Molecular Catalysis
·
2022
·
IF 5.089
Cong Wang,Gang Li,Hongchen Guo
Compared with the mainstream approaches of doping the active metal in the MOFs structure and post-synthetic modification, it is more convenient to directly use the coordinatively unsaturated metal sites of MOFs for catalytic reactions. Herein, two forms of Ni-MIL-77 (1D Ni-MIL-77 and 3D MIL-77) were prepared using one-pot method and characterized by ICP-AES, XRD, FT-IR, XPS and SEM. Among them, 1D Ni-MIL-77 without high temperature heat treatment exhibited a better heterogeneous catalytic ethylene dimerization activity that was up to 989.6 g pro. /(g cat. ·h) (TOF=5544 h −1 ) and the selectivity of 1-butene could reach 93.3% at the optimal conditions. In addition, a probable Cossee-Arlman-like mechanism was proposed. By studying the catalyst structure after reaction, it was found that the reason for limited reuse was the hydrolysis products of the co-catalyst covered the catalysts.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Hengxi He,Weirui Chen,Jiaxin Zhou,Xukai Li,Jing Wang,Laisheng Li
The sluggish Me (n+m)+ / Me n+ redox cycle greatly restrained the catalytic ozonation performance of metal-based catalysts. To break this bottleneck, we adopted an interfacial oxidation reaction to create electron-deficient/rich centers within carbon skeleton derived from MOF (C-MOF) by utilizing the electronegativity difference between cerium (Ce) and manganese (Mn), and evaluated its catalytic ozonation activity with ibuprofen (IBP) as model pollutant. XPS, H 2 -TPR, LSV and EPR characterizations as well as DFT calculation demonstrated that there existed electron-deficient Ce sites and electron-rich Mn sites on CeO x /MnO x /C-MOF. Under the co-function of Ce and Mn sites, CeO x /MnO x /C-MOF/O 3 process achieved 100% IBP removal in 90 min, which was 3.1 times of sole ozonation process. IBP could be absorbed at the electron-deficient Ce center and directionally donate its electron to the O 3 around electron-rich Mn center. Singlet oxygen ( 1 O 2 ) played the major role in IBP degradation. Cl − , HCO 3 − , NO 3 − and SO 4 2− demonstrated limited inhibitions on IBP degradation. This work provided a sustainable strategy for breaking the rate-limiting step in the traditional catalytic ozonation.
研究领域:
环境科学
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催化
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材料科学
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产品关联
DOI
高影响因子
ChemElectroChem
·
2016
·Vol. 4
·期 2
·340-344
·
IF 3.506
Yan Li,Pinwwei Cai,Suqin Ci,Zhenhai Wen
Graphical Hydrogen evolution catalyst : Nanohybrids of Ni 2 P nanofilms on carbon nanosheets show high catalytic activity and excellent stability for the hydrogen evolution reaction in pH-universal electrolyte. A reliable strategy has been developed to prepare Ni 2 P nanofilms on carbon nanosheets (CNS) nanohybrids (Ni 2 P/CNS), which involves the preparation of three-dimensional (3D) CNS followed by in situ growth of Ni 2 P nanofilms on the surface of CNS. The Ni 2 P/CNS nanohybrids possess a robust 3D hierarchical structure, in which the Ni 2 P films are solidly overlaid on the surface of the CNS. The Ni 2 P/CNS nanohybrid was characterized by a variety of techniques, including X-ray diffraction (XRD), electron microscopy, X-ray photoelectron spectroscopy (XPS), etc. A series of electrochemical tests demonstrate the Ni 2 P/CNS nanohybrid shows high catalytic activity and excellent stability towards the hydrogen evolution reaction (HER) in pH-universal electrolyte, that is, in acidic, neutral, and basic media. The outstanding performance for Ni 2 P/CNS is correlated with the synergic effects between Ni 2 P and CNS associated with its unique and robust structure.
研究领域:
材料科学
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纳米技术
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电化学
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能量转换
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催化
✓ 已验证
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Lina Dai,Qiang Li,Xianglan Dong,Enqi Zhang,Yufeng Hu,Xin Guo,Yanduo Liu
Photocatalysis exhibits great potential for applications in solving energy and environmental problems, and has received widespread attention. This article constructs a new type of Mn-Fe Prussian blue analogues S-scheme mechanism photocatalytic material. The material is composed of oxidized photocatalysts (Ag 2 MoO 4 ) and reduced photocatalysts (Mn-Fe PBAs). The composite photocatalyst constructed in this way shows advantages such as a wide spectral response range, high charge carrier separation efficiency, and strong oxidation–reduction ability, which can significantly enhance photocatalytic efficiency. By studying the construction method and CO 2 reduction performance of the photocatalyst, the structure-performance relationship can be clarified. The CO production rate is 43.3 μmol/g/h, and the selectivity can reach 94.9 %, which is far superior to the current mainstream photocatalytic system. The electron transfer kinetics and S-scheme charge separation mechanism between the Mn-Fe PBAs and Ag 2 MoO 4 interfaces are explained by steady-state surface photovoltage spectroscopy (SS-SPS) and near ambient pressure XPS (NAP-XPS). In-situ DRIFTS techniques are used to monitor the changes of transition intermediates, and combined with theoretical calculations, the activation mechanism of CO 2 by the Mn-Fe catalytic site is deeply revealed at the atomic level. This study provides new theoretical guidance and profound insights for the construction of Prussian blue analogues photocatalysts.
研究领域:
材料科学
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环境科学
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物理化学
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纳米技术
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催化
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能量转换
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xinyan Wang,Yuting Zhang,Jian Zhang,Chengpeng Shao,Jiaxing Yang,Yuning Zhang,Ruoyi Li,Zheng Xing
In this study, a Z-type heterojunction photocatalyst CoWO 4 /CS/BiOCl-10 was constructed by hydrothermal synthesis for the efficient removal of norfloxacin (NOR) contaminants in water. X-ray photoelectron spectroscopy (XPS) combined with Fourier transform infrared spectroscopy (FT-IR) confirmed that the hydroxyl group in the chitosan (CS) molecule was bonded with the oxygen atom on the surface of CoWO 4 through hydrogen bonding to form a directional charge transport channel, which greatly improved the photocatalytic degradation efficiency of CoWO 4 /CS/BiOCl-10, and the degradation rate was as high as 98.30 % within 90 min under 300 W xenon lamp irradiation. Optoelectronic measurements show that the interfacial potential difference drives electrons to migrate along the Z-path. Density functional theory (DFT) and liquid chromatography-mass spectrometry (LC-MS) were used to identify intermediates in the NOR degradation process, revealing the degradation pathway of NOR through piperazine ring cleavage and defluorination. The kinetics of NOR degradation intermediates were revealed using two-dimensional correlation spectroscopy (2DCOS) techniques. Rice seed germination experiments have shown that the degraded NOR solution is virtually non-toxic, greatly reducing the environmental impact. This study provides a new strategy for the development of efficient photocatalytic systems through the synergistic regulation mechanism of hydrogen bonding and heterojunction.
研究领域:
环境科学
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材料科学
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光催化
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水处理
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化学工程
·
光谱学
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毒理学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Zailun Liu,Yunfei Ma,Junqing Li,Ying Tu,Hui Yang,Kelin He,Chao Chen,Yulin Wang,Xiang Lin,Hongli Sun,Chenliang Su,Qitao Zhang
Uncovering the excitation processes of photocatalysts and enhancing the dissociation of excitons into free photogenerated electrons and holes for photocatalytic CO 2 reduction is imperative yet quite challenging. Herein, an efficient strategy of reducing the binding energy of excitons to boost exciton dissociation is reported by anchoring the low valence single-atom Cu sites in In 2 S 3 nanosheets (Cu-In 2 S 3 ), which can enhance photocatalytic CO 2 reduction activity. The investigations of photo-irradiated Kelvin probe force microscopy (KPFM), in situ irradiates X-ray photoelectron spectroscopy (XPS), and temperature-dependent photoluminescence (TD-PL) indicate that the doping of low valence single-atom Cu can efficiently drive the charge transfer and separation. Moreover, the studies of the dynamic behaviors of charge carriers by femtosecond time-resolved spectroscopy (fs-TAS) reveal that the doping of low valence Cu single-atom sites allows the promotion of exciton dissociation by reducing the binding energy of the exciton, resulting in an enhanced photocatalytic CO 2 reduction of Cu-In 2 S 3 nanosheets. The aforementioned strategy for enhancing the dissociation efficiency of excitons in photocatalysts will offer a highly efficient and promising approach for the photocatalytic CO 2 reduction and other photocatalytic applications.
研究领域:
光催化
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材料科学
·
纳米技术
·
物理化学
·
能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shufan Yu,Zhao Sun,Zhiqiang Sun
Methanol steam reforming is a promising approach for real-time hydrogen production, while its practical application is hindered by catalyst deactivation and undesired CO byproduct formation. In this study, we propose a self-activation approach to anchoring a series of x CuO/YCrO 4 catalysts by employing methanol and steam as reductants. The self-activated 0.8CuO/YCrO 4 catalyst achieves a high hydrogen production rate of 22.3 μmol H 2 ·g −1 cat ·s −1 and demonstrates exceptional stability over 3000 min at 220°C. TEM-EDS, XPS, EPR, and XAS collectively reveal the promotion of generating Cu δ + /Y-O v -Cr interfacial sites and oxygen vacancies via self-activation, and in situ Raman spectroscopy confirms the structural stability of the Y-O v -Cr framework. In situ DRIFTS analysis further confirms that Cu δ + /Y-O v -Cr interfacial sites effectively anchor and promote the hydrogenation of bidentate formate intermediates, mitigating active site blockage by byproduct species and enhancing catalytic efficiency. This work provides new insights into the self-activation mechanism of Cu-based catalysts and offers a promising strategy for developing highly active and durable catalysts.
研究领域:
催化化学
·
制氢技术
·
材料科学
·
表面化学
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化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Yanan Cai,Jing He
The release of Mn(II) occurs in the degradation of organic matters by manganese ore (MnO 2 ), resulting in a reduced efficiency. During the degradation of ciprofloxacin (CIP), in a biofilter, this paper put forward a novel method that similar to the geo-cycle of Mn (MnCS) on the Earth to regenerate MnO 2 . The freshly prepared MnO 2 was suitable for the use in the MnCS. It indicated that the mutual conversion between Mn(II), Mn(III), and Mn(IV) in the MnCS, which was driven by CIP and manganese oxidizing bacteria (MnOB), could maintain the activity of MnO 2 . The MnCS showed feasibility in the coexistence of ammonia or humic acid , and provided a kinetic degradation. The physicochemical features of MnO 2 before and after bio-regeneration were characterized by TEM , XRD, BET, and XPS. It was found that the morphological structure of MnO 2 became loose and the maximum peak of pore size distribution became smaller, but the increase of surface area, the change of Mn(III/IV) content, and the decrease of crystallinity favored the bio-regeneration process. Moreover, as a mediator in the MnCS, the group of MnOB was dramatically inhibited by CIP, and the bacterial community had changed significantly. The typical MnOB shared low abundance in the biofilter, while the rarely reported genera (e.g. Sphingomonas ) that related to the formation of Mn deposits appeared to be involved in the MnCS.
研究领域:
环境科学
·
微生物学
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化学
·
生物技术
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Shengyong Lu,Xinlei Huang,Minghui Tang,Yaqi Peng,Shuchao Wang,Chengetai Portia Makwarimba
Typical organic pollutants from coal-combustion flue gas such as volatile organic compounds (VOCs) need to be effectively controlled. This work synthesized a series of nitrogen-doped hierarchical porous carbons (NHPCs) by one-step activation with various proportions of cellulose, (NH 4 ) 2 C 2 O 4 and KHCO 3 /NaHCO 3 . The NHPCs have a high specific surface area and pore volume up to 2816 m 2 /g and 1.413 cm 3 /g as well as a hierarchical porous structure with micro-meso-macropores distribution. The dynamic adsorption tests of toluene at 600 ppm showed that NHPCs have a high adsorption capacity up to 585 mg/g (NHPC(K)131), this was about 3 times more than that of AC (208 mg/g), and is a better absorbent compared to many other carbon adsorbents. The porous characteristics and toluene adsorption properties of NHPCs improved along with the fluctuation of the proportions of raw materials and active agents. The micropore size of the material is the main factor that affecting the toluene adsorption capacity. The analysis of toluene dynamic adsorption breakthrough curves revealed that NHPCs had great toluene adsorption kinetics with high adsorption rate constants and short mass transfer zone. The excellent toluene adsorption kinetics of NHPCs can be attributed to the hierarchical porous structure. The abundant 2–10 nm mesopores and macropores of NHPCs act as mass transfer channels for toluene molecules. The XPS analysis showed that the NHPCs have nitrogen doping up to 6.71% (NHPC(Na)161) and they effectively promote toluene adsorption. The nitrogen doping mechanism can be attributed to the reactions between cellulose pyrolysis substances and NH 3 which decomposed from (NH 4 ) 2 C 2 O 4 . Moreover, the pore forming reactivity of KHCO 3 is better than that of NaHCO 3 in the NHPCs activation process.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Niu Liu,Jun Cheng,Wen Hou,Xiao Yang,Junhu Zhou
In order to form strengthened active sites for superior CO 2 adsorption on core shell ZIF-8@ZIF-67 nanocomposites , graphene oxide (GO) with oxygen-containing functional groups was used as support to synthesize hybrid adsorbents with unsaturated Zn–N 2 –O active sites. The results of XPS O 1s and FTIR analysis revealed that the Me–O functional group content in the 0.5 wt% graphene oxide (GO)-supported core shell ZIF-8@ZIF-67 nanocomposite (38.9 at.%) was much higher than that in the 0.5 wt% reduced graphene oxide (RGO)-supported nanocomposite (19.4 at.%). This was because hydroxyl functional groups in the GO formed coordination bonds with zinc atoms in core shell ZIF-8@ZIF-67. XPS N 1s spectra indicated that the incorporation of oxygen-containing functional groups in GO resulted in the transition of binding form from Me–N 4 to Me–N 2 . The CO 2 adsorption capacity of GO-supported core shell ZIF-8@ZIF-67 gradually decreased from 2.15 to 1.30 mmol/g as GO weight percentage increased from 0.5 to 4 wt%, which was consistent with the decrease in BET surface area from 1378 to 585 m 2 /g and increase in peak pore diameter from 7.7 to 8.2 Å. Density functional theory (DFT) calculations demonstrated that unsaturated Zn–N 2 –O active sites in GO-supported core shell ZIF-8@ZIF-67 nanocomposites resulted in a decreased O C⋯Zn interaction distance from 4.65 (Zn–N 4 sites in core shell ZIF-8@ZIF-67) to 3.46 Å and an increased binding energy from 34.02 to 38.87 kJ/mol. Therefore, 0.5 wt% GO-supported core shell ZIF-8@ZIF-67 nanocomposites exhibited the highest CO 2 adsorption capacity of 2.15 mmol/g (at 273 K and 1 bar), 1.34 times higher than that of core-shell ZIF-8@ZIF-67.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2015
·
IF 1.098
Yong Zhou,Zhelan Dai,Ding Zhai,Congjie Gao
Polypiperazine-amide membranes were modified with poly(ethyleneimine) (PEI) by self-assembled method, through which PEI molecules were fixed on the membrane surface by ionic interaction. In the experiments, the PEI concentration ranged from 50 to 2000 mg·L − 1 while the depositing time was fixed at 20 min. The results showed that low PEI concentration resulted in a slight increase of pure water flux, which was attributed to the enhanced membrane surface hydrophilicity. The PEI adsorption on membrane surface had less effect on the rejections to neutral PEG and sucrose, but improved the rejections to divalent cationic ions and methylene blue as the result of reversion of the membrane surface charge from negative to positive according to the XPS analysis and zeta potential measurements. The membrane modified at PEI = 1500 mg·L − 1 exhibited high rejection to methylene blue (MB) and is potential to be applied in the treatment of effluents containing positively charged dyes.
研究领域:
环境工程
·
膜科学
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Hao Zhu,Shunyan Ning,Zengzhiqiang Li,Xinpeng Wang,Toyohisa Fujita,Yuezhou Wei,Xiangbiao Yin
Here, a nano disc-shaped bimetallic organic framework (NbCo-piperazine) was prepared by the solvothermal method for the activation of PMS for the degradation of contaminants. The effects of Nb/Co ratio, synthesis time and temperature on the morphology, structure and performance of the NbCo-piperazine catalyst were characterized by XRD, FT-IR, SEM-EDS and TEM. The optimum conditions for NbCo-PZ to activate PMS degradation of tetracycline were investigated by adjusting the dosage of catalyst, tetracycline concentration, pH and PMS concentration. The catalytic performance of NbCo-PZ in the presence of co-existing anions (Cl − , NO 3 – , HCO 3 2– , H 2 PO 4 − ) was also evaluated. XPS explained that cyclic changes in the valence states of Nb 4+ /Nb 5+ and Co 2+ /Co 3+ accelerated the activation of the PMS degradation process. EPR results showed the presence of free radicals (SO 4 ·− , ·OH and O 2 ·− ) and non-free radicals ( 1 O 2 ) in the degradation process, with free radicals playing a major role in the degradation process. The degradation rate of tetracycline after three cycles was 92.2%. In addition, NbCo-piperazine showed good catalytic performance for other organic pollutants such as methyl blue, tylosin tartrate and tetracycline with the degradation rate of 97.8%, 95.2% and 95.5%, respectively. Moreover, it also has good catalytic properties in various water systems such as river water and sea water.
研究领域:
环境化学
·
催化
·
水处理
·
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）