ChemCatChem
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2021
·Vol. 13
·期 15
·3490-3500
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IF 5.686
Mingwei Wu,Wenzhi Li,Xia Zhang,Fengyang Xue,Tao Yang,Liang Yuan
Graphical Methane combustion : Defect-Rich CeO 2 −Al 2 O 3 supported palladium catalysts can prominently improve the dispersion of palladium species and strengthen the concentration of active surface oxygen species, resulting in excellent catalytic activity for methane combustion. In heterogeneous catalysis, the strong interaction between metal and support can significantly modulate the electronic properties of the metals and play a crucial role in metal particle dispersion and morphology. Herein, a facile strategy was utilized to fabricate highly dispersive palladium catalysts supported on defective Al 2 O 3 −CeO 2 for lean methane oxidation. Ceria was immobilized on the coordinatively unsaturated Al 3+ penta sites of γ-alumina activated by pre-reduction to fabricate hybrid-oxide support (abbreviated as RAl 2 O 3 −CeO 2 ), and then Pd precursor was uniformly deposited on the defective surface. Such a RAl 2 O 3 −CeO 2 interface can effectively upgrade the dispersion of deposited palladium species and improve the concentration of reactive oxygen species owing to strong electronic interactions, invoking a superior catalytic activity for lean methane oxidation. After loading 1.0 wt% palladium, Pd/RAl 2 O 3 −CeO 2 exhibited a 90 % methane conversion at 328 °C under the space velocity of 60,000 mL g −1 h −1 , far lower than that of bare 1.0 wt% Pd/RAl 2 O 3 (400 °C). In addition, Pd/RAl 2 O 3 −CeO 2 catalyst showed an excellent hydrothermal stability under the harsh conditions (600 °C, water vapor)for 120 h without obvious deactivation. The reaction pathway of total methane combustion was elucidated by in situ DRIFTS. The crucial intermediate compositions (carbon oxygenates and carbonate)on Pd/RAl 2 O 3 −CeO 2 surface are more readily oxidized into CO 2 and H 2 O. This work provides an effective interface-promoted strategy to develop efficient and durable palladium catalysts for many challenging reactions.
研究领域:
催化化学
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材料科学
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环境工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Min-Ping Zhu,Jia-Cheng E. Yang,Xiaoguang Duan,Shaobin Wang,Darren Delai Sun,Baoling Yuan,Ming-Lai Fu
Immobilizing metal-organic frameworks in macro-supports to form three-dimensional catalysts holds a great promise in environmental remediation, however quantitative structure/property-catalytic activity relationship remains unknown currently. In this work, we constructed Co 2 AlO 4 /CoAl 2 O 4 @Al 2 O 3 monoliths derived from ZIF-67@γ-Al 2 O 3 pellets and systematically investigated their surface chemistry-activity relationships in peroxymonosulfate (PMS) activation for organic degradation. The activities of Co 2 AlO 4 /CoAl 2 O 4 @Al 2 O 3 catalysts were selectively correlated with their ratios of Co 3+ /Co 2+ and O Defect /O Lattice . The optimized Co 2 AlO 4 /CoAl 2 O 4 @Al 2 O 3 demonstrated an excellent catalytic efficacy toward PMS activation for metronidazole removal in a wide pH range (3.29–10.26) and OH was the dominant oxidant for metronidazole oxidation. The catalyst also exhibited desirable performance for eliminating other emerging contaminants and enduring catalytic activity and stability in PMS activation without regeneration. This study provides new prospects in rational design of robust, cost-effective and self-cleaning/repairing three-dimensional Co-based macroscale-catalysts with an outstanding and lasting catalytic activity for water purification.
研究领域:
环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Weimeng Zheng,Zhongyue Zhang,Nannan Liu,Qingyu Li,Jianbo Sun
The construction of heterogeneous structures could boost the performance of materials in gas sensing applications since the interface may enhance charge transfer. However, appropriate design and containable synthesis methods of heterogeneous structures with high-quality interfaces remain challenging. In this paper, heterolayered SnO2/SnSe nanosheet composites were prepared by regulating the alkali concentration to control the self-assembly rates of SnSe nanosheets while forming defect point oxidation. Heterolayered SnO2/SnSe nanosheets were synthesized by a one-step hydrothermal method and then used as a highly sensitive sensor for the detection of NO2 at room temperature. The as-obtained SnO2/SnSe materials were characterized using scanning electron microscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and I–V polarization to analyze the relationships between the heterogeneous structural morphology, crystallography, chemical components, electrical properties, and sensitivity mechanism. The results showed that the SnO2/SnSe-0.4 sample was prepared by the one-step hydrothermal method at the NaOH concentration of 0.04 mol/L. The SnO2/SnSe-0.4 sensor showed great sensitivity and higher selectivity to 1 ppm NO2 (resistance ratio = 7.8) at room temperature, roughly 7.1 and 2.7 times higher than that of pure SnSe and SnO2, respectively. In addition, the sensor exhibited a lower detection limit of 0.1 ppm. The improved sensing performance could be attributed to the large number of P–N heterojunctions of the SnO2/SnSe-0.4 material, enhanced interface charge transfer, and increased defect point oxidation in the material surface. The experimental results showed that SnO2/SnSe-0.4 is a very promising room-temperature NO2 gas sensing material, providing guidance for the rational design of heterogeneous structural sensors.
研究领域:
材料科学
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传感器技术
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纳米材料
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产品关联
DOI
高影响因子
MOLECULES
·
2021
·Vol. 26
·期 15
·4517
·
IF 4.412
Ye Tian,Qi Wang,Zhijian Peng,Shundong Guan,Xiuli Fu
A novel product consisting of a homogeneous tin oxide nanowall array with abundant oxygen deficiencies and partial Ni-Sn alloying onto a Ni foam substrate was successfully prepared using a facile solvothermal synthesis process with subsequent thermal treatment in a reductive atmosphere. Such a product could be directly used as integrated anodes for supercapacitors, which showed outstanding electrochemical properties with a maximum specific capacitance of 31.50 mAh·g−1at 0.1 A·g−1, as well as good cycling performance, with a 1.35-fold increase in capacitance after 10,000 cycles. An asymmetric supercapacitor composed of the obtained product as the anode and activated carbon as the cathode was shown to achieve a high potential window of 1.4 V. The excellent electrochemical performance of the obtained product is mainly ascribed to the hierarchical structure provided by the integrated, vertically grown nanowall array on 3D Ni foam, the existence of oxygen deficiency and the formation of Ni-Sn alloys in the nanostructures. This work provides a general strategy for preparing other high-performance metal oxide electrodes for electrochemical applications.Keywords:integrated anode;supercapacitor;nanowall array;oxygen-deficient tin oxide;Ni-Sn alloys
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
·
IF 5.723
Longyu Xu,Shuya Hua,Jing Zhou,Yiqi Xu,Chunshan Lu,Feng Feng,Jia Zhao,Xiaoliang Xu,Qingtao Wang,Qunfeng Zhang,Xiaonian Li
Semi-hydrogenation of acetylene is one of the most promising methods to eliminate acetylene from ethylene / acetylene mixtures to avoid Ziegler−Natta polymerization catalysts being poisoned. Given that acetylene is always over-hydrogenated on conventional palladium-based catalyst, it is of great importance to facilitate the desorption of ethylene to enhance the ethylene selectivity. Herein, we report a simple method to anchor Pd by unsaturated penta-coordinated aluminum (Al 3+ penta ) on Al 2 O 3 (meso-Al 2 O 3 ). Characterized by 27 Al-NMR, XRD, HR-TEM, CO chemisorption and XPS, Pd/meso-Al 2 O 3 catalyst had a highly dispersion and unique electronic property of Pd, thus exhibiting a high ethylene selectivity (~83%) while the acetylene conversion is > 99%. Besides, the agglomeration of Pd is suppressed by the metal-support interaction (MSI) between Pd and meso-Al 2 O 3 support. Therefore, the preparation method of the catalyst is relatively simple and has certain commercial application prospects.
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
Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Wei Fen,Zhao Jiwu,Liu Yu-Chun,Hsu Yung-Hsi,Hung Sung-Fu,Fu Junwen,Liu Kunlong,Lin Wei,Yu Zhiyang,Tan Li,Lu Xue Feng,Feng Chengyang,Zhang Huabin,Wang Sibo
Lattice oxygen-mediated photocatalytic ethane dehydrogenation represents a sustainable strategy for ethylene production, yet achieving a balance between high productivity, selectivity, and durability remains challenging. Here, we report a defective NiO-300 catalyst, where precisely engineered Ni vacancies activate lattice oxygen by weakening Ni–O bond and improving lattice oxygen mobility. This promotes efficient ethane activation and C–H bonds cleavage through photoinduced hole capture, intensifying ethane dehydrogenation via a light-boosted Mars-van Krevelen mechanism. The NiO-300 catalyst manifests a high ethylene yield of 604.5 μmol g −1 h −1 with 100% selectivity and stability over 200 cycles. In situ spectroscopic and theoretical studies elucidate the generation of active oxygen species, the evolution of Ni coordination, the formation of key intermediates, and the underlying photocatalytic mechanism. Our findings highlight cation vacancy engineering as a powerful tactic to fully activate lattice oxygen for solar-driven alkene production from alkane dehydrogenation over oxide photocatalysts.
研究领域:
催化
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材料科学
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化学工程
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物理化学
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Gels
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2025
·Vol. 11
·期 10
·783
·
IF 5.3
Jiefeng Yan,Zhenxing Fang,Jinxing Hu,Yangming Sun,Xinyi Huang,Guannan Zhou,Lu Li,Rui Wang,Yan Chen
Oxygen-deficient tungsten oxide W18O49was synthesized through lattice oxygen escaping at high temperature in N2atmosphere. The temperature and inert atmosphere were critical conditions to initiate the lattice oxygen escaping to obtain W18O49. The large amount of oxygen vacancies supports its performance in photothermal conversion. The synthesized tungsten oxides were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and ultraviolet-visible absorption spectroscopy (UV-Vis). The composite gel was fabricated by the insertion of oxygen-deficient tungsten oxide into PVA-based gel, which was cross-linked by glutaraldehyde. The PVA-based gel ensures a matched water supply speed with that of the evaporation rate due to its hydrophilic nature. The result of the solar steam generation shows that the W18O49-PVA gel (steam generation rate 2.65 kg m−2h−1) was faster than that of the pure PVA gel.
研究领域:
材料科学
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物理化学
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能源工程
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纳米材料
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光热治疗
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环境功能材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Wenquan Gu,Wanjun Wang,Guiying Li,Haojing Xie,Po Keung Wong,Taicheng An
Surface defect modulation has emerged as a potential strategy for promoting the photocatalytic activity of photocatalysts for various applications, while the impact of the oxygen vacancy on bacterial inactivation is still debated. In this study, oxygen vacancies were introduced to tungsten trioxide nanosheets (WO 3– x ) via a microwave-assisted route. The as-prepared WO 3– x nanosheets exhibited excellent visible-light-driven photocatalytic activity toward E. coli K-12 inactivation, and 6 log orders of the bacterial cells could be completely inactivated within 150 min. The obtained bacterial inactivation rate constant was 15.2 times higher than that of pristine WO 3 without oxygen vacancies, suggesting that the surface oxygen vacancy could significantly promote the bacterial inactivation efficiency. The mechanism study indicated that the inactivation of bacterial cells occurs via a direct h + oxidation pathway. In addition, the role of the oxygen vacancy was studied in detail; the oxygen vacancy was found to not only promote interfacial charge separation but also tune the band structure of WO 3 , thereby leading to increased h + oxidation power. Finally, a possible oxygen vacancy-dominated photocatalytic bacterial inactivation mechanism is proposed. This work is expected to offer new insights into the microwave-assisted synthesis of defective photocatalysts and the use of the oxygen vacancy for promoting photocatalytic antibacterial activities.
研究领域:
材料科学
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光催化
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环境科学
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Qiuyao Jiao,Yan Liu,Ran Yu,Lei Li
For supported heterogeneous catalyst, metal-support interaction (MSI) is very important factors for catalytic performance. Commercial γ-alumina was reduced with hydrogen in advance, providing strong anchoring sites for metal (metal oxide) species. This research demonstrates the use of pre-reduced alumina as catalyst carrier to anchor metal Co species in FTS compared with unreduced one. The defective alumina supported catalyst displayed a supeior performance. The Co/RAl2O3-550 catalyst showed surprisingly high CO conversion of 56.0%, C5+ hydrocarbons selectivity of 93.2%, and a low methane selectivity of 2.7% at a remarkable high activity (CTY = 1.1 × 10-5 molCO gCo-1 s−1). It revealed the strong reduction of alumina generated more defective sites, which was strongly anchored with metal cobalt species under MSI. Besides, the reduction of alumina also boosted the number of surface L-acidity, promoting the CO absorption rate through CO dissociation. These results reveal the unique property of defective Al2O3 supported cobalt catalysts, and provide a practical strategy to explore stable and efficient FTS catalysts.
研究领域:
催化化学
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材料科学
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化学工程
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
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