CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Uddin Sk Raihan,Jingqi Zhang,Jingbo Chao,Qing Hu,Frederic Coulon,Xiao Jin Yang
Chlorinated phenols are highly toxic to human and ecosystem and their biological degradation is difficult. In this work, a novel MgAlNi alloy catalyst was developed for rapid chemical degradation of p-chlorophenol (4-CP) in water under mild conditions via in situ hydrodechlorination ( i HDC) without external hydrogen gas supply. A complete conversion of 0.195 mM 4-CP to phenol was achieved within 15 min with a reaction rate constant of 7.65 h −1 , 19.4 times higher than that of the traditional Raney Nickel (AlNi alloy) catalyst. The excellent performance of MgAlNi alloy catalyst is attributed to enhanced H 2 generation by Mg etching, surface self-reconstruction by growth of in situ layered double hydroxide ( i LDH) nanosheets of 0.08–1 nm, exposed active sites of AlNi intermetallic compounds Al 3 Ni 2 and Al 3 Ni. The findings of this study provide new insights into broader applications of nanoconfinement catalysis to environmental remediation and open a new domain of in situ nanoconfinement catalysis ( i NCC).
研究领域:
环境科学
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催化化学
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DOI
高影响因子
ChemCatChem
·
2018
·Vol. 10
·期 10
·2254-2259
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IF 4.674
Zhenchao Zhao,Yanlu Li,Mathias Feyen,Robert McGuire,Ulrich Müller,Weiping Zhang
Noble metal nanoparticles (NPs) encapsulated in zeolites bearing distinct shape-selective properties at molecular level expand their new applications in catalysis. Here we report a synthesis strategy for the encapsulation of Pd NPs inside FER zeolite via a layer reassembling process. Pd precursors were introduced by swelling FER layers in RUB-36 through the surfactant cetyltrimethylammonium cations (CTA + ) and then an ion-exchange process at ambient temperature. Pd@FER was formed with a uniform diameter distribution of Pd NPs at about 1.4 nm during the topotactic transformation from layered zeolite precursors to 3-dimensional zeolites followed by calcination. The as-prepared Pd@FER catalyst exhibits distinct shape-selective properties in hydrogenation reactions. It has relatively lower activity for 1-hexene and almost no activity for 1-phenyl-1-cyclohexene compared with Pd/RUB-37 catalyst prepared via wet impregnation due to the restrictions of channels in the FER zeolite. On the contrary, Pd@FER shows very high hydrogenation activity for benzaldehyde and very low activity for diphenylmethanone hydrogenation, while Pd/RUB-37 exhibits high hydrogenation activity for both benzaldehyde and diphenylmethanone. This synthesis strategy may be extended to other noble metals or two-dimensional layered zeolite systems for size-selective hydrogenation reactions. Graphical There's the RUB : FER zeolite encapsulating Pd nanoparticles with excellent shape-selective catalytic properties were constructed and synthesized through swelling RUB-36, ion exchange, and topotactic conversion processes.
研究领域:
催化化学
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材料化学
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纳米催化
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多相催化
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分子筛化学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Jiahui Zhang,Hongyi Zhang,Zhen Chen,Zhenghua Zhang
Pervasive exposure to different micropollutants (e.g. endocrine disrupting chemicals and pharmaceuticals) present in water environments, presents a notable risk to public health. Herein, three Co-based bimetallic layered double hydroxides (LDHs) were fabricated, then assembled into LDH-based nanoconfined catalytic membranes (CoM m , M: Fe, Mn, and Cu) with similar structural and physicochemical properties. The micropollutant removal performance of CoM m in the presence of peroxymonosulfate (PMS) was ranked in the order: CoMn m > CoFe m > CoCu m . The CoMn m achieved a 100% removal efficiency for pharmaceuticals and endocrine disrupting chemicals, achieving a first-order rate constant (1.64 ms −1 for ranitidine) that was 10 2 –10 6 higher than traditional LDH catalysts. Density functional theory (DFT) results revealed that CoMn m possessed the highest adsorption energy with PMS and d-band centre, exhibiting superior chemisorption activity and faster charge transfer than the other prepared membranes. Furthermore, the nanoconfinement effect within membrane nanochannels contributed to the outstanding performance of CoMn m . This study provides an atomic-scale understanding of the catalytic mechanisms of CoM m , guiding the design and optimization of catalytic membranes for water purification.
研究领域:
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
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2025
·
IF 7.5
Yanxin Zhang,Xuesi Hong,Yuzhu Shi,Duo Xu,Yueqin Song,Xiaolong Zhou,Jin An Wang
The present study investigated a novel bimetallic Pt-Mo catalyst encapsulated within Silicalite-1 zeolite for propane dehydrogenation (PDH). The catalyst was synthesized via in situ hydrothermal crystallization, followed by direct high-temperature H 2 reduction without conventional calcination, leading to uniform encapsulation of Pt nanoparticles within the zeolite framework and simultaneous removal of the template and organic ligands. PDH performance was evaluated in a continuous-flow fixed-bed microreactor. Comprehensive characterizations (XPS, CO-DRIFTS, NH 3 -TPD, Raman, etc.) reveal that Mo incorporation in 0.4Pt@S-1 catalyst significantly enhances propane conversion while maintaining high propylene selectivity. Moreover, the bimetallic 0.4PtXMo@S-1 catalyst with 0.1 % Mo doping achieved an outstanding performance at 550 °C and a WHSV of 5.49 h −1 (propane conversion: 43 %, propylene selectivity: 97 %, propylene formation rate: 16.27 mol C3H6 ·g Pt -1 ·h −1 ). The prepared catalyst possessed favorable stability and regeneration performance, showing a deactivation rate of only 0.001454 h −1 after four reaction-regeneration cycles. This enhancement is attributed to synergistic effects arising from Mo incorporation, which promotes Pt nanoparticle dispersion, modulates Brønsted /Lewis acidity, and facilitates interfacial electron transfer between Pt and Mo species. These findings highlight the role of Pt-Mo interactions within zeolite frameworks, providing new insights for designing efficient and stable PDH catalysts.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chenchen Meng,Zheng Wang,Wei Zhang,Lele Cui,Bo Yang,Haijiao Xie,Zhenghua Zhang
Practical applications for the degradation of organic contaminants by conventional batch-mode heterogeneous advanced oxidation processes remain elusive due to mass-transfer limitations of short-lived reactive oxygen species (ROS). Nanoconfinement catalysis has received increasing attention because of enhanced reaction efficiency and mass and electron transfer. Here, we implemented the concept of nanoconfinement catalysis using a two-dimensional membrane. Ultrathin cobalt-copper oxide nanosheets (Co-Cu ONS) rich in active sites and oxygen vacancies were prepared through a facile solution reduction method. The assembled Co-Cu ONS membrane with active sites confined within membrane nanochannels spontaneously activates peroxymonosulfate and facilitates the generation of ROS and the redox cycles of metal cations. Therefore, an ultimate degradation efficiency (∼100%), ultrafast (∼86 ms) decomposition of organic pollutants, and excellent catalytic stability (greater than120 h) were achieved. The degradation rate is 10 3−5 times faster than the best state-of-the-art. This approach offers an attractive alternative for water purification with membrane-based nanoconfinement catalysts.
研究领域:
环境科学
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材料科学
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催化
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水处理
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Jiankang Wang,Yajing Wang,Yuan Peng,Zhongping Yao,Peng Zhang,Taiping Xie
The limited mass transfer and sluggish reaction kinetics of traditional powder catalysts, as well as the trade-off between permeate flux and the removal efficiency of confined membranes, have significantly hindered practical application in wastewater treatment. In this work, a Co 2 CO 3 (OH) 2 /polyvinylidene fluoride (Co 2 CO 3 (OH) 2 /PVDF) confined catalytic membrane was constructed via a one-step hydrothermal method and used as a peroxymonosulfate (PMS) activator for tetracycline (TC) degradation. Surprisingly, Co 2 CO 3 (OH) 2 /PVDF achieved 99.67 % TC removal under continuous flow-through mode with an extremely short hydraulic retention time of 5.4 ms and a high permeate flux of 7085.5 L m −2 h −1 bar −1 . Furthermore, the reaction kinetic constant was five orders of magnitude higher than that under batch mode (1.07 ms −1 vs 0.37 min −1 ), demonstrating the superiority of membrane-confined catalysis in enhancing TC removal. Reactive oxygen species (ROS) scavenging experiments, electron paramagnetic resonance (EPR) spectra and electrochemical measurement revealed that the oxidative degradation of TC was dependent on cooperative attack of radicals (SO 4 • − , •OH and O 2 • − ) and non-radicals ( 1 O 2 ). Subsequently, three possible degradation pathways were proposed. This study highlighted the significance of confined effect and Co(Ⅱ) catalysis in synergistically promoting PMS activation for ultrafast TC removal, demonstrating the potential application of membrane-confined catalysis in industrial wastewater treatment.
研究领域:
环境科学
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化学工程
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催化
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材料科学
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水处理技术
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产品关联
DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Bo Tang,Xu Zuo,Ang Li,Jiajun Wang,Haojun Zou,Lili Xu,Weili Dai
Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., AuxPty@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au1Pt3@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h–1 at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O2 and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.
研究领域:
催化化学
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绿色化学
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纳米材料科学
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多相催化
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生物质转化
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 38
·32731-32740
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IF 9.5
Ying Li,Dandan Song,Bing Liu,Xin Li,Jie Huang,Haiyan Zhu,Gang Shi
A surface-enhanced Raman spectroscopy sensor combined with the molecular imprinting technique (MIT-SERS) has the ability of high sensitivity and specific recognition, but its accurate quantitative analysis and high-stability reuse are poor. To solve the above problems, a novel MIT-SERS sensor with internal standard self-correction and spatially separated photocatalysis is designed. This MIT-SERS sensor is composed of a SERS substrate and a MIT recognizer. Photocatalyst TiO2, co-reductant catalyst Ag and co-oxidant catalyst Fe2O3 are the main materials of the SERS substrate. The occupying molecule C3H6S and the template molecule 4-ATP are adsorbed on the surface of Ag and Fe2O3 in turn. The molecularly imprinted layer is SiO2. It is worth noting that the space-confined assembly of C3H6S and 4-ATP ensures that C3H6S is protected and 4-ATP is completely degraded during the photocatalysis process, realizing the reusability of the MIT-SERS sensor. In addition, SiO2 is used as an internal standard to improve the accuracy of quantitative analysis of the sensor. For this MIT-SERS sensor, the detection limit (LOD) is as low as 2.24 × 10−11 M and the linear fit (R2) of quantitative analysis is as high as 0.9975. During repeated use, the relative standard deviation (RSD) of the corrected signals from the MIT-SERS sensor is as low as 1.27%.
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DOI
高影响因子
WATER RESEARCH
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2024
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IF 11.4
Peijie Li,Daliang Xu,Yunfei Gao,Peng Liu,Zihan Liu,Junwen Ding,Junyong Zhu,Heng Liang
Despite widespread deployment and investigation of ultrafiltration (UF) for secondary effluent purification, the challenge of membrane fouling due to effluent organic matter (EfOM) remains formidable. This study introduced a novel pretreatment method utilizing Co nanoparticles-encapsulated carbon nanotubes activated peroxymonosulfate (Co@CNT/PMS) to degrade EfOM and mitigate membrane fouling. Characterization of Co@CNT revealed the efficient encapsulation of Co nanoparticles within nanotubes, which notably enhanced the catalytic degradation of bisphenol A and typical organics. The tube-encapsulated structure increased the concentration of reactive species within the confined nanoscopic space, thereby improving the probability of collisions with pollutants and promoting their degradation. The Co@CNT/PMS pretreatment led to substantial reductions in aromatic compounds, fluorescent components, and both high and middle molecular weight substances. These changes proved crucial in diminishing the fouling potential in subsequent UF processes, where reversible and irreversible fouling resistances decreased by 97.1 % and 72.8 %, respectively. The transition volume from pore blocking to cake filtration markedly increased, prolonging the formation of a dense fouling layer. Surface properties analysis indicated a significant reduction of pollutants on membrane surfaces after the Co@CNT/PMS pretreatment. This study underscored the efficacy of confinement-based advanced oxidization pretreatment in enhancing UF performance, presenting a viable resolution to membrane fouling.
研究领域:
环境工程
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水处理
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纳米技术
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催化
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膜科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子