiting from the synergistic effect, the pebbles sintered at 1000 °C exhibit a refined grain size of <2 μm, significantly smaller than that of traditional Li 4 SiO 4 -based ceramics. Meanwhile, a satisfactory relative density of ∼82 %T.D. and a high crushing load of >70 N were achieved due to the improved sinterability. This study demonstrates that the Li 2 (Ti,Zr)O 3 -Li 4 SiO 4 ceramic, which integrates the advantages of structural stability from solid solutions and mechanical robustness from biphasic composites, holds great promise as a high-performance tritium breeder.
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Journal of the Taiwan Institute of Chemical Engineers
·
2026
·
IF 6.9
Abrar Hussain,Ndumiso Vukile Mdlovu,Kuen-Song Lin,Chi-Jung Chang,Amin Hussain
Background The conversion of CO 2 into value-added fuels and chemicals remains one of the major challenges in catalysis and sustainable energy research. Developing efficient catalysts for CO₂ hydrogenation to methanol and dimethyl ether (DME) is essential for reducing greenhouse gas emissions and promoting carbon recycling. Methods In this work, a Zr-modified CuO–ZnO–Al₂O₃ (CZZA) catalyst was synthesized via a co-precipitation method for CO 2 hydrogenation. The catalyst systems “CZZA/HZSM-5-L” and “CZZA/com-HZSM-5” represent Zr-modified CZZA physically integrated with loofah-templated and commercial HZSM-5 (Si/Al = 25), respectively. A bio-HZSM-5 catalyst was also prepared using loofah sponge and rice husks as dual biotemplates to promote methanol dehydration into DME. The novelty lies in (i) the dual-biomass templating strategy (silica-rich rice husk vs. low-silica loofah) to achieve macro– meso –micro hierarchies while retaining MFI crystallinity, and (ii) Zr-promotion of the Cu–ZnO–Al₂O₃ matrix to enhance Cu⁺/Cu²⁺ and Cu–Zn interfacial sites, enabling efficient one-pass CO₂ → MeOH → DME conversion at 280 °C and 30 bar. Significant findings Zr incorporation significantly improved the structural and electronic properties of the CZZA catalyst, leading to enhanced surface area, active site dispersion, and CuO–ZnO interfacial synergy. Among all tested catalysts, the CZZA/HZSM-5-L bifunctional catalyst achieved the highest DME yield (13.2 %), DME selectivity (58.6 %), and CO₂ conversion (22.5 %) at 280 °C and 30 bar. An economic evaluation of 5- and 10-ton-per-day (TPD) DME production using refinery waste CO₂ showed payback periods of 2.98 and 2.44 years, respectively. Sensitivity analysis (±20 % variation in H 2 and DME prices) confirmed the payback remained below 4 years, demonstrating the technical and economic viability of the developed Power-to-DME process.
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Advanced Science
·
2023
·Vol. 10
·期 10
·2206877
·
IF 15.1
Lu Chen,Youbing Li,Biao Zhao,Shanshan Liu,Huibin Zhang,Ke Chen,Mian Li,Shiyu Du,Faxian Xiu,Renchao Che,Zhifang Chai,Qing Huang
Electromagnetic (EM) wave pollution is harmful to human health and environment, thus it is absolutely important to develop new electromagnetic wave absorbing materials. MAX phases have been attracted more attention as a potential candidate for electromagnetic wave absorbing materials due to their high conductivity and nanolaminated structure. Herein, two new magnetic MAX phases with multiprincipal elements ((Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC) in which Fe atoms replace Al atoms in the A sites are successfully synthesized by an isomorphous replacement reaction of multiprincipal (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 AlC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 AlC MAX phases with Lewis acid salt (FeCl 2 ). (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC exhibit ferromagnetic behavior, and the Curie temperature ( T c ) are 302 and 235 K, respectively. The dual electromagnetic absorption mechanisms that include dielectric and magnetic loss, which is realized in these multiprincipal MAX phases. The minimum reflection loss (RL) of (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC is −44.4 dB at 6.56 GHz with 3 mm thickness, and the effective bandwidth is 2.48 GHz. Additionally, the electromagnetic wave absorption properties of the magnetic MAX phases indicate that magnetic loss also plays an important role besides dielectric loss. This work shows a promising composition-design strategy to develop MAX phases with good EM wave absorption performance via simultaneously regulating dielectric and magnetic loss together.
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PubMed
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Linmeng Huo,Lin Wang,Jingjie Li,Yanfeng Pu,Keng Xuan,Congzhen Qiao,Hao Yang
The disadvantage of Ce/Zr metal oxide as catalyst for direct synthesis dimethyl carbonate (DMC) from CO 2 and methanol is low DMC formation rate because of its low specific surface area and active sites. In this work, it can be improved by highly uniform dispersion cerium doped Zr-based metal-organic frameworks (UiO-66 MOFs), which were synthesized via a modified hydrothermal method. The as-prepared catalysts have been extensively characterized using XRD, BET, FT-IR, SEM, TEM, TGA, NH 3 -TPD, CO 2 -TPD, XPS techniques. Experimental evaluation results indicated that the highly uniform dispersed Ce-doped UiO-66 MOFs exhibited markedly improved catalytic performance than traditional Ce/Zr metal oxide catalyst. The highest yield of DMC catalyzed by Ce-UiO-66–2 was 0.295% (reaction time was 12 h; reaction temperature was 140 °C; reaction pressure was 11 MPa). Then, it was found that doping of Ce atoms into the zirconium lattice to produce UiO-66 MOFs could effectively increase the number of acidic and medium basic sites than UiO-66 (none Ce), thus could greatly enhance the catalytic performance. Moreover, using 2-cyanopyridine as dehydrating agent, the DMC yield could be further raised greatly. Last, based on reported literature and our results, a possible reaction mechanism over Ce-UiO-66-X was proposed.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jing Liu,Heguo Li,Bin Yan,Chao Zhong,Yue Zhao,Xuan Guo,Jinyi Zhong
Developing high-performance protective materials is important for soldiers and civilians who are exposed to the atmosphere of highly toxic chemical warfare agents (CWAs). Polyelectrolyte membranes are promising candidates with excellent chemical resistance and moisture permeability, but they cannot efficiently degrade CWAs. Here, we design and prepare a hybrid membrane through in situ growth of catalytically active zirconium-based metal–organic frameworks (Zr-MOFs) on a polyelectrolyte membrane mediated by biofilm-inspired curli nanofibers (CNFs). Superior to the bare polyelectrolyte membrane, the prepared MOF-808@CNF-PQ hybrid membrane exhibits improved rejection of the nerve agent simulant dimethyl methyl phosphonate (DMMP) vapor and permeation of the water vapor by 113 and 45%, respectively. The water/DMMP selectivity of the hybrid membrane reaches 498.6, approximately 13 times that of the commercial polyelectrolyte membrane Nafion 117. In addition, the hybrid membrane possesses appreciable catalytic activity for the hydrolysis of the nerve agent simulant dimethyl 4-nitrophenyl phosphate (DMNP) with a half-life of ∼38 min. Nanomechanical characterization results based on atomic force microscopy (AFM) techniques demonstrate the critical role of CNFs in mediating Zr-MOF nucleation and the dominant effect of electrostatic interactions on self-assembly of CNFs on polyelectrolyte base. It is also confirmed that the Zr-MOF toppings serve as the key components in physically adsorbing and chemically degrading the DMNP molecules through multiple strong intermolecular interactions. Our work offers a rational strategy to develop advanced membranes toward efficient chemical protection, moisture permeation, and catalytic detoxification against CWAs.
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PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2022
·
IF 3.841
Wei Qin,Xue Han,Junwei Wang,Xie Wang,Jianli Zhang
To design some excellent extractants for the separation of Zr(Ⅳ) and Hf(Ⅳ), a novel set of polyamidoamine dendrimers peripherally modified with salicylaldehyde (Abbreviated as PAMAM-SA) have been synthesized. UV-vis absorption and fluorescent spectrometry were used to study the selectivity of G.1.0, G2.0, G3.0 and G4.0 PAMAM-SA on Zr(Ⅳ) and Hf(Ⅳ) compared with other metal ions, and their extraction/separation performance on Zr(Ⅳ) and Hf(Ⅳ) was also investigated under different pH solutions. The results show that these dendrimers have superior selectivity on Zr(Ⅳ) and Hf(Ⅳ) as compared with Ca 2+ , Mg 2+ , Fe 3+ and Ni 2+ ions. The binding stoichiometry of G1.0, G2.0, G3.0 and G4.0 PAMAM-SA dendrimers with Zr(Ⅳ) is 1:4, 1:8, 1:10, 1:16 molar ratio determined by fluorescent titration respectively and the molar ratio of these dendrimers with hafnium is similar to that of zirconium. Both of the maximum extraction efficiency (EE%) on Zr(Ⅳ) and the separation coefficient (β Zr/Hf ) are following the order of G2.0-PAMAM-SA > G1.0-PAMAM-SA > G3.0-PAMAM-SA > G4.0-PAMAM-SA, and the maximum EE% on Zr(Ⅳ) is up to 98.9% and furthermore the β Zr/Hf is 1.52 for G2.0-PAMAM-SA at lower acid concentration compared with the reported extractants. The favorable higher EE% and β Zr/Hf indicate that G2.0-PAMAM-SA may be potentially employed as a highly selective and efficient extractant to enhance separating zirconium from hafnium.
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高影响因子
FUEL
·
2022
·
IF 8.035
Qiuju Fu,Dandan Liu,Weijing Niu,Shuo Zhang,Ruihua Chen,Yujia Wang,Pengze Zhao,Huimin Jiang,Yanchao Zhao,Lingzhi Yang,Liting Yan,Haiyan Wang,Xuebo Zhao
The highly efficient production of furfuryl alcohol (FFA) from biomass-derived furfural (FFR) is attracting increasing attention due to its wide application in the production of value-added chemicals. Zr-based MOF-808 is promising for liquid catalytic transfer hydrogenation (CTH) of FFR to FFA in terms of possessing a great number of Lewis-acid sites. Herein, a series of defective MOF-808 (D x -MOF-808) samples were prepared via a competitive coordination-removal strategy by modulating with benzoic acid (HBC). HBC was introduced as the temporary ligand for competing with formal ligand 1,3,5-benzenetricarboxylic acid (H 3 BTC) to coordinate with metal clusters and then it was removed with methanol to obtain the D x -MOF-808. The results showed that HBC serves not only as a temporary ligand participating in the synthesis of MOF-808 to obtain defective structure but also as a modulator controlling the particle size by terminating the growth of crystals. By changing the amount of HBC addition, the degree of ligand deficiency and the number of exposed Zr sites can be well regulated. Especially, excellent performance of FFR conversion (99%), FFA selectivity (94.4%) and FFA formation rate (48.6 mmol·g −1 ·h −1 ) was achieved over D 40 -MOF-808 sample with 2-propanol as a hydrogen donor under mild conditions (90 °C, 2 h), ranking it the best among the reported catalysts. Detailed characterizations proved that the high activity of D 40 -MOF-808 was jointly influenced by the high surface area, the high content of exposed Zr metal sites and ligand deficiency.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Qiong Li,Hao Qian,Tianyang Zheng,Xiaoyuan Sun,Yunfei Liu,Yinong Lyu
The cation displacement closely related to the local symmetry and corner-connected oxygen octahedral rotation are the structural origin of macroscopic properties in ABO 3 perovskite oxides. This work describes in detail the relationship between microstructure and macroscopic properties in 0.78BT-0.12CT-0.1BZS ceramic, which achieves the enhanced strain of 0.19 % with a hysteresis of 6.56 %. The atomic level structure is revealed by aberration corrected scanning transmission electron microscope (AC-STEM). The AC-STEM HAADF images reveal the coexisting of polar nanoregions with O and T symmetries. Such a microstructure has a lower energy barrier, facilitating dynamic polarization rotation flexibly under external stimuli. The AC-STEM ABF image reveals the existence of the BO 6 octahedral rotation, with rotation patterns of the a 0 b 0 c 0 and a - b + c - , and rotation angles are quantitatively measured. The BO 6 octahedral rotation and cation displacement are found to be consistent, the greater octahedral rotation with greater cation displacements. These results have important implications for understanding the structural origin of the excellent properties in ferroelectrics .
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