Molecular Catalysis
·
2021
·
IF 5.062
Jiarong Li,Zhe Liu,Guangfa Hu,Ruimin Gao,Ronglan Zhang,Jianshe Zhao
A series of hybrid catalyst PMoW@HKUST-1@ZSM-5-MCM-41 was prepared in which H 3 PMo 6 W 6 O 40 were supported in the pore of micro/mesoporous materials ZSM-5-MCM-41 and HKUST-1 by one-pot method. Five types of ZSM-5-MCM-41 were prepared and corresponding ODS catalysts PMOW@HKUST-1@ZSM-5-MCM-41 were synthesized. The prepared catalysts were characterized and the most efficient catalyst was selected by XRD, FT-IR, UV–vis, N 2 adsorption-desorption, SEM, TEM. The removal of DBT reached 98.13 % by using PMoW@HKUST-1@ZSM-5-MCM-41−2 under 60 °C with molecular oxygen as oxidant after 150 min. After desulfurization, the catalyst can be simply recovered and reused 7 times with an unnoticeable decrease in catalytic activity, indicating the successful combination of heteropolyacids and micro/mesoporous materials for desulfurization.
研究领域:
化学工程
·
催化材料
✓ 已验证
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Ruijie Zhu,Leilei Kang,Lin Li,Xiaoli Pan,Hua Wang,Yang Su,Guangyi Li,Hongkui Cheng,Rengui Li,Xiao Yan Liu,Aiqin Wang
Catalytic oxidation is a commonly employed technology in the industry for removing volatile organic compounds (VOCs) due to its exceptional efficiency under mild operating conditions. Although supported Pt-based nano-catalysts are recognized widely as one of the most promising and extensively used industrial catalysts for VOC abatement, their practical application, and development are restricted by their exorbitant cost. Single-atom catalyst (SAC) with maximized metal utilization and exclusive electronic character has been explored extensively in various catalytic reactions. However, Pt SAC is usually deemed to be inactive in hydrocarbon oxidation reactions in thermal catalysis, compared with its nanoparticle counterpart. Here, we demonstrate that the WO 3 -TiO 2 supported Pt SAC (Pt 1 /WO 3 -TiO 2 ) exhibits much higher activities than the corresponding nanoparticle catalyst (Pt NP /WO 3 -TiO 2 ) in photo-thermo catalytic oxidation of C 3 H 8 and C 3 H 6 , which represent different kinds of typical VOCs. A key finding is that the activities of Pt 1 /WO 3 -TiO 2 and Pt NP /WO 3 -TiO 2 can be accelerated in photo-thermo catalytic C 3 H 8 oxidation by overcoming oxygen poisoning. Upon the light irradiation, the apparent active energy ( E a ) of the Pt 1 /WO 3 -TiO 2 and Pt NP /WO 3 -TiO 2 decline from 116 to 60 kJ·mol −1 and from 103 to 30 kJ·mol −1 , respectively, substantiating their effectiveness in photo-thermo catalysis. Notably, a substantially higher reaction rate of 3792 μmol∙g Pt −1 ∙s −1 on the Pt 1 /WO 3 -TiO 2 is achieved, which should be a benchmark for C 3 H 8 oxidation. More intriguingly, photo-thermo catalytic C 3 H 6 oxidation on the Pt NP /WO 3 -TiO 2 is prohibited due to the strong adsorption-induced C 3 H 6 poisoning on the Pt nanoparticles, for which the E a of the Pt NP /WO 3 -TiO 2 catalyst for C 3 H 6 oxidation is maintained at approximately 55 kJ·mol −1 , regardless of the light irradiation. In comparison, the C 3 H 6 poisoning on the Pt 1 /WO 3 -TiO 2 can be mitigated by light illumination, where the E a of the Pt 1 /WO 3 -TiO 2 catalyst for C 3 H 6 oxidation dramatically reduced from 49 to 16 kJ·mol −1 , signifying that the high energy barrier of C 3 H 6 oxidation can be mediated by the light. Profiting from the apt affinity between C 3 H 6 and Pt single atoms, the photogenerated electrons accumulated on the Pt single atoms produce repulsive force towards the electron-rich C 3 H 6 molecules, which is conducive to the C 3 H 6 desorption from the Pt 1 /WO 3 -TiO 2 . Therefore, the Pt 1 /WO 3 -TiO 2 exhibits enhanced activity in photo-thermo catalytic C 3 H 6 oxidation. This study exemplifies that the advantages of SAC are not only saving the consumption of precious metals but also discovering new catalytic reactions on the account of the specific electronic characteristic. Download: Download high-res image (85KB) Download: Download full-size image
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 12
·892
·
IF 3.8
Yangzhou Deng,Yuqi Zhang,Kunkun Wei,Yue Wang,Shihui Zou,Juanjuan Liu
Advanced oxidation catalyzed by metal oxides is a promising approach for degrading organic pollutants in wastewater. A critical strategy to enhance the performance of these catalysts is optimizing the dispersion of their active components through innovative synthesis methods. In this study, we report a one-pot synthesis of g-C3N4nanomeshes supported with highly dispersed VO2catalysts (V-g-C3N4) for the advanced oxidation of methylene blue (MB). The characterization results reveal that the involvement of VCl3in the pyrolysis of melamine facilitates the formation of g-C3N4nanomeshes with abundant amino groups (NH/NH2). The strong interaction between vanadia species and amino groups prevents VO2particles from agglomerating, resulting in a significantly higher vanadia dispersion than V-g-C3N4-im synthesized via the traditional impregnation method. V-g-C3N4exhibits a sophisticated microstructure and surface structure, which leads to a rate constant 2.3-fold higher than V-g-C3N4-im in the catalytic degradation of methylene blue using H2O2as the oxidant. X-ray photoelectron spectroscopy, trapping experiments, and electron paramagnetic resonance measurements reveal that the rapid adsorption and fast diffusion of MB over g-C3N4nanomeshes, together with the efficient H2O2activation into ·OH radicals via the V4+/V5+redox cycle, synergistically contribute to the superior MB removal efficiency of V-g-C3N4. Moreover, V-g-C3N4demonstrates no significant decrease in activity even after the fourth cycle, indicating its excellent stability during the pollutant removal process.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Qiang Zhao,Dandan Li,Guofeng Gao,Wen Yuan,Genyan Hao,Jinping Li
We describe a novel nanostructured iron oxide catalyst film electrodeposited from iron(II) triflate under mild conditions (room temperature, atmospheric pressure, and near-neutral solution) that can catalyze water oxidation in potassium carbonate solution. The structure, morphology, composition, and catalytic activity of the catalyst were characterized by X-ray diffractometry, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical measurements. The results indicate that nanostructured iron oxide is an active electrocatalyst for water oxidation at higher catalytic current and low overpotential.
研究领域:
无机化学
·
材料科学
·
电化学
·
能源化学
·
纳米科技
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 11
·2644-2658
·
IF 7.779
Xiaoyan Yang,Xiaoling Zeng,Xing Ming,Li Yang,Alberto J. Fernández-Carrión,Sihao Deng,Lunhua He,Xiaojun Kuang
BiVO4 scheelite is one of the few tetrahedra-based structures able to display vacancy-mediated oxide-ion conduction upon the use of an acceptor-doping strategy, leading to oxide-ion migration. In order to modulate the ionic migration process, it is of utmost importance to understand the different parameters affecting it. Here we review phase formation, oxygen vacancy stabilization, and migration for a wide variety of acceptor metal dopants in scheelite BiVO4. Among them, Ca2+-doped materials present the widest solid-solution range, leading to optimized oxide-ion conductivities at moderately high temperatures (σb: ∼10−3 S cm−1 at 500 °C), mainly as a result of their smaller size mismatch with Bi3+ and lower oxygen vacancy defect energy. The results gathered herein provide a useful guide for designing new oxide-ion conductors and tailoring oxide conductivity through the proper selection of doping agents according to several criteria, such as the oxygen defect formation energy, atom size mismatch, polarizability, and bond-dissociation energy with oxygen.
研究领域:
材料科学
·
无机化学
·
固体离子学
·
能源材料
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电化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2017
·Vol. 4
·期 11
·1791-1797
·
IF 4.036
Jiangli Meng,Jiaqi Fu,Xiaoxuan Yang,Meijie Wei,Song Liang,Hong-Ying Zang,Huaqiao Tan,Yonghui Wang,Yangguang Li
The development of stable, highly active and cheap electrocatalysts towards the oxygen evolution reaction (OER) has been an ongoing challenge due to practical problems such as slow kinetics and high overpotential. Herein, we utilized a one-pot hydrothermal method to prepare cobalt/nickel molybdate hierarchical microflowers on conductive carbon cloth (MMoO4-CC, M = Co, Ni) as three-dimensional self-supported electrodes for the oxygen evolution reaction. CoMoO4-CC showed better catalytic activity than NiMoO4-CC. Benefiting from the synergistic effect of a large active area, fast charge and mass transport as well as a three-dimensional conducting path, the CoMoO4-CC nanosheet electrode showed a large current density and a relatively low starting potential, delivering 10 mA cm−2 current densities at an overpotential of 290 mV and a Tafel slope of 94 mV dec−1. Furthermore, the CoMoO4-CC nanomaterial shows better electrocatalytic stability than IrO2-CCa, which could be a promising electrocatalyst for large-scale water oxidation.
研究领域:
电催化
·
材料科学
·
能源化学
·
电化学
·
纳米材料
✓ 已验证
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2022
·
IF 6.364
Qiankun Xu,Qingliang Shan,Jianbao Hu,Yewei Wang,Yu Wang,Qian Ma,Changrong Chen,Yuqian Zhou,Anze Shui
The oxidation property of SiC-B 4 C- x Al 2 O 3 ( x ranges from 0 wt% to 30 wt%) ceramics was studied in air at 1400 ℃. Results show that the porous oxide layer becomes dense and smooth with addition of Al 2 O 3 . When the content of Al 2 O 3 is proper, the DOP (degree of polymerization) of borosilicate network can be improved with increase of Al 2 O 3 content, inhibiting the migration of atoms and molecular groups. With that, the crystallization of SiO 2 and volatilization of B 2 O 3 can be restrained. When the content of Al 2 O 3 is excessive, the DOP of borosilicate network will be decreased, deteriorating the oxide layer morphology. It is believed that the damage of borosilicate network by excess Al 2 O 3 should be responsible for this phenomenon. In this research, the SiC-B 4 C ceramic with optimal oxidation resistant can be obtained when the content of Al 2 O 3 is 15 wt%.
研究领域:
材料科学
·
无机非金属材料
·
高温材料
·
表面工程
·
陶瓷学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Dandan Liu,Xueyan Li,You Li,Shu Yin,Jiajia Liu,Jiatao Zhang
Highly sensitive and selective gas sensors hold great potential in disease diagnosis. However, the rational design of non-noble-metal-based, high-efficiency sensing materials for trace gas detection remains a crucial challenge. Herein, a chemiresistive sensor that can detect parts per billion (ppb)-level acetone was realized based on three-dimensional (3D) α-Fe2O3/ZnO nanocages, which were achieved by a simple encapsulation and calcination process. In particular, we found that Fe species play an intriguing role in the evolution from Fe-ZIF-8 to heterogeneous α-Fe2O3/ZnO nanocages. α-Fe2O3 functionalization empowered the α-Fe2O3/ZnO nanocage-based sensor with a high response of 45.25, an ultrafast response (7 s) and recovery (6 s) time toward 50 ppm of acetone, a limit of detection (LOD) of 500 ppb, and superior selectivity. Moreover, in situ Fourier transform infrared analysis allowed one to devise of an acetone sensing mechanism for dissociative acetone adsorbed on the α-Fe2O3/ZnO nanocages, involving the first oxidation of acetone to form formate and acetate complexes, followed by further oxidation to CO2 and H2O. The enhanced acetone sensing performance can be attributed to the high specific surface area, abundant oxygen vacancies, well-tuned heterojunction, and optimal acid–base property.
研究领域:
材料科学
·
分析化学
·
生物医学工程
✓ 已验证
DOI
高影响因子
Environmental Chemistry
·
2023
·Vol. 20
·期 6
·235-248
·
IF 4.3
Hailiang Zhang,Long Jia,Yongfu Xu
Environmental context The process of ethylene ozonolysis is an essential source of CH2OO radicals, and the latter is an important oxidant for the atmospheric pollutant SO2. The accuracy of a widely used atmospheric chemistry model (Master Chemical Mechanism, MCM) in quantifying SO2 oxidation has not been evaluated. In this study, this accuracy was evaluated, and optimal parameters underpinned by data from smog chamber experiments.Rationale The oxidation of SO2 by CH2OO radicals in the ethylene-O3 system is one of the important pathways of sulfate aerosol formation, but the accuracy of Master Chemical Mechanism (MCM) simulation for this reaction was not evaluated, although the MCM has been widely used in previous studies.Methodology The oxidation of SO2 in the ethylene-O3 system was performed in detail under different conditions, which were used to evaluate the accuracy of MCM simulation for the reactions in this study.Results The experimental conditions of low RH and high initial SO2 concentration favour the SO2 oxidation in the ethylene ozonolysis, and the yield of CH2OO in the ethylene ozonolysis without irradiations was determined to be 0.43. The n-hexane (C6H14) oxidation intermediates can promote the SO2 oxidation rate by generating sulfur-containing organics in the aerosol water. The original MCM simulated SO2 consumption after 4-h reaction was more than 70% smaller than the measured results. By adjusting the yield of CH2OO and updating the reaction rate constants of CH2OO-related reactions (e.g. with SO2, H2O and organic acid), the difference between experiments and simulations decreased from 70% to 6.6%.Discussion The promotion effects of n-hexane on the oxidation of SO2 suggest that alkanes may be the precursors of sulfur-containing organics in the atmospheric environment. This study further confirms the effect of CH2OO on the oxidation of SO2 in the atmospheric environment and provides information on the performance of MCM simulation.
研究领域:
大气化学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2015
·
IF 2.002
Lei Chen,Zhichun Si,Xiaodong Wu,Duan Weng,Zhenwei Wu
A MnO x –NbO x –CeO 2 catalyst for low temperature selective catalytic reduction (SCR) of NO x with NH 3 was prepared by a sol–gel method, and characterized by NH 3 –NO/NO 2 SCR catalytic activity , NO/NH 3 oxidation activity, NO x /NH 3 TPD , XRD , BET, H 2 -TPR and in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The results indicate that the MnO x –NbO x –CeO 2 catalyst shows excellent low temperature NH 3 -SCR activity in the temperature range of 150–300°C. Water vapor inhibits the low temperature activity of the catalyst in standard SCR due to the inhibition of NO x adsorption. As the NO 2 content increases in the feed, water vapor does not affect the activity in NO 2 SCR. Meanwhile, water vapor significantly enhances the N 2 selectivity of the fresh and the aged catalysts due to its inhibition of the decomposition of NH 4 NO 3 into N 2 O.
研究领域:
环境催化
·
大气污染控制
·
材料化学
·
表面科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
·
2024
·
IF 3.4
Jianqiao Yang,Yining Ding,Fen Zhao,Shuzhong Wang,Yanhui Li,Donghai Xu
In this study, a Cr coating was fabricated on Ni-based alloys to prevent under-deposit corrosion. The effect of salt deposition on the structural integrity of the Cr coating in SCW environment with/without oxygen was investigated. Results show that the Cr coating kept its integrity after exposure in SCW environment, successfully avoided the metallic ions leaching from Ni-based alloys. The structure of the oxide layer after exposure is a thin Fe 2 O 3 or FeCr 2 O 4 layer and a Cr 2 O 3 layer. The oxidation rate of the Cr coating decreased to one third of the sample after exposure in the same environment without salt deposit layer, indicating that the inward mass-transfer of oxygen to the alloy surface was inhibited by the salt deposit layer. The volume expansion of the sample due to the growth of Cr oxide layer was restrained by the salt deposit layer, forming a growth stress in the coating.
研究领域:
材料科学
·
腐蚀科学
·
高温材料学
·
表面工程
·
能源材料
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2014
·
IF 2.871
Hao Li,Qingni Yu,Bin Yang,Zhongjian Li,Lecheng Lei
Galvanostatic anodic oxidation of artificial human urine (AHU) was carried out by using boron doped diamond (BDD) and IrO 2 electrodes respectively. It was found that organic compounds in urine could be almost completely mineralized in a few hours and ammonia may be oxidized into N 2 by the electro-catalytic process. However, the oxidation processes were highly dependent on the electrode materials. On the non-active BDD electrode complete oxidation occurred, and the final oxidation products of inorganic ions, including ClO 4 − and NO 3 − , were formed. Whereas on the active IrO 2 electrode, the final products generated and left in solution were highly toxic substances, including N 2 H 4 and NO 2 − , because the oxidizing activity on the IrO 2 electrode surface is relatively low. The pH values during the degradation process were monitored and the corresponding degradation mechanisms and pathways on both electrodes are proposed based upon the measured inorganic intermediates.
研究领域:
环境科学
·
电化学
·
水处理技术
·
生物医学工程
·
分析化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）