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
✓ 已验证
DOI
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
·
材料科学
·
物理化学
✓ 已验证
DOI
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
✓ 已验证
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
✓ 已验证
DOI
PubMed
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
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yuan Meng,Jianguo Jiang,Aikelaimu Aihemaiti,Tongyao Ju,Yuchen Gao,Jiwei Liu,Siyu Han
Amine-functionalized sorbents are investigated widely for CO2 capture from flue gas, to mitigate the crisis of global CO2 emission, with the advantages of excellent adsorption and regeneration performance. However, the presence of O2 in flue gas (3–10%) would induce the degradation of the sorbents, and some previous works proposed the strategies at the sacrifice of partial CO2 adsorption capacity. Herein, we focused on the oxidation behavior of PEI-functionalized silica in the long-term operation and analyzed the degradation mechanism by characterizing the oxidized sorbents. The sorbent proved to be oxidative stable under a lower temperature of air exposure, but the oxidative degradation would indeed occur at more harsh temperatures (above 90 °C). This study demonstrated that CO2 capture from O2-containing flue gas was feasible by controlling the operating temperature (below 75 °C), and the effective capacity of above 135 mg/g could be maintained in the cyclic CO2 capture.
研究领域:
环境科学
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化学工程
·
碳捕集与封存（CCS）
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Qiong Yang,Peng-Fei Wang,Jin-Zhi Guo,Zi-Ming Chen,Wei-Lin Pang,Ke-Cheng Huang,Yu-Guo Guo,Xing-Long Wu,Jing-Ping Zhang
As a promising cathode material of sodium-ion battery, P2-type Na2/3Ni1/3Mn2/3O2 (NNMO) possesses a theoretically high capacity and working voltage to realize high energy storage density. However, it still suffers from poor cycling stability mainly incurred by the undesirable P2–O2 phase transition. Herein, the electrochemically active Fe3+ ions are introduced into the lattice of NNMO, forming Na2/3Ni1/3Mn2/3–xFexO2 (x = 0, 1/24, 1/12, 1/8, 1/6) to effectively stabilize the P2-type crystalline structure. In such Fe-substituted materials, both Ni2+/Ni4+ and Fe3+/Fe4+ couples take part in the redox reactions, and the P2–O2 phase transition is well restrained during cycling, as verified by ex situ X-ray diffraction. As a result, the optimized Na2/3Ni1/3Mn7/12Fe1/12O2 (1/12-NNMF) has a long-term cycling stability with the fading rate of 0.05% per cycle over 300 cycles at 5 C. Furthermore, the 1/12-NNMF delivers excellent rate capabilities (65 mA h g–1 at 25 C) and superior low-temperature performance (the capacity retention of 94% at −25 °C after 80 cycles) owing to the enhanced Na diffusion upon Fe doping, which is deduced by the studies of electrode kinetics. More significantly, the 1/12-NNMF also displays remarkable sodium-ion full-cell properties when merged with an LS–Sb@G anode, thus implying the possibility of their practical application.
研究领域:
材料科学
·
电化学
·
能量存储
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2017
·
IF 1.815
W.S. Huo,H. Zeng,Y. Yang,Y.H. Zhang
Enzymatic electrodes over-coated by thin film of nano-composite made up of polymer and functionalized nano-gold particle was prepared. Glucose/O 2 membrane-free enzymatic fuel cell based on nano-composite based electrodes with incorporated glucose oxidase and laccase was assembled. This enzymatic fuel cell exhibited high energy out-put density even when applied in human serum. Catalytic cycle involved in enzymatic fuel cell was limited by oxidation of glucose occurred on bioanode resulting from impact of sophisticated interaction between active site in glucose oxidase and nano-gold particle on configuration of redox center of enzyme molecule which crippled catalytic efficiency of redox protein.
研究领域:
生物化学
·
纳米生物学
·
能源科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 5
·459
·
IF 4
Dan Wang,Yanan Liu,Kun Wan,Danning Feng,Yan Pei,Minghua Qiao,Xiaoxin Zhang,Baoning Zong
The electrocatalytic reduction of O2via two-electron reaction (2e-ORR) to H2O2represents a promising alternative to the current anthraquinone process, since it is advantageous in the sustainable and decentralized production of H2O2. Herein, we report the development of oxygen and nitrogen-rich few-layered graphene-like materials (ms-dcda) by the one-step carbonization of biomass-sourced monosaccharides (D-glucose, D-fructose, D-galactose, D-ribose, D-xylose, L-arabinose, and D-mannose) with the aid of dicyandiamide for electrochemical O2reduction to H2O2. The ms-dcdamaterials were porous and possessed wrinkled morphology typical of graphene nanosheets. In H2O2production via 2e-ORR in an acidic electrolyte, these ms-dcdamaterials were all active and stable catalysts, among which glu-dcdaderived from D-glucose and dicyandiamide displayed the lowest onset potential of 0.553 V and the highest selectivity of up to 91.6%. The catalyst was also highly stable in chronoamperometric tests. Selective chemical titration of the C–OH and C=O groups revealed that the latter is far more active and selective than the former in 2e-ORR. Moreover, a positive correlation between the contents of C=O and pyrrolic N and the H2O2partial current suggests that the pyrrolic N group also contributes to 2e-ORR. This work affords a facile strategy for the sustainable fabrication of metal-free carbon-based catalysts efficient for H2O2electrosynthesis.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
NEW CARBON MATERIALS
·
2025
·
IF 6.8
Xiu-zhen LV,Xiang-xiang XU,Meng-meng YU,Yi-chen WEI,Jun-ying WANG,Jun-zhong WANG
The need for bi-functional catalysts that facilitate both the oxygen reduction (ORR) and carbon dioxide reduction (CO 2 RR) reactions arises from their potential to help solve the critical problems of carbon neutrality and renewable energy conversion. However, there are few reports on the development of bi-functional catalysts for zinc-air battery-driven CO 2 RR devices. We introduce a novel approach for synthesizing Fe 2 N/Fe 3 C species embedded in nitrogen-doped carbon nanofibers by electrospinning a solution of Hemin and polyacrylonitrile in N,N-dimethylformamide. The material has an exceptional catalytic performance, with a half-wave potential of 0.91 V versus RHE for the ORR and values of over 90% for both the selectivity and Faradaic efficiency for the CO 2 RR. The high catalytic performances are attributed to the strong coupling between the Fe 3 C/Fe 2 N heterostructure and the Fe-N-C sites in the nitrogen-doped carbon nanofibers. Notably, both Fe 3 C and Fe 2 N play distinct roles in both the ORR and CO 2 RR. This investigation indicates a way for designing advanced carbon-based bi-functional catalysts for use in this field.
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研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
BIOORGANIC CHEMISTRY
·
2023
·
IF 5.1
Xinxin Liu,Lei Chen,Ze Chen
Photodynamic therapy (PDT) has emerged as a highly efficacious therapeutic modality for malignant tumors owing to its non-invasive property and minimal adverse effects. However, the pervasive hypoxic microenvironment within tumors significantly compromises the efficacy of oxygen-dependent PDT, posing a formidable challenge to the advancement of high-efficiency PDT. Here, we developed a nanostructured photosensitizer (PS) assembled by cationic and anionic zinc phthalocyanines to load oxygen-throttling drug atovaquone (ATO), which was subsequently coated with polydopamine to obtain the final product ATO/ZnPc-CA@DA. ATO/ZnPc-CA@DA exhibited excellent stability, particularly in the blood milieu. Interestingly, the acidic microenvironment can trigger drug release from ATO/ZnPc-CA@DA, leading to a significant enhancement in fluorescence and an augmented generation of reactive oxygen species (ROS). ATO/ZnPc-CA@DA can induce synergistic cytotoxicity of PS and ATO, and significantly enhance the killing ability against tumor cells under hypoxic conditions. The mechanism underlying cytotoxicity of ATO/ZnPc-CA@DA was demonstrated to be associated with augmented cell apoptosis, disruption of mitochondrial membrane potential, diminished ATP production, heightened intracellular ROS generation, and reduced intracellular oxygen consumption. The animal experiments indicated that ATO/ZnPc-CA@DA possessed enhanced tumor targeting capability, along with a reduction in PS distribution within normal organs. Furthermore, ATO/ZnPc-CA@DA exhibited enhanced inhibitory effect on tumor growth and caused aggravated damage to tumor tissue. The construction strategy of nanostructured PS and the synergistic antitumor principle of combined oxygen-throttling drugs can be applied to other PSs, thereby advancing the development of photodynamic antitumor therapy and promoting the clinical translation.
研究领域:
生物医学工程
·
肿瘤学
·
药剂学
✓ 已验证
DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·
IF 3.5
Yan Jiaqi,Chen Wenkai,Ni Wenjin,Li Lu,Fu Jinfeng,Yang Qian,Yang Zhiyong
N -cyclohexylcyclohexanimine (N-CCA), a by-product of cyclohexylamine (CHA) oxidation to cyclohexanone oxime (CHO), was used as the starting reactant for the efficient conversion to CHO under an oxygen atmosphere, utilizing the constructed surface hydroxyl-rich Ti-based catalysts. Of these, the 20% TiO 2 /Hβ catalyst exhibited unique catalytic activity and stability, achieving 45.9% N-CCA conversion and 82.1% CHO selectivity, with the content of high-boiling by-products not exceeding 1.0%. The superior catalytic performance, as evidenced by characterization results, stems primarily from: (i) the combination of TiO 2 and Hβ, which promotes the formation of a high specific surface area with fine TiO 2 nanoparticles and high-density Ti δ+ active sites, which facilitate the adsorption and activation of N-CCA; (ii) the construction of rich hydroxyl groups, which enhances the Brønsted acid sites, thereby improving the generation of active oxygen species; (iii) the intercrystalline embedding of TiO 2 and Hβ, which forms Ti–O–Si bonds, effectively inhibiting Ti leaching and ensuring excellent catalyst stability. The conversion of N-CCA, the main by-product of CHA oxidation, to the desired CHO using an efficient and robust 20% TiO 2 /Hβ catalyst represents an attractive pathway.
研究领域:
催化
·
材料科学
·
化学反应工程
·
表面化学
✓ 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）