ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Yanyan Zhao,Zhen Wu,Yong Zhang,Bicheng Zhu,Jianjun Zhang
Photocatalytic oxygen reduction reaction (ORR) offers a mild and cost-effective approach for hydrogen peroxide (H 2 O 2 ) production. However, its practical application is significantly hindered by rapid charge carrier recombination and insufficient O 2 adsorption capacity in photocatalysts. To address these limitations, we developed a strategy involving the creation of S-vacancy-rich CdIn 2 S 4 (S v –CIS) to facilitate charge separation and subsequent deposition of Au nanoparticles on its surface (Au–S v –CIS) to strengthen O 2 adsorption. The results suggest that the optimized Au–S v –CIS achieves a significantly increased H 2 O 2 production yield of 2542 μmol·h·g −1 in 10%-ethanol/water solution, which is about 12.8 and 1.7 times higher than that of pure CIS and S v –CIS. Comprehensive characterizations including photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent response, electrochemical impedance spectra, and femtosecond transient absorption spectroscopy confirm the improved charge dynamics of Au–S v –CIS. In addition, temperature-programmed desorption of O 2 combined with density functional theory calculations conclusively demonstrates the superior O 2 adsorption capacity of Au–S v –CIS. This work provides a design strategy for efficient solar–to–chemical energy conversion through cooperative photocatalyst engineering.
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Nano Materials Science
·
2025
·
IF 17.9
Hongjing Liu,Shan Ren,Xiaodi Li,Liang Wang,Bofeng Bai,Shouning Chai,Peng Chen,Fan Dong
Photocatalytic oxidation of nitrogen oxides (NO x ) is a promising technology for environmental protection and green sustainable development. However, its practical application remains limited due to inefficient activation of NO and O 2 , stemming from inadequate structural design of photocatalysts. Herein, we developed a thin-layer two-dimensional (2D) material Bi 2 MoO 6 (BMO) via cetyl trimethyl ammonium chloride (CTAC) addition in synthesis process, which effectively modulates the surface electronic structure, enhance the light absorption and activation of NO and O 2 . This thin-layer Bi 2 MoO 6 nanosheets achieved a NO oxidation efficiency of 45.3 %, which was about 5.5 times that of traditional bulk BMO (8.2 %). Additionally, it demonstrated superior selectivity for NO 2 − /NO 3 − production (86.6 %) compared to bulk BMO (60.5 %) and significantly reduced the formation of toxic NO 2 byproducts (13.4 % vs. 39.5 %). Combining experimental characterizations and density functional theory (DFT) simulations, it demonstrated that the electron-hole pair separation could be promoted and targeted adsorption activation of O 2 can be enhanced to form superoxide radicals (•O 2 − ) and singlet oxygen ( 1 O 2 ) via the effect of surface charge transfer adjustment on the thin-layer structure of Bi 2 MoO 6 , which are key factors affecting the efficiency and selectivity of photocatalytic oxidation of NO. This work provides important insights into the formation of directed ROS and proposes a unique mechanism for selective NO oxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yixi Wang,Wenqing Xu,Zhi Liu,Yulong Shan,Wanrong Chen,Xinyu Zhang,Tingyu Zhu
Controlling both CO and NOx pollutants without additional cost is necessary but challenging, especially in industrial flue gas with complex components. Previous studies mainly focused on the effect of O 2 and SO 2 on the CO oxidation side reaction and valence state of Ir species on various catalysts, while neglecting the impact on NO conversion pathway. Herein, we propose an "ineffective reaction pathway" in the presence of O 2 with nitrate as an intermediate according to the results of in situ DRIFTS and DFT. And we also reveal the contribution of SO 2 in inhibiting the adsorption of O 2 and promoting the selective adsorption of NO and CO even at lower injection concentrations, based on the oxidation of SO 2 on Ir(111). This is quite a favorable characteristic for the treatment of industrial flue gas, resolving the long–standing dispute on the involvement of these components in the CO–SCR reaction. Under specific conditions (CO/NO=20, O 2 =5%, SO 2 =200 ppm) at 250 °C, the NOx conversion is as high as 78%. These results will contribute to the development of more efficient catalysts in the future for simultaneously controlling two pollutants (CO and NOx).
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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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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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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yang Zhan,Shun-zhi Yu,Shao-hua Luo,Jian Feng,Qing Wang
Transition-metal sulfides (TMS) are one of the most promising cathode catalysts for Li–O2 batteries (LOBs) owing to their excellent stabilities and inherent metallicity. In this work, a highly efficient mode has been used to synthesize Co@CNTs [pyrolysis products of metal–organic frameworks (MOFs)]-derived CoS2(CoS)@NC. Benefiting from the special yolk–shell hierarchical porous morphology, the existence of Co–N bonds, and dual-function catalytic activity (ORR/OER) of the open metal sites contributed by MOFs, the CoS2@NC-400/AB electrode illustrated excellent charge–discharge cycling for up to nearly 100 times at a current density of 0.1 mA cm–2 under a limited capacity of 500 mA h g–1 (based on the total weight of CoS2@NC and AB) with a high discharge voltage plateau and a low charge cut-off voltage. Meanwhile, the average transferred electron number (n) is around 3.7 per O2 molecule for CoS2@NC-400, which is the chief approach for a four-electron pathway of the ORR under alkaline media. Therefore, we believe that the novel CoS2@NC-400/AB electrode could serve as an excellent catalyst in the LOBs.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
Small Methods
·
2022
·Vol. 6
·期 6
·2200178
·
IF 15.367
Rui Xu,Phei Er Saw,Lei Xu
Two-dimensional (2D) nanomaterials have attracted increasing attention in cancer theranostics due to their ultrahigh specific surface area resulting in more radicals and/or reactive oxygen species (ROS) generation in chemodynamic therapy (CDT). However, their biomedical prospects are greatly limited by poor biocompatibility, low dispersion, weak stability, and the potential threat of their high immunogenicity. Moreover, rapid depletion of ROS by the high level of antioxidants (e.g., glutathione) in cancer cells severely limits the therapeutic effects of cancer CDT. Herein, a robust method is developed to improve the biomedical application of 2D nanomaterials via constructing a 2D nanomaterials delivery nanoplatform with hemoglobin-based minerals biological coat for the safe encapsulation, long blood circulation, and controlled release of 2D nanomaterials. After intravenous administration and then internalization by cancer cells, the acidic microenvironment and high concentration of H 2 O 2 can trigger rapid release of Cu-T nanoscale metal-organic frameworks (nMOFs) from Cu-T@MH. Then, the released Cu-T nMOFs with simultaneous high ROS production and GSH depletion endow the Cu-T@MH nanoplatform with enhanced cancer CDT. Besides, the fluorescence recovery of tetrakis(4-carboxyphenyl) porphyrin in Cu-T nMOFs during the GSH depletion process can accurately visualize the cancer therapeutic action.
研究领域:
生物医学工程
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肿瘤学
·
纳米医学
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PubMed
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Ziling Wang,Xianzhu Peng,Shuai Guo,Mingjie Sun,Junfang Cheng,Lu Zou,Bo Chi,Jian Pu
Catalysts with high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performances are crucial to the development of lithium-oxygen batteries (LOBs), which aim to promote Li2O2 deposition and decomposition and then avoid the active site passivation. Considering the metallic Ag possessing good electrical conductivity and excellent catalytic activity and perovskite oxides exhibiting high abundance, an easily tunable structure, and excellent intrinsically catalytic activity, we adopt the ultraviolet light to realize the deposition of Ag nanoparticles on the La0.6Sr0.4Fe0.9Mn0.1O3 (LSFM) substrate as a high-performance cathode for LOBs. The results confirm that the synergetic effect of Ag nanoparticle decoration and the La0.6Sr0.4Fe0.9Mn0.1O3 substrate could dramatically improve the electronic conductivity and ORR/OER kinetics of the nanohybrids. Ag@LSFM hybrids with abundant active sites and considerable electronic conductivity promote the deposition of a thinner discharge product film, and the corresponding LOBs deliver high discharge capacity (12 477 mAh g–1), a small gap between charge and discharge potentials (∼1.3 V), and high cycling stability (147 cycles). Overall, the study suggests that such a bifunctional catalyst is a promising candidate in LOBs.
研究领域:
材料科学
·
电化学
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 24
·8445-8457
·
IF 5.721
Kun Liu,Yichen Zhao,Jiale Wang,Qingsong Xue,Guofeng Zhao
The fabrication of qualified catalysts is a key issue to implement gas-phase aerobic alcohol oxidation but necessarily requires understanding the structures of catalytic active sites and the supply of active oxygen species. Herein, we present one example of the Ag–CoO/Ti- powder catalyst for gas-phase benzyl alcohol aerobic oxidation. The first interesting observation is that the Ag–Co3O4 ensembles on the fresh catalyst could be transformed into Ag–CoO due to the presence of reductive benzyl alcohol. The preferred catalyst with 3 wt% Ag and 3 wt% CoO exhibits 93% benzyl alcohol conversion and 99% benzaldehyde selectivity at a weight hourly space velocity of 20 h−1 and a temperature of 240 °C. The structures of Ag–CoO ensembles and oxygen species supply were probed and identified by electron microscopy and other spectroscopy techniques in combination with temperature-programmed thermal analyses, pulse experiments, and kinetic studies. In nature, the oxygen species is generated at the Ag–CoO interfacial sites in the form of atomic oxygen with appropriate chemisorption strength on these sites to achieve a high oxidation activity of benzyl alcohol. Moreover, the Co3O4 ↔ CoO cycle is promoted by Ag at low temperature such as 240 °C to endow the Ag–CoO ensembles with excellent catalytic performance.
研究领域:
催化化学
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材料科学
·
物理化学
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高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2017
·Vol. 34
·期 12
·3132-3141
·
IF 2.007
Zhang Wei,Li Xin,Wang Hong,Song Yongji,Zhang Shenghong,Li Cuiqing
Deep desulfurization of model oil by photocatalytic air oxidation and adsorption using Ti (1− x ) M
x
O 2 (M=Zr, Ce) was investigated. Ti (1− x ) M
x
O 2 (M=Zr, Ce) was prepared by urea gelation/co-precipitation method, and characterized by N 2 adsorption, XRD and UV-vis spectra. UV irradiation greatly enhanced the adsorptive capacity and selectivity of TiO 2 -ZrO 2 for organosulfur in model oil because organosulfur compounds were first photocatalytically oxidized to sulfoxides and sulfones over TiO 2 -ZrO 2 , which were then selectively adsorbed on the bifunctional material due to much higher polarities of generated sulfoxides and sulfones. The Ti/Zr molar ratio and calcination temperature were optimized to 5 : 5 and 500 °C with the sulfur removal of 99.6% after reaction for 2 h under UV irradiation. After adding 25 wt% toluene into model oil, the sulfur removal could still reach 97.2% after reaction for 7 h. TiO 2 -ZrO 2 could be well regenrated by washing with acetonitrile followed by thermal treatment in air.
研究领域:
化学工程
·
环境科学
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高影响因子
Frontiers in Chemistry
·
2019
·
IF 3.782
Song Hongbing,Liu Zong,Gai Hengjun,Wang Yongjie,Qiao Lin,Zhong Caiyun,Yin Xiangyang,Xiao Meng
Introducing electron-rich nitrogen atoms to ordered mesoporous carbons (OMC) as supports for noble metal catalysts, not only improves the hydrophilic properties of a mesoporous carbon surface, but also enhances the coordination and binding abilities of metal ion. In the present work, nitrogen-doped ordered mesoporous carbons (NOMCs) were successfully fabricated via a facile hydrothermal self-assembly. The prepared NOMCs were characterized through powder X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption-desorption isotherm. The analyses demonstrated that the NOMCs prepared at a pyrolysis temperature of 750°C possessed an ordered 2D hexagonal mesoporous structure, a high graphitization degree, large surface area, and a well-distributed pore size. In particular, NOMCs could anchor Pd nanoparticles uniformly because of the introducing N atoms with strong electronegativity, which were selected as efficient catalysts for the partial oxidation of benzyl alcohol to benzaldehyde. Approximately 24.63% conversion with 85.71% selectivity to benzaldehyde was obtained without using any solvent by molecular O2 oxidation. Most importantly, the TOF value of the catalyst in the reaction system was up to 8698 h−1. After five runs reaction, TOF and selectivity of the catalyst remained essentially same. Hence, the proposed catalyst has a potential engineering application value.
研究领域:
材料科学
·
催化化学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Feng Li,Yuhang Tian,Yanyun Sun,Peiyu Hou,Xianqi Wei,Xijin Xu
High-voltage and low-cost manganese-based P 2-type oxides show real promise as promising cathode for sodium-ion batteries (SIBs). But the P 2 − O2 phase transformation and Na + /vacancy ordering results in the inferior structural stability and Na + diffusion coefficient , which further leads to rapid decay of capacity and poor rate capability. Herein, in consideration of the synergetic effects of dual cationic doping, electrochemically inactive Li + and active Co 3+ codoping are proposed to solve the above issues. The novel two-step doping strategy, Co doping during synthesis of precursors via coprecipitation reaction followed by Li doping during solid-state reaction, are rationally developed. As anticipated, the Li/Co codoped P 2-type oxide exhibits the absence of P 2 − O2 phase transformation and Na + /vacancy disordering, which gives rise to an outstanding cycling stability (86.7% capacity retention within 100 cycles at 0.1C) and high-rate capability (reversible capacity of 109 mAh g −1 even at 10C). In addition, the full-cells composed of the codoped P 2-type positive and hard carbon negative show high energy-density, good lifespan and high-rate property. This proposed cationic codoping provides an effective and scalable tactics for modulating the structural properties of high-voltage P 2-type cathodes for advanced SIBs.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
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