Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 19
·9813-9824
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IF 11.301
Yue Li,Jian Song,Mengting Jiang,Mbage Bawa,Xiaohong Wang,Yuyang Tian,Guangshan Zhu
Na5[IMo6O24]·3H2O and a porous aromatic framework (iPAF-1) were used to build an off-the-shelf building material (IMo6@iPAF-1) to realize the highly efficient oxidation of organic sulfurs like oxygenase. The synergy between IMo6 and iPAF-1 resulted in a higher BET surface area, hydrophobic microenvironment, and redox sites to show higher activity in aerobic oxidative desulfurization with almost 100% removal of model organic sulfurs under atmospheric pressure with almost 246 times higher TOFs compared to IMo6. It also showed efficiency in the desulfurization of gasoline and diesel to give very low S contents of 7.1 and 7.6 ppm with 99.3% and 99.4% removal, respectively, at 100 °C for 6 h. More importantly, IMo6@iPAF-1 could also catalyze desulfurization using concentrated O2 mixed with N2 or air instead of pure O2 with better safety and economics, while as low as 4.9 and 6.9 ppm S contents were achieved for gasoline and diesel, respectively. The special surroundings of IMo6@iPAF-1 repelled the sulfone product and allowed it to perform with the same efficiency when recycled without any treatment of the used catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Yong Liu,Ni Tan,Jinrui Guo,Jianlong Wang
In this study, a novel Al°-CNTs-Cu 2 O composite, capable of activating O 2 to generate H 2 O 2 and further to reactive oxygen species (ROSs) at a wide pH range, was synthetized, characterized and applied for the degradation of sulfamerazine. In the activation of O 2 by Al°-CNTs-Cu 2 O composite, H 2 O 2 was generated from the reaction of O 2 with Al°-CNTs, which could be catalytically decomposed into O 2 − and OH by Cu 2 O, the formed Cu(II) could be rapidly reduced to Cu 2 O by Al°-CNTs in composite, which made Al°-CNTs-Cu 2 O composite reusable and decreased the leaching of copper ions into solution. The removal efficiency of SMR and TOC was 73.91 % and 56.80 %, respectively at initial pH = 5.8, T = 20 °C, O 2 flow rate = 100 mL/min, Al°-CNTs-Cu 2 O dosage = 2 g/L, SMR = 50 mg/L, and reaction time = 60 min. The removal efficiency of SMR kept almost unchanged and the concentration of copper ions in solution was below 0.5 mg/L. The Al°-CNTs-Cu 2 O/O 2 process could be used as a novel catalyst for the degradation of refractory organic contaminants in water and wastewater by Fenton-like process at a wide pH range through the in situ generation of H 2 O 2 .
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 27
·11808-11816
·
IF 3.288
Shi-Yuan Zhang,Jing-Jing Ma,Hong-Lin Zhu,Yue-Qing Zheng
Syngas, as a necessary feedstock dependent on non-renewable fossil fuels, is a mixture of CO and H2, which could be prepared by a renewable strategy via electrochemical CO2 reduction in water electrolyte solutions. Herein, beaded Au@Co3O4 nanowire arrays (denoted as Au@Co3O4 NAs) were obtained by immersion in HAuCl4 solution with Co3O4 nanowire arrays. The Au@Co3O4 NAs exhibited outstanding electrochemical performance of producing syngas via tuning from 1 : 1 to 4 : 1 with controlling voltage. In addition, the Au@Co3O4 NAs showed better catalytic performance for the oxygen evolution reaction with an overpotential of 320 mV at a current density of 50 mA cm−2, along with a small Tafel slope of 75 mV dec−1 in 1 M KOH solution. The electrochemical performance of Au@Co3O4 NAs is obviously superior to Co3O4 NAs, which will open up a viable strategy for the design and fabrication of a bi-functional electrocatalyst for the overall reaction (CO2 + H2O → CO + H2 + O2).
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
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Journal of Materials Chemistry A
·
2015
·Vol. 4
·期 4
·1399-1407
·
IF 7.443
Guangyu Zhao,Li Zhang,Jixian Lv,Changle Li,Kening Sun
Hydrothermal self-assembly is a highly efficient and low cost method to prepare graphitic foam from graphene oxides; however, the self-assembly frameworks usually do not have controllable pore structures because of the spontaneous process. In this paper, a hydrothermal synthesis assisted by ammonium peroxo-polymolybdate [(NH4)2Mo2O11] tailoring to fabricate graphitic foam is presented. The foam possesses pore structures which can be controlled by adjusting the rate of charge in the hydrothermal experiments. Furthermore, the foam obtained from a definite rate of charge [(NH4)2Mo2O11 : graphene oxide is 1 : 2 in weight] has a hierarchical pore structure and a through-hole net. In electrochemical energy storage, such unique features are beneficial for providing efficient mass transport as well as abundant, accessible active sites. The graphitic foam was tested for use as self-supported electrodes of Li–O2 batteries (LOBs) and Li ion batteries (LIBs) without any metallic current collectors or organic binders, and the foam frameworks exhibited remarkable lithium ion storage properties in both of the two batteries (e.g., 5500 mA h g−1 at 0.2 A g−1 as LOB cathodes and 250 mA h g−1 at 50 A g−1 as LIB anodes).
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xiang Yu,Yuwei Mi,Zihan Gong,Yongfang Zhang,Lei Wang,Suyuan Zeng
Constructing heterojunctions is an effective strategy for increasing semiconductor photocatalytic activity. Herein, a Bi2O3/Bi4O5Br2 type-II heterojunction was synthesized using a simple one-pot solvothermal route. The 0-dimensional (0D) Bi2O3 nanoparticles are uniformly distributed within the 2D Bi4O5Br2 nanosheets with (101̅) facets dominantly exposed. In comparison with pure Bi2O3 and Bi4O5Br2, they show higher photocatalytic activity degradation of resorcinol (RO) and Rhodamine B (RhB). The Bi2O3/Bi4O5Br2 composite containing 10% Bi2O3 (BOB4) displays the best photocatalytic activity. For instance, compared with pure Bi4O5Br2 and Bi2O3, the k(RO) values of BOB4 (0.58 h–1) are 3.1 and 4.8 times higher. The enhanced photocatalytic activity is attributed to the formation of a large heterojunction interface that results from the homogeneous distribution of Bi2O3 nanoparticles in the Bi4O5Br2 nanosheet, which effectively enhances the photogenerated charge separation in a type-II mode. Major active species include superoxide radicals (•O2–), hydroxyl radicals (•OH), and holes (h+). In addition, the Bi2O3/Bi4O5Br2 photocatalysts exhibit outstanding resistance to inorganic ions, pH, water matrix, as well as outdoor sunlight and favorable stability and biocompatibility. This work presents a simple method to construct Bi-based heterojunction architectures for photoactivity improvement.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
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Chemical Science
·
2024
·
IF 7.6
Yinglei Tao,Tao Wang,Xingyu Yu,Ke Gong,Hao Gong,Haixia Chen,Xiaoli Fan,Aidi Zhang,Xianli Huang,Kun Chang,Jianping He
Li–O2 batteries (LOBs) boast an exceptionally high theoretical energy density; however, the slow kinetics of the oxygen electrode reaction have been a significant hurdle in their advancement and practical application. In this study, a composite of bismuth oxyhalide heterojunction incorporated with metal–organic frameworks (MOFs) was engineered on carbon cloth (Zr-MOF/BiOIBr/CC) as an efficient bifunctional catalyst to enhance the oxygen electrode reaction in photo-assisted LOBs. Compared to Zr-MOF/CC, Zr-MOF/BiOIBr/CC significantly expands the light absorption spectrum of the catalyst. Furthermore, the built-in electric field in the heterojunction aids in the separation and directional movement of photogenerated carriers, thereby expediting the reaction kinetics of LOBs. Consequently, the photo-assisted LOBs with Zr-MOF/BiOIBr/CC as the cathodes display a discharge potential of 3.05 V, a low charge potential of 3.20 V, and an energy efficiency of up to 95.3%, and can sustain an extended cycle life of over 255 cycles. This study underscores the potential application of MOFs/semiconductor heterostructural materials in photo-assisted LOBs and offers insights into the systematic design of photo-assisted air batteries and other advanced semiconductors.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 8
·4880-4889
·
IF 12.732
Wei Wu,Wang Lin,Hongjiang Chen,Keyan Wei,Zhitong Li,Haitao Yang,Mingxian Liu,Huaicheng Xiang,Libo Deng,Lei Yao
The development of high-performance solid-state batteries (SSBs) that integrate high safety with high energy density has long been pursued. However, conventional lithium-containing anode materials are unable to balance these two requirements, thereby necessitating the exploration of lithium-free anodes for SSBs. In the current study, a core–shell lithium-free α-Fe2O3@TiNb2O7 (TNO) nanofiber composite is synthesized and applied as an SSB anode. The confinement effect from the hollow TNO nanotubes on the encapsulated α-Fe2O3 nanoparticles can buffer the volume-change crushing during charging/discharging, leading to robust structural stability. Moreover, the high rate capability of TNO and high capacity of α-Fe2O3 work synergistically to provide superior electrochemical performances. The prepared α-Fe2O3@TNO composite delivers twice the reversible capacity (625 mA h g−1 at 0.1 A g−1) of pristine TNO as well as a remarkably prolonged cycle life (500 cycles with 79.2% capacity retention) and an improved rate performance (305 mA h g−1 at 3 A g−1) compared with those of α-Fe2O3, making this composite the most efficient TNO-based anode material ever reported. By pairing the composite with the high-energy Li[Ni0.8Co0.1Mn0.1]O2 (NCM811) cathode, the SSB full cell exhibits a high energy density of 400 W h kg−1. These results demonstrate the feasibility and great potential of the proposed lithium-free anode material in SSBs for practical applications.
研究领域:
材料科学
·
电化学
·
能源存储
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Catalysts
·
2025
·Vol. 15
·期 6
·545
·
IF 4
Xiaohong Yao,Jian Zhang,Chao Long
This study explored how pore size engineering in Nb-Mn/MCM-41 catalysts affects plasma-catalytic toluene oxidation. Adjusting the pore diameter (2.49–3.98 nm) modulated metal-support interactions and oxygen dynamics, with pore expansion to 3.73 nm (M3) optimizing the Mn4+/(Mn2++ Mn3+) ratio (XPS: 36.8%), the amount of lattice oxygen species (O2-TPD: 0.222 mmol/g), and crystallite size control (1.5 ± 0.2 nm, TEM). Smaller pores (M1: 2.49 nm) enhanced toluene adsorption but limited active site accessibility, while oversized pores (M4: 3.98 nm) reduced oxygen storage capacity (0.600→0.412 mmol/g). The Nb-Mn/M3 catalyst achieved superior performance with 96.8% toluene conversion, 55.0% CO2selectivity, and 85.4% carbon balance, while minimizing organic byproducts (GC-MS). Mechanistic studies revealed pore-mediated oxygen storage-transport cycles as critical for decoupling adsorption and oxidation steps. This study reveals fundamental mechanisms linking pore architecture to plasma-catalytic synergy in toluene oxidation, offering critical insights for the systematic design of energy-efficient, plasma-catalytic systems targeting industrial VOCs remediation.
研究领域:
催化化学
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环境化学
·
材料科学
·
等离子体化学
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纳米技术
·
表面科学
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tong Zhou,Guohui Dong,Jiahao Geng,Kai Han,Chenyang Xiao
In this study, a novel Z-scheme + II-type ternary heterojunction nanocomposite was prepared by one-step solvothermal method using g-C 3 N 4 , FeS 2 and Fe 2 O 3 as raw materials. The successful preparation of this ternary heterojunction was confirmed by the structural analysis and the surface morphology study. Compared with g-C 3 N 4 , the ternary photocatalyst showed excellent photocatalytic performance for the degradation of tetracycline (TC). The enhancement of photocatalytic activity is mainly due to the increase of light absorption capacity, effective separation of carrier in space, and increase of electron transfer channels in this Z-Scheme + II-type composite system. The scavenger test and electron spin resonance spectroscopy show that O 2 − is the main oxidizing free radical in the photocatalytic system. Based on liquid chromatograph-mass spectrometer, a possible degradation pathway of TC was proposed. This study opens up a new idea for the design and synthesis of efficient Z-Scheme + II-type photocatalysts for environmental purification.
研究领域:
环境科学
·
材料科学
·
化学
·
光催化
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Catalysis Science & Technology
·
2025
·
IF 4.2
Yu-Le Wang,Songhai Wu,Yu-Zhen Xu,Yu-Dong Shan,Yong Liu,Xu Han
The selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) using O2 remains challenging due to low epoxidation selectivity. In this work, a series of Mo-doped TS-1 (Mo-TS-1) catalysts were successfully synthesized for the epoxidation of Cy under solvent- and initiator-free conditions with O2 as the oxidant. Among them, 5Mo-TS-1 exhibited high catalytic performance, achieving 43.5% Cy conversion and 50.6% selectivity toward Cy-ep. Additionally, valuable byproducts such as 2-cyclohexen-1-ol (Cy-ol) and 2-cyclohexen-1-one (Cy-one) were obtained with yields of 28.0% and 21.4%, respectively. Since both Cy-ol and Cy-one are valuable intermediates in fragrance synthesis, over 43.5% of Cy was effectively converted into high-value products. Quenching experiments and Raman spectroscopy revealed that surface oxygen vacancies (Ov) facilitate the activation of O2 to form ≡Ov‑superoxo species, which abstract hydrogen from the allylic C-H bond of Cy to generate 3-cyclohexenyl radicals (Cy•). These radicals subsequently react with O2 to form Cy-OO•, followed by hydrogen abstraction from another Cy molecule to yield 2-cyclohexene-1-hydroperoxide (Cy-OOH). A positive correlation between Cy-OOH and Cy-ep formation underscores the critical role of Cy-OOH in the epoxidation process. Furthermore, Raman spectroscopy confirmed the presence of ≡Mo-(η2-O2) peroxo species on the catalyst surface, which preferentially attack the C=C bond of Cy to form Cy-ep. DFT calculations elucidated two distinct O2 activation pathways: In Pathway I, O2 is activated at Ov sites to form ≡Ov‑superoxo, which subsequently reacts with Cy to generate ≡Ov‑peroxo, Cy-OOH, and Cy•. In Pathway II, Mo(V/VI) sites either directly activate O2 or react with peroxo intermediates (≡Ov‑peroxo or Cy-OOH) to form ≡Mo-(η2-O2). This species selectively epoxidizes the alkene bond in Cy to Cy-ep. Notably, the direct activation of O2 at Mo(V/VI) sites bypasses the allylic oxidation route, thereby enhancing the epoxidation selectivity beyond the theoretical limit of 50.0%. This study provides new insight on the importance of surface superoxo and peroxo mediated by Ov and Mo(V/VI) in the epoxidation processes.
研究领域:
催化化学
·
材料化学
·
绿色化学
·
多相催化
·
氧化反应
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