JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Ping Li,Huanhuan Wu,Chengming Zhang,Quangui Liang,Huihui Ding,Haibao Zhu,Jun Ma,Xiang Li,Shuangshuang Huai,Congliang Cheng,Xiufang Wang
The lack of active sites and the low availability of photoelectrons severely limit the photocatalytic reduction of nitrogen to ammonia in semiconductor materials. Here, we successfully designed a BiOBr/O v -TiO 2 -Cu heterojunction catalyst toward N 2 fixation into NH 3 . The optimized BiOBr/O v -TiO 2 -Cu heterojunction has a promising photocatalytic performance and stability with the highest NH 3 yield of 259.82 μmol·g −1 ·h −1 . The combination of detailed theoretical simulation calculations and comprehensive characterizations indicates the BiOBr/O v -TiO 2 -Cu heterojunction with oxygen vacancy (O v ) stabilized Cu nanoparticles (NPs) as active sites can effectively adsorb and activate N 2 molecules. The close contact between BiOBr and Ov-TiO 2 elevates the quick transmission of photogenerated electrons at the interface and the enrichment on Cu NPs. This work not only provides an efficient photocatalyst for the N 2 reduction, but also supplies theoretical support for identifying the active sites and charge transfer kinetics of the nitrogen reduction reaction.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Carbon Energy
·
2025
·
IF 24.2
Zhao Sun,Kun Lei,Louise R. Smith,Nicholas F. Dummer,Richard J. Lewis,Haifeng Qi,Kieran J. Aggett,Stuart H. Taylor,Zhiqiang Sun,Graham J. Hutchings
Advanced oxygen carrier plays a pivotal role in various chemical looping processes, such as CO 2 splitting. However, oxygen carriers have been restricted by deactivation and inferior oxygen transferability at low temperatures. Herein, we design an Fe–O v –Ce–triggered phase-reversible CeO 2− x ·Fe·CaO ↔ CeO 2 ·Ca 2 Fe 2 O 5 oxygen carrier with strong electron-donating ability, which activates CO 2 at low temperatures and promotes oxygen transformation. Results reveal that the maximum CO 2 conversion and CO yield obtained with 50 mol% CeO 2− x ·Fe·CaO are, respectively, 426% and 53.6 times higher than those of Fe·CaO at 700°C. This unique multiphase material also retains exceptional redox durability, with no obvious deactivation after 100 splitting cycles. The addition of Ce promotes the formation of the Fe–O v –Ce structure, which acts as an activator, triggers CO 2 splitting, and lowers the energy barrier of C═O dissociation. The metallic Fe plays a role in consuming O 2− lattice transformed from Fe–O v –Ce, whereas CaO acts as a structure promoter that enables phase-reversible Fe 0 ↔ Fe 3+ looping.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengyu Zhang,Jing Wu,Wen Tang,Jinfei Mei,Qian Zhang,Junrong Wu,Deyun Xu,Zhaodi Liu,Fuying Hao,Liangquan Sheng,Huajie Xu
Regulating interfacial active sites to improve peroxymonosulfate (PMS) activation efficiency is a hot topic in the heterogeneous catalysis field. In this study, we develop an inverted loading strategy to engineer asymmetric Mn–O V –Ce sites for PMS activation. Mn 3 O 4 @CeO 2 prepared by loading CeO 2 nanoparticles onto Mn 3 O 4 nanorods exhibits the highest catalytic activity and stability, which is due to the formation of more oxygen vacancies (O V ) at the Mn–O V –Ce sites, and the surface CeO 2 layer effectively inhibits corrosion by preventing the loss of manganese ion active species into the solution. In situ characterizations and density functional theory (DFT) studies have revealed effective bimetallic redox cycles at asymmetric Mn–O V –Ce active sites, which promote surface charge transfer, enhance the adsorption reaction activity of active species toward pollutants, and favor PMS activation to generate (•OH, SO 4 •− , O 2 •− and 1 O 2 ) active species. This study provides a brand-new perspective for engineering the interfacial behavior of PMS activation.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mufan Wang,Shiying Fan,Shaomin Liu,Xinyong Li
5-Hydroxymethylfurfural (HMF) serves as a key platform molecule for producing high-value chemicals via green and efficient photocatalytic oxidation. Transition metal oxides, particularly spinel substances, are promising heterogeneous catalysts due to their ability to promote interfacial electron transfer. However, the impact of interfacial electron transfer in HMF photocatalytic oxidation on spinel catalysts remains largely unexplored. In this study, we engineered Mn 4+ -O V -Co 2+ active sites in cobalt-based spinel by in-situ (MCO 4-δ -1) and post-doping (MCO 4-δ -2) strategies to investigate their impact on photocatalytic HMF oxidation. The microstructure morphology, chemical valence states, and band structure of prepared catalysts were systematically characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and UV–vis diffuse reflectance spectra (DRS) techniques. The results revealed that the post-doping catalyst (MCO 4-δ -2) exhibited a higher density of surface oxygen vacancy (Ov), significantly enhancing charge transfer and HMF photocatalytic conversion activity. Specifically, MCO 4-δ -2 achieved an outstanding HMF oxidation product yield of 356.55 μmol g −1 under visible light over 4 h. Furthermore, density functional theory (DFT) calculations provided mechanistic insights, revealing that the oxygen in the aldehyde group of HMF preferentially occupies surface Ov sites at Mn 4+ -Ov-Co 2+ interfaces, thereby facilitating selective HMF oxidation pathways. This study not only expand the application scope of cobalt-based spinel photocatalysts in biomass valorization but also provides an insight on the effects of doping-induced interfacial electronic effects in photocatalytic oxidation reactions.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
Revista Brasileira de Farmacognosia-Brazilian Journal of Pharmacognosy
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2024
·
IF 1.4
Xie Huilong,Fu Yunrong,Lin Zhisheng,Wang Jiayi,Wu Jingyu,You Xiuhua,Xie Jieming
This study explores the synergistic effect of T-CUS 245C combined with cyclosporin A, and its possible mechanism. T-CUS 245C is an immunotoxin conjugated with tastuzumab and recombinant cucurmosin 245C (CUS 245C ). Cyclosporin A is a calcium antagonist mainly used as an immune-suppressive agent, which enhances the cytotoxicity of immunotoxins through an unknown mechanism. The sulforhodamine B assay, flow cytometry, DNA fragmentation apoptosis assay, and western blot analysis were used to evaluate the synergistic effects of cyclosporin A combined with T-CUS 245C on proliferation inhibition and apoptosis induction in SK-OV-3 ovarian cancer cells with HER-2-overexpressing. Meanwhile, using confocal microscopy and flow cytometry, the effect of cyclosporin A on the intracellular distribution of T-CUS 245C was observed and quantified. The results of this study showed that the combination index of cyclosporin A combined with T-CUS 245C is less than 0.7, indicating that cyclosporin A significantly enhances the proliferation inhibition and apoptosis induction induced by T-CUS 245C in SK-OV-3 cells. The confocal microscopy and flow cytometry results show that cyclosporin A effectively increases the dispersion of T-CUS 245C in the cytoplasm by promoting the endolysosomal escape. This study demonstrates that cyclosporin A combined with T-CUS 245C has a synergistic anticancer effect, by facilitating the release of T-CUS 245C in the intracellular space. Graphical Abstract
研究领域:
肿瘤学
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细胞生物学
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药理学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Yujia Han,Teng Zong,Yuehan Wang,Ming Tian,Chaojie Wang,Nanxin Wang,Xiaodong Wang
Chemical looping H 2 O splitting is considered as a promising approach to produce hydrogen thanks to its lower energy consumption and carbon footprint compared with traditional steam reforming. Fe-based oxides have been paid much attention but suffer from inferior H 2 production rate and stability due to insufficient activation for H 2 O. Herein, it was found that the introduction of Cr into MgFe spinel oxides (MgFe x Cr 2-x O 4 , MFCO) could greatly increase the performance of H 2 O splitting driven by CH 4 reduction with the highest peak H 2 production rate of about 4.65 mmol min −1 g −1 , H 2 productivity of about 2.88 mmol g −1 and good stability during multiple redox cycles for MFCO-46 (the atomic ratio of Fe and Cr of 2:3), which exceeded most of the state-of-the-art Fe-based oxides. This originated from the Cr doping promoting Fe 0 nanoparticles exsolution by activating CH 4 and Fe-O v -Cr species formation which relay catalyzed H 2 O splitting and was favorable for the fast recovery of lattice oxygen converted.
研究领域:
化学工程
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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
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·
IF 3.1
Xiang Shuang,Guo Yong,Liu Xiaohui,Wang Yanqin
The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis reactions. Herein, we create the Au-CoO-O V interface in the 1.0%Au/Co 3 O 4 -Rod-250 catalyst, which could dissociate H 2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-O V surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen (signals of Au—D and O—D vibration) compared with bare CoO (Co 3 O 4 -Rod-250). This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 25
·14286-14295
·
IF 3.049
Wenhui He,Yawen Wang,Caimei Fan,Yunfang Wang,Xiaochao Zhang,Jianxin Liu,Rui Li
The introduction of oxygen vacancies (OVs) on the surface of photocatalysts has already been proven to be an effective way to extend the light response to visible light and trap charge carriers, thereby promoting the photocatalytic performance. In this study, h-BN/OV-BiOCl composites were prepared using hexagonal boron nitride (h-BN) to further improve the visible-light photocatalytic activity of oxygen-vacancy-enriched bismuth oxychloride (OV-BiOCl). The composition and morphology of these materials were investigated, and the photocatalytic performance experiments showed that the introduction of h-BN could significantly improve the visible-light photocatalytic activity of OV-BiOCl, which was 1.7 and 1.4 times that of pure OV-BiOCl for the degradation of rhodamine B (RhB) and bisphenol A (BPA) when the h-BN content was 5 wt%, respectively. The role of h-BN was comprehensively investigated, and the results revealed that the presence of negatively charged h-BN could improve the separation efficiency of photoinduced electrons (e−) and holes (h+) by promoting the migration of positively charged h+ to the surface of the photocatalyst, as expected. Moreover, the oxygen vacancies in OV-BiOCl were increased in the presence of h-BN; this favored the activation of more adsorbed O2 for the oxidation of pollutants. Finally, a probable mechanism was proposed for the improved photocatalytic activity of the h-BN/OV-BiOCl composites. This study provides an insight into the roles of h-BN in oxygen-vacancy-enriched photocatalysts.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
POLYMER BULLETIN
·
2024
·Vol. 81
·期 11
·10081-10118
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IF 3.1
Alassod Abeer,Alkhateeb Weaam,Alghoraibi Ibrahim,Alassod Ghrood,Alassod Rasha
In this study, we successfully fabricated biocomposite monoliths using a facile, cost-effective, and friendly method via the thermally induced phase separation method using Polystyrene, Lignin, and OV-POSS. The properties of the prepared composites were estimated using Fourier transform infrared measurement (FTIR), scanning electron microscopy (SEM), and thermogravimetric analyzer (TGA). Furthermore, wettability properties were studied using water and oil. FTIR analysis indicates Polyester, Lignin, and OV-POSS were physically blended. The investigation by SEM showed the successful merging of components. Moreover, it revealed that OV-POSS nanoparticles acted as a support for reduced surface roughness. TGA measurements revealed that thermal stability was much better with increased OV-POSS loading. OV-POSS modified monolith exhibited hydrophobic with water contact angles of more than 130°. Results indicate that the produced monolith has a good sorption behavior to oils and organic liquids, whereas PL10L-0.3P showed higher sorption capacities followed by PL10L-0.1P, PL10L, and PL, respectively. The performance of the monoliths on oil/water separation was investigated through the selective removal of oil or organic solvent from water. Hence, the monoliths showed high separation efficiency above 90% and good reusability. The analysis showed that the adsorption for the oil and solvent process followed the pseudo-second-order model with a linear regression coefficient ( R 2 ) of > 0.999. The equilibrium data fit well with the Langmuir model. Besides, thermodynamic parameter analysis results showed that the adsorption was spontaneous and endothermic. An economic study examining the obtained resulted in a rate of investment (ROI) of 38.12%, a breakeven point (BEP) of 44.70%; this research is expected to be useful for the monolith industry that has attractive potential in practical industrial water treatment. Graphical abstract
研究领域:
材料科学
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环境工程
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纳米技术
·
高分子科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
En-Ze Deng,Qijie Mo,Yuying Li,Zongwen Mo,Li Zhang,Jiewei Liu
Although Z-scheme heterojunction composites have been widely studied in photocatalysis, in-depth investigation of oxygen vacancies (Ov) in the Z-scheme photocatalysts is still rare. Herein, an oxygen vacancies modified NU-1000/BiOCl-Ov composite with Z-scheme heterojunction was rationally designed and fabricated. The combination of X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) experiment verified the presence of oxygen vacancies, meanwhile the Z-scheme charge transfer across the heterojunction interface was confirmed in detail by the in situ -XPS, Kelvin probe force microscope (KPFM) studies, ultraviolet photoelectron spectroscopy (UPS), EPR radical capture experiment, as well as density functional theory (DFT) calculation. Importantly, compared to pristine NU-1000 and BiOCl, the optimized NU-1000/BiOCl-Ov composite displayed enhanced photocatalytic performance in the degradation of tetracycline hydrochloride (TCH) under visible light (λ ≥ 400 nm). Theoretical calculations reveal that the oxygen vacancies could induce electron redistribution, facilitating the activation of O 2 and TCH molecules, thereby promoting the photodegradation efficiency. Moreover, mechanism studies suggested that the synergistic effect of oxygen vacancies and Z-scheme heterojunction could facilitate the effective separation of photogenerated carriers. At last, the degradation routes of TCH were proposed and the toxicity of degradation intermediates was assessed. This work underlines the cooperative functions of oxygen vacancies and Z-scheme heterojunction towards improved photocatalytic performance, which offers new perspectives on the design of metal–organic frameworks (MOFs) composites for efficient photocatalysis.
研究领域:
材料科学
·
环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Lixin Zhang,Zhengxuan Zhu,Wei Tan,Jiawei Ji,Yandi Cai,Qing Tong,Yan Xiong,Haiqin Wan,Lin Dong
Strong metal–support interactions (SMSIs) have a significant effect on the performance of supported noble-metal catalysts for volatile organic compound (VOC) elimination. Herein, the strength of the SMSI of Pt/OMS-2 between Pt and the OMS-2 support is regulated by simply changing calcination temperatures, and the catalyst calcined at 300 °C (Pt/OMS-2-300) performs the best in the catalytic combustion of toluene. Through systematic structural characterizations, it is revealed that much more Pt2+–Ov–Mnδ+ species are formed in Pt/OMS-2-300, which can help facilitate the generation of more reactive oxygen species and promote lattice oxygen mobility. Moreover, the results of in situ DRIFTS experiments further confirm that abundant Pt2+–Ov–Mnδ+ species at the Pt–MnO2 interface on Pt/OMS-2-300 can better enhance the adsorption and activation of toluene, thus boosting the catalytic performance in toluene combustion. This newly developed strategy of thermal-driven regulation of the SMSI provides a novel perspective for constructing highly efficient catalysts for VOC emission control.
研究领域:
催化化学
·
环境科学
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DOI
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
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制氢技术
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材料科学
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表面化学
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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）