ChemistrySelect
·
2024
·Vol. 9
·期 13
·e202303633
·
IF 1.9
Mingyan Chen,Wentao Wang,Xinkai Feng,Dehua Zhang,Yao Zhang,Yucheng Liu
Graphical This work describes the application of a highly efficient catalyst (NH 2 -UiO-66-Mo) to the catalytic oxidation desulfurization process. NH 2 -UiO-66-Mo can greatly improve the efficiency of oxidative desulfurization The optimum operating conditions of NH 2 -UiO-66-Mo are investigated through experiments, which prove the excellent performance of the catalyst, and the reaction mechanism is further studied through a series of characterizations. A highly efficient oxidative desulfurization composite catalyst NH 2 -Uio-66-Mo has been prepared and applied in the catalytic oxidative desulfurization. It was elucidated that Mo 6+ could increase the oxygen vacancies and active sites on the catalyst and increase the pore size of UiO-66. Meanwhile, the removal rate of dibenzothiophene (DBT) reached 99.2 % after 60 min under optimal conditions and remained above 90 % after 5 cycles, showing the composite catalyst's remarkable catalytic performance and satisfactory reusability NH 2 -UiO-66-Mo. In addition, kinetic studies revealed that the desulfurization process can present a pseudo-first-order kinetic process. The apparent activation energy was 10.6 kJ/mol. Finally, in combination with oxides, possible oxidation pathways were identified.
研究领域:
化学工程
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材料科学
·
催化反应
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DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 6
·544
·
IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
研究领域:
化学
·
催化材料科学
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高影响因子
Journal of Cleaner Production
·
2025
·
IF 10
Mingjie Huang,Bingyuan Xu,Ke Feng,Wei Xiang,Xiaohui Wu,Yiliang Lv,Tao Zhou
Microscale zero valent iron (ZVI) is a promising material for in situ water purification through O 2 activation, but its activity is hindered by the slow electron transfer rate caused by the shielding effect of the surface passivation layer. Herein, we introduce a synergistic strategy that combines an inorganic ligand, i.e., tetrapolyphosphate (TPP), with magnetic field (MF) to boost the O 2 activation efficiency of ZVI under neutral conditions. This approach has resulted in a 4.7-fold increase in the degradation rate of diclofenac (DCF) compared to the MF-unassisted system and a remarkable 22.0-fold improvement over an analogous system with MF and EDTA. Multiphysics simulations, batch experiments, and characterizations revealed that the enhanced degradation rate was not only attributed to the elevated magnetic gradient on the ZVI surface to enrich the paramagnetic O 2 and Fe ions, but also to the functions of TPP to suppress the annihilation of •OH and reduce the redox potential of Fe 2+ /Fe 3+ . Furthermore, a synergistic mechanism between MF and TPP that facilitates the detachment of the surface-bound Fe 3+ -TPP complex into the aqueous phase, thereby regenerating the surface active sites was elucidated. This study underscores the potential of the MF-TPP synergy as an effective strategy to enhance ZVI-based Fenton-like catalysis for pollutant remediation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF NUCLEAR MATERIALS
·
2025
·
IF 3.2
Chengyu Wang,Xiaorui Xu,Yang Tong,Wentao Zhou,Yafei Wang
Pyroprocessing of spent nuclear fuel is an important step in nuclear fuel cycle with the purpose of minimizing the radiation impact on environment and recycling useful elements. One major concern in the development of pyroprocessing is the structural material corrosion in LiCl-KCl molten salt electrolyte, which is the core component of the spent nuclear fuel reprocessing. To understand the influence of O 2- impurity on the structural material corrosion in LiCl-KCl molten salt, the study investigates the corrosion behavior of Inconel 600 alloy in LiCl-KCl molten salt containing different amounts of O 2- impurities at 500 °C by immersion corrosion experiments and electrochemical analyses.The results indicate that O 2- could accelerate the high-temperature corrosion behavior. The alloy surface developed a bilayer oxide structure following 500-hour exposure to molten salt with 3 mol% O 2- , identified as a 3.36-μm-thick outer Li 2 NiO 2 layer and a 1.11-μm-thick inner LiCrO 2 layer. Based on the corrosion behaviors of Inconel 600 alloy in LiCl-KCl molten salt with different amounts of O 2- impurities, a new O 2- affected corrosion mechanism involving the formation of dual-layer oxide films and nickel-rich particles was proposed, which could provide new insights for the corrosion study in the applications of pyroprocessing of spent nuclear fuel.
研究领域:
核能工程
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材料科学
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DOI
高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Shang Shi,Zhenzhen Shen,Shanshan Li,Qian Wang,Rui Wen,Bing Liu
The use of carbon materials in porous electrodes has impressive advantages. However, precisely tailoring the multilevel pore structure of carbon electrodes remains an unsolved challenge. Here, we report a highly efficient site-selective growth strategy to synthesize colloidal carbon rings by templating patchy droplets. Carbon rings are used for the direct fabrication of self-standing porous electrodes with hierarchical pores for lithium–oxygen batteries (LOBs). In situ atomic force microscopy reveals that during discharge the discharge products densely nucleate and grow on carbon rings, demonstrating that such rings are a very potential electrode material in LOBs. The hollow carbon ring electrode (HCRE) possesses micrometer-scale channels formed by random packing of rings and nanochannels consisting of ring-shaped hollow cavities connected by nanosized pores in the wall. Both channels contribute to ion transportation and gas diffusion, but the storage of the discharge products mainly lies in micrometer-scale channels, leading to a high discharge capacity of LOBs (20 658 mAh/g). Our work paves a new way to construct hierarchically porous electrodes for application in electrocatalysis and electrochemical energy storage.
研究领域:
材料科学
·
电化学能源存储
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DOI
高影响因子
FREE RADICAL BIOLOGY AND MEDICINE
·
2018
·
IF 6.02
Qing Li,Jie Su,Shi-Jie Jin,Wei Wei,Xiao-dong Cong,Xiao-Xue Li,Ming Xu
Background Insulin resistance in endothelial cells contributes to the development of cardiovascular disease in type 2 diabetes mellitus (T2DM). Therefore, there are great potential clinical implications in developing pharmacological interventions targeting endothelial insulin resistance. Our previous studies indicated that argirein which was developed by combining rhein with L -arginine by a hydrogen bond , could substantially relieved stress related exacerbation of cardiac failure and alleviated cardiac dysfunction in T2DM, which was associated with suppressing NADPH oxidase activity. However, it is unclear whether argirein treatment attenuates the vascular lesion and dysfunction in T2DM and its underlying mechanisms. Methods and results The rat aortic endothelial cells (RAECs) were used to treat with palmitic acid (PA), a most common saturated free fatty acid , which could induce insulin resistance. It was showed that argirein increased glucose uptake and glucose transporter-4 (Glut4) expression and reversed the phosphorylation of IRS-1-ser307 and AKT-ser473, consequently resulting in the increase of the production of eNOS and NO in PA-induced RAECs. We further found that argirein blocked the Nox4-dependent superoxide (O 2 -. ) generation, which regulated glucose metabolism in RAECs during PA stimulation. In vitro, argirein increased the release of endothelial NO to relieve the vasodilatory response to acetylcholine and insulin, and restored the expression of Nox4 and pIRS-1-ser307 in the aorta endothelium of high-fat diet (HFD)-fed rats following an injection of streptozocin (STZ). Conclusion These results suggested that argirein could improve endothelial insulin resistance which was attributed to inhibiting Nox4-dependent redox signaling in RAECs. These studies thus revealed the novel effect of argirein to prevent the vascular complication in T2DM.
研究领域:
药理学
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内分泌学
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心血管科学
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糖尿病研究
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DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 16
·期 11
·12697-12705
·
IF 9.9
Gao Xinshuang,Zheng Jia-jia,Li Hanbo,Cai Rui,Gao Xingfa,Wu Xiaochun
Nanozymes, as a novel form of enzyme mimics, have garnered considerable interest. Despite overcoming the main disadvantages of their natural analogs, they still face challenges such as restricted mimic types and low substrate specificity. Herein, we introduce a reactive ligand modification strategy to diversify enzyme mimic types. Specifically, we have utilized helical plasmonic nanorods (HPNRs) modified with para -nitrothiophenol (4-NTP) to create an oxygen-sensitive nitroreductase (NTR) with light-controllability. HPNRs act as a light-adjustable source of nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate (NAD(P)H), providing photon-generated energetic electrons to adsorbed 4-NTP molecules. In the presence of O 2 , the activated 4-NTP transfers the captured electron to the adsorbed O 2 , mimicking the electron transfer process in its natural counterpart. This enhanced O 2 activation notably boosts the oxidative coupling of para -aminothiophenol (4-ATP). Density functional theory (DFT) calculations reveal that hot electrons injected into the lowest unoccupied molecular orbital (LUMO) energy level of 4-NTP can be transferred to that of molecular oxygen. In conclusion, our findings underline the potential of the reactive ligand modification strategy in developing new types of enzyme reactions, which opens up promising avenues for the enhancement and diversification of nanozyme functionalities.
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高影响因子
Journal of Physical Chemistry C
·
2014
·
IF 4.835
Sujie Chang,Shigang Ruan,Erlong Wu,Weixin Huang
Oxide-on-metal particles with exposed interfaces exhibit wealthy structures and functions, but their facile synthesis remains as a challenge. Herein we report a facile O2-assisted hydrothermal method to synthesize CeO2-on-Ag particles with different CeO2 thicknesses. In this novel approach Ag particles catalyze the O2 + H2O reaction to form surface hydroxyls that induce the preferential nucleation of Ce(OH)3 on the surfaces of Ag particles, eventually forming CeO2 adlayers on Ag particles. CeO2-on-Ag particles exhibit the CeO2 thickness-dependent SERS effect in which their best SERS effect is 2 orders stronger than that of Ag particles. They also exhibit CeO2 thickness-dependent catalytic performance in CO oxidation in which the best one is as active as traditional CeO2-supported Ag catalyst. These results open up new opportunities to synthesize oxide-on-metal particles and explore their functions by tuning the oxide adlayer thickness.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
GREEN CHEMISTRY
·
2014
·Vol. 17
·期 1
·335-342
·
IF 6.852
Muge Niu,Yucui Hou,Shuhang Ren,Wenhua Wang,Qitian Zheng,Weize Wu
Conversion of cellulose, the most abundant biomass, shows a high selectivity to yield formic acid (FA), when oxidized by O2 in NaVO3–H2SO4 aqueous solution. This conversion involves various reactions including hydrolysis and oxidation. In this work, the relationships between these reactions were studied. There are mainly two hydrolyses and two oxidations occurring in the conversion: initial hydrolysis (from cellulose to monosaccharides) and deep hydrolysis (from monosaccharides to levulinic acid); catalytic oxidation (from monosaccharides to FA) and ordinary oxidation (from levulinic acid to acetic acid). Among these four reactions, catalytic oxidation to FA and deep hydrolysis to byproducts are competitive. The increasing rate of deep hydrolysis is faster than that of catalytic oxidation, when temperature is increased. Catalytic oxidation is promoted and deep hydrolysis is suppressed, when the O2 pressure is increased. Moreover, deep hydrolysis is promoted and catalytic oxidation is suppressed, when H2SO4 concentration is increased. The hydrolysis–oxidation pathway of this conversion was proposed. Thus, the byproducts could be inhibited, and FA-oriented transformation could be realized.
研究领域:
生物化学
·
可再生能源
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DOI
高影响因子
MATERIALS LETTERS
·
2014
·
IF 2.269
Ming Yan,Yan Yan,Chao Wang,Wei Lu,Weidong Shi
In this letter, Ni 2+ doped InVO 4 nanocrystals were successfully synthesized by a simple one-pot microwave-assisted method. The energy bandgap of obtained samples can be precisely controlled by varying the Ni 2+ doping amount. The O 2 production rate of obtained Ni–InVO 4 nanocrystals is higher than that of pure InVO 4 nanocrystals under visible-light, which can be ascribed to the narrowed band gaps. The corresponding 1% doped sample N1 has the highest O 2 production rate (394 μmol/h) in all samples, which is 66% higher than the undoped sample N0.
研究领域:
材料科学
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环境科学
·
化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
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高影响因子
Small
·
2023
·Vol. 19
·期 33
·2301391
·
IF 13.3
Wenjing Zhang,Jian Zheng,Ruoyu Wang,Li Huang,Junkai Wang,Tianran Zhang,Xiangfeng Liu
Lithium–oxygen (Li–O 2 ) batteries have received extensive attention owing to ultrahigh theoretical energy density. Compared to typical discharge product Li 2 O 2 , LiOH has attracted much attention for its better chemical and electrochemical stability. Large-scale applications of Li–O 2 batteries with LiOH chemistry are hampered by the serious internal shuttling of the water additives with the desired 4e − electrochemical reactions. Here, a metal organic framework-derived “water-trapping” single-atom-Co-N 4 /graphene catalyst (Co-SA-rGO) is provided that successfully mitigates the water shuttling and enables the direct 4e − catalytic reaction of LiOH in the aprotic Li–O 2 battery. The Co-N 4 center is more active toward proton-coupled electron transfer, benefiting - direction 4e − formation of LiOH. 3D interlinked networks also provide large surface area and mesoporous structures to trap ≈12 wt% H 2 O molecules and offer rapid tunnels for O 2 diffusion and Li + transportation. With these unique features, the Co-SA-rGO based Li–O 2 battery delivers a high discharge platform of 2.83 V and a large discharge capacity of 12 760.8 mAh g −1 . Also, the battery can withstand corrosion in the air and maintain a stable discharge platform for 220 cycles. This work points out the direction of enhanced electron/proton transfer for the single-atom catalyst design in Li–O 2 batteries.
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PubMed
高影响因子
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