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Catalysts · 2025 ·Vol. 15 ·期 6 ·544 · IF 4

Ligand-Mediated Tuning of Pd-Au Nanoalloys for Selective H2O2 Production in Direct Synthesis from H2 and O2

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.

CAS / MDL: 124-64-1
研究领域: 化学 · 催化材料科学
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Journal of Cleaner Production · 2025 · IF 10

Exploring the synergy between magnetic field and inorganic ligand for boosted O2 activation by microscale zero-valent iron

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 · 材料科学
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JOURNAL OF NUCLEAR MATERIALS · 2025 · IF 3.2

O2- Affected Corrosion of Nickel-based Alloy in LiCl-KCl Molten Salt for Pyroprocessing of Spent Nuclear Fuel

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 · 材料科学
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Journal of the American Chemical Society · 2023 · IF 15

High-Yield Synthesis of Colloidal Carbon Rings and Their Applications in Self-Standing Electrodes of Li–O2 Batteries

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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FREE RADICAL BIOLOGY AND MEDICINE · 2018 · IF 6.02

Argirein alleviates vascular endothelial insulin resistance through suppressing the activation of Nox4-dependent O2- production in diabetic rats

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 · 内分泌学 · 心血管科学 · 糖尿病研究
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RSC Advances · 2018 ·Vol. 8 ·期 41 ·23397-23403 · IF 2.936

3D web freestanding RuO2–Co3O4 nanowires on Ni foam as highly efficient cathode catalysts for Li–O2 batteries

Zhuo-Liang Jiang,Jing Xie,Cong-Shan Luo,Meng-Yang Gao,Huan-Liang Guo,Mo-Han Wei,Hong-Jun Zhou,Hui Sun

The mechanism of Li–O2 batteries is based on the reactions of lithium ions and oxygen, which hold a theoretical higher energy density of approximately 3500 W h kg−1. In order to improve the practical specific capacity and cycling performance of Li–O2 batteries, a catalytically active mechanically robust air cathode is required. In this work, we synthesized a freestanding catalytic cathode with RuO2 decorated 3D web Co3O4 nanowires on nickel foam. When the specific capacity was limited at 500 mA h g−1, the RuO2–Co3O4/NiF had a stable cycling life of up to 122 times. The outstanding performance can be primarily attributed to the robust freestanding Co3O4 nanowires with RuO2 loading. The unique 3D web nanowire structure provides a large surface for Li2O2 growth and RuO2 nanoparticle loading, and the RuO2 nanoparticles help to promote the round trip deposition and decomposition of Li2O2, therefore enhancing the cycling behavior. This result indicates the superiority of RuO2–Co3O4/NiF as a freestanding highly efficient catalytic cathode for Li–O2 batteries.

CAS / MDL: 90076-65-6 143-24-8
研究领域: 材料科学 · 电化学
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Energy Storage Materials · 2020 · IF 16.28

Water-proof, electrolyte-nonvolatile, and flexible Li-Air batteries via O2-Permeable silica-aerogel-reinforced polydimethylsiloxane external membranes

Xiaohong Zou,Kaiming Liao,Di Wang,Qian Lu,Chuan Zhou,Ping He,Ran Ran,Wei Zhou,Wanqin Jin,Zongping Shao

Although aprotic Li-air batteries offer an attractive option for achieving ultrahigh energy density of electrochemical energy storage devices, the now-established system has so far fallen short of its potential due to a daunting challenge related to its open configuration, which results in not only the rapid corrosion of Li metal anodes but also the gradual evaporation of organic liquid electrolytes. Here, we show that these issues can be well addressed by protecting the Li-air battery with a new O 2 -permeable silica-aerogel-reinforced polydimethylsiloxane external membrane (OPSP). The highly flexible OPSP basically benefiting from hydrogen-bond cross-linking can be constructed in situ on any substrate with particularly desirable properties such as being water-/electrolyte-proof, O 2 -permeable, high thermotolerance, and transparent, which allows stable cycling of coin-type and flexible Li-air batteries under harsh conditions, such as a highly volatile DMSO electrolyte (over 660 ​h), a humid air (O 2 ) atmosphere (over 700 ​h) or circumstances in air (O 2 )-saturated liquid water (over 25 ​h). This work could potentially open a new research direction in developing O 2 -permeable membranes through hydrogen-bond cross-linking for the unfettered design of metal-air batteries.

CAS / MDL: 90076-65-6 9002-84-0
研究领域: 材料科学 · 能源存储技术
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Nano Research · 2023 ·Vol. 16 ·期 11 ·12697-12705 · IF 9.9

Plasmonic nanostructures acting as a light-driven O2-sensitive nitroreductase mimic for enhanced photochemical oxidation of para-aminothiophenol

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.

CAS / MDL: 299-11-6 7757-82-6
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Journal of Physical Chemistry C · 2014 · IF 4.835

CeO2 Thickness-Dependent SERS and Catalytic Properties of CeO2-on-Ag Particles Synthesized by O2-Assisted Hydrothermal Method

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.

CAS / MDL: 123334-00-9
研究领域: 材料科学 · 催化化学
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GREEN CHEMISTRY · 2014 ·Vol. 17 ·期 1 ·335-342 · IF 6.852

The relationship between oxidation and hydrolysis in the conversion of cellulose in NaVO3–H2SO4 aqueous solution with O2

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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SOLID STATE IONICS · 2016 · IF 2.38

Understanding the enhanced electrochemical performance of samarium substituted Li[Li0.2Mn0.54 − xSmxCo0.13Ni0.13]O2 cathode material for lithium ion batteries

Guofeng Xu,Qingrui Xue,Jianling Li,Zhanyu Li,Xinping Li,Tianheng Yu,Jiguang Li,Xindong Wang,Feiyu Kang

Lithium-excess layered cathode materials Li[Li 0.2 Mn 0.54   −   x Sm x Co 0.13 Ni 0.13 ]O 2 (x   =   0, 0.01, 0.03, 0.05) with different quantities of Sm were synthesized by the coprecipitation-calcination method. The rare earth element samarium (Sm) was introduced into the structure of Li[Li 0.2 Mn 0.54 Co 0.13 Ni 0.13 ]O 2 as the replacement at Mn sites. The refinement unit cell parameters from the X-ray powder diffraction patterns illustrate the doping of Sm facilitates enlarging the lithium ions diffusion passageway space of the Li[Li 0 . 2 Mn 0.54 Co 0 . 13 Ni 0.13 ]O 2 structure. The Li[Li 0.2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode presented the best electrochemistry properties. The initial discharge capacity is 287.5   mAh   g −   1 and the initial coulombic efficiency increases from 81.31% to 85.34% with a constant current density of 12.5   mA   g −   1 , which can be attributed to the suppression of the oxygen release from the structure at the initial charge-discharge process. The Li[Li 0·2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode delivers 236.1   mAh   g −   1 after 40   cycles and the capacity retention ratio is 82.12% while only 206.8   mAh   g −   1 and 70.85% are obtained after 40 times of cycling for the pristine electrode. The Nyquist plots indicate that the electrical conductivity and interfacial electrochemical reaction activity increase as well.

CAS / MDL: 12060-58-1
研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2018 · IF 0

Enhanced Cycling Performance of Li–O2 Battery by Using a Li3PO4-Protected Lithium Anode in DMSO-Based Electrolyte

Huanhuan Guo,Guangmei Hou,Jianguang Guo,Xiaohua Ren,Xiaoxin Ma,Linna Dai,Shirui Guo,Jun Lou,Jinkui Feng,Lin Zhang,Pengchao Si,Lijie Ci

Lithium–oxygen batteries (LOBs) have attracted increasing interest because of their superior theoretical specific energy. However, the stability of lithium metal anode is one of the obstacles limiting their practical applications. Here, we introduce an artificial Li3PO4 solid electrolyte interphase (SEI) film to protect the lithium anode in LOB with LiI/LiNO3/DMSO (dimethyl sulfoxide) electrolyte. The Li3PO4-protected Li anode exhibits excellent electrochemical stability during the Li stripping/plating process and leads to a relatively uniform and featureless surface in LOB after cycling. Our research demonstrates that superior electrochemical performance can be achieved in the Li–O2 battery with the synergistic combination of the DMSO-based electrolyte, the LiI redox mediator, and the Li3PO4-protected Li anode. The LOB with a Li3PO4-protected Li anode exhibits a prolonged cycling life span of 152 cycles with a fixed capacity of 1000 mA h g–1 at 2 A g–1. The results in this work provide knowledge for the development of a robust strategy for protecting the Li anode in the applications of Li–O2 batteries.

研究领域: 材料科学 · 电化学 · 能源存储技术
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