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Results in Chemistry · 2025 · IF 4.2

Nanostructure-controlled Cu-doped MnO2 for ozone synergistic catalytic disinfection

JianGuo Huang,Rashid Khan,Chunhui Zhai,Xianting Ding,Li-Sha Zhang,Jin-Ming Wu,Zhizhen Ye

The development of efficient disinfection techniques that can persistently eradicate viruses or disrupt their transmission is of paramount significance for curbing the spread of pandemics. Existing disinfection techniques commonly suffer from secondary pollution and difficulty in achieving continuous disinfection while ensuring safety and effectiveness, particularly in crowded environments. In this study, we adopted ozone synergistic catalytic oxidation (OSCO) technology for the highly efficient disinfection of bacteria and viruses. The OSCO route is based on the catalytic decomposition of ozone into active radicals in the presence of an optimized rod-like Cu/MnO 2 catalyst. The high catalytic activity of the Cu-doped MnO 2 catalyst can be attributed to the presence of numerous oxygen vacancies, which facilitate the catalytic decomposition of ozone into active radicals. This method serves multiple purposes, including the eradication of bacteria and viruses as well as the prompt decomposition of ozone to prevent any potential leakage. A disinfection rate of 99.9 % for both Staphylococcus albicans and H1N1 viruses was achieved within 20 min. The catalyst also demonstrated exceptional efficiency in degrading residual ozone, achieving a high removal rate of 99.99 % within 25 min, thus assuring safe disinfection. Density functional theory (DFT) calculations further supported that Cu doping induced lattice defects in MnO 2 , promoting the formation of interfacial oxygen vacancies and in turn favoring the catalytic oxidation process. The current OSCO technology offers a highly efficient and secure disinfection method with a wide range of potential applications in various fields.

研究领域: 环境科学 · 材料科学 · 微生物学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Tailoring hypervalent Nickel induced by oxygen vacancy toward enhanced oxygen evolution reaction performance in self-supporting NiFe-(oxy)hydroxides electrodes

Chun Kong,Chuang Zhi,Zirui Wu,Wenqiang Yang,Juan Yang,Zhongti Sun

NiFe-(oxy)hydroxides are the most active transition metal oxide electrocatalysts for oxygen evolution reaction (OER) under the alkaline media. Herein, we controllably manipulated oxygen vacancy (V O )-tunable NiFe-(oxy) hydroxides that their OER performances possessed a volcano-type relationship with V O concentration, positively-correlated with Ni 3+ /Ni 2+ ratio. Theoretical simulations further unearthed the enhanced activation and dissociation of H 2 O by the inserting of V O . As a result, the optimal sample featuring the Ni 3+ /Ni 2+ ratio of 30.3 % and V O of 23.8 % exhibited the overpotential of 243 mV at the current density of 100 mA cm –2 , simultaneously lasting 120 h durability without any attenuation, exceding the most reported NiFe-(oxy)hydroxides. This work offers an innovative view to understand the OER performance using hypervalent Ni ratio induced by V O defects.

CAS / MDL: 7782-61-8
研究领域: 材料科学 · 电化学 · 能源科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Interfacial synergism in NiMoO4/FeOOH heterostructure for enhanced alkaline oxygen evolution and urea oxidation

Junyi Chen,Jing Wang,Dongsheng Lou,Yingying Xiang,Tongming Sun,Yanfeng Tang,Minmin Wang

FeOOH with excellent catalytic properties for oxygen evolution and also considered to be a true active site has attracted great interest in recent years. However, the intrinsic low conductivity limits its catalytic performance. Herein, a one-dimensional core-shell NiMoO4/FeOOH heterojunction with high OER activity and stability was developed. At current densities of 10 and 100 mA cm-2, low overpotentials of 194 and 266 mV are need to drive oxygen evolution, meanwhile, the electrode exhibits high catalytic kinetics with small Tafel slopes of 53.4 mV dec-1 and excellent stability over 100 hours. Further analysis showed that the ultrathin FeOOH layer (~5 nm) uniformly covered the surface of NiMoO4 nanorods, acting as an active species and facilitating the surface change transfer to the interior. The internal NiMoO4 cores, on the other hand, provides reliable electron transmission as a highly conductive medium, and can effectively overcome the low conductivity of FeOOH. DFT calculations further manifest the strong electronic interactions between NiMoO4 and FeOOH species. The NiMoO4 core serves as mass transport of active materials is beneficial to tune the adsorption energy of OH- on the surface of electrocatalysts.

研究领域: 材料科学 · 电化学 · 催化科学
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2025 · IF 4.6

In-situ identification and dynamic transformation of FeOOH with different phases for oxygen evolution reaction

Ze-Feng Xu,Chuan-Wu Chen,Ya-Nan Jing,Da-Qiang Liu,Lei-Lei Li,Xing-Liang Yin

Iron(III) oxyhydroxide (FeOOH) is a highly promising non-precious metal oxygen evolution reaction (OER) catalyst due to its abundance, cost-effectiveness, and favorable electrochemical characteristics. Nevertheless, its low electrical conductivity and sluggish OER kinetics pose significant challenges for practical applications. OER typically occurs through the adsorbed evolution mechanism (AEM), involving multiple proton-coupled electron transfer steps with higher theoretical overpotential requirements. In contrast, the lattice oxygen mechanism (LOM) facilitates oxygen generation through direct coupling of the O−O bond, potentially circumventing the thermodynamic constraints inherent in AEM. In this study, an effective ion exchange between small-sized anions with large dipole moments and chloride ions residing within the tunnels of β-FeOOH was successfully achieved through phase-induced oxygen defect engineering. The experimental findings demonstrate that the synthesized α/β-FeOOH with high-density oxygen vacancy (O V ) exhibits enhanced lattice oxygen redox reactivity, expedited OER kinetics, and reduced thermodynamic barriers. Those improvements are ascribed to the activation of lattice oxygen within FeOOH, which has triggered a transition in its OER mechanism from AEM to LOM. Further investigations suggest that elevated reaction temperatures, within an appropriate range, foster ion exchange in β-FeOOH channels and actively encourage the creation of O V in FeOOH. That dynamic behavior transition of FeOOH enables it to overcome the inherent thermodynamic limitations of the AEM, resulting in a remarkable enhancement of its intrinsic OER activity. Remarkably, this improvement is achieved without relying on additional co-catalysts, which is expected to promote the understanding of intrinsic kinetic alterations in FeOOH electrocatalysts.

研究领域: 材料科学 · 电化学 · 能源科学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Bi-active sites of stable and highly dispersed platinum and oxygen vacancy constructed by reducing a loaded perovskite-type oxide for CO oxidation

Siran Zhang,Kang An,Shuangshuang Li,Ziyang Zhang,Ruolin Sun,Yuan Liu

A new scheme for constructing bi-active sites of highly dispersed Pt and oxygen vacancies on a catalyst was put forward in this study. Pt/LaCo x Ni 1−x O 3 /SiO 2 was synthesized by reducing LaCo x Ni 0.87−x Pt 0.13 O 3 with the structure of perovskite loaded on silica. The catalytic performance for carbon monoxide oxidation over the catalysts were studied. The catalysts were characterized via using XRD, XPS, XAFS, N 2 adsorption–desorption, H 2 -TPR, TEM, O 2 and CO-TPD techniques. The results pointed out that nanocrystal lines of LaCo x Ni 0.87−x Pt 0.13 O 3 were supported on SiO 2 . Pt clusters could be formed through reduction process at 300 °C and highly dispersed on catalyst’s surface, and the catalyst transformed to Pt/LaCo x Ni 1−x O 3 /SiO 2 ; at the same time, oxygen vacancies also formed on the surface of LaCo x Ni 1−x O 3 . The catalytic test revealed that LaCo 0.44 Ni 0.43 Pt 0.13 O 3 /SiO 2 displayed high activity and good stability for the oxidation of CO. The highly dispersed closely contact bi-active sites, the confinement of oxygen vacancies and strong interaction between Pt clusters and support were responsible for the significant catalytic activity and stability of LaCo 0.44 Ni 0.43 Pt 0.13 O 3 /SiO 2 catalyst.

研究领域: 催化化学 · 材料科学
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Molecular Catalysis · 2019 · IF 2.938

In situ formed Co clusters in selective oxidation of α-CH bond: Stabilizing effect from reactants

Zhijie Wang,Anxiang Guan,Mayfair C. Kung,Anyang Peng,Harold H. Kung,Ximeng Lv,Gengfeng Zheng,Linping Qian

Aerobic oxidation of α-C H bond of organic compounds to valuable chemicals is widely investigated in both fundamental research and industry. Due to the good stability of molecular oxygen, severe reaction conditions are generally required. Herein, by in situ synthesis we used molecular oxygen to induce cobalt nanoclusters with the sensitive catalysis in mild selective oxidation. The cobalt containing clusters with an average diameter around 0.9 nm are in situ prepared in the presence of cis -cyclooctene epoxidation and cyclooctene dimer oxide is formed at the interface to stabilize Co clusters with electron donation as an oil-soluble surfactant. The soluble clusters exhibit high activity in selective oxidation of α-C H bond of ethylbenzene into acetophenone and turnover number (TON) reaches about 7 × 10 4 during 50 h’ reaction at 373 K, which is around 960 times more active than the one using CoCl 2 salt as the catalyst, resulting from efficient mass transportation, π bond interaction and oxygen gas activation. Extended work based on this understanding demonstrates that cobalt nanoclusters also effectively catalyze aerobic oxidation of cyclohexene.

研究领域: 化学催化 · 有机合成 · 材料科学
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ENERGY & FUELS · 2017 · IF 3.091

Effects of CeO2, ZrO2, and Al2O3 Supports on Iron Oxygen Carrier for Chemical Looping Hydrogen Generation

Shiwei Ma,Shiyi Chen,Ahsanullah Soomro,Wenguo Xiang

Fe2O3 is an excellent active metal oxide for chemical looping hydrogen generation (CLHG) with high conversion of CO to CO2 in the reduction stage, and high H2 mole fractions in the subsequent steam oxidation stage, especially for its low cost and abundance in nature. However, supports are generally used to improve its reactivity and stability and to eliminate its carbon deposition. In this paper, Fe-based oxygen carriers are prepared by a coprecipitation method with three supports, i.e., CeO2, ZrO2, and Al2O3. The reactivity, carbon deposition, redox stability, and sintering characteristics of the oxygen carriers are analyzed to investigate the effects of supports as well as the fundamental mechanism. The results show that the properties of the oxygen carriers highly rely on the support and its interaction with iron oxide. The oxygen carrier supported on Al2O3 exhibits poor reactivity and stability, and the oxygen carrier supported on ZrO2 leads to much carbon deposition, decreasing H2 purity, despite its high reactivity and stability. Nevertheless, the oxygen carrier supported on CeO2 demonstrates good reactivity and stability with no carbon deposition observed, and the reducible support CeO2 counteracts the negative effect originating from sintering and guarantees the reactivity and stability of Fe2O3/CeO2 due to its oxygen mobility property and the oxygen mobility enhancement originating from the formation of Fe–Ce solid solution and perovskite-type CeFeO3. Overall, the reducible CeO2 is a potential support to improve the redox characteristics of iron oxygen carrier in CLHG, and the Fe2O3/CeO2 exhibits the highest reactivity at 850 °C. In addition, all three oxygen carriers are characterized by scanning electron microscopy images, energy dispersive X-ray spectrometer analysis, and X-ray diffraction patterns before and after the redox cycles.

研究领域: 能源技术 · 材料科学 · 化学工程 · 环境科学
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Catalysts · 2023 ·Vol. 13 ·期 4 ·781 · IF 3.9

Efficient Oxidative Dehydrogenation of Ethylbenzene over K/CeO2 with Exceptional Styrene Yield

He Sun,Juping Zhang,Kongzhai Li,Hua Wang,Xing Zhu

HighlightsWhat are the main findings?A styrene yield of 91.4% was found for 10% k/CeO2at 500 °C and CO2-O2mixed atmosphere. The excellent catalytic performance of 10% k/CeO2is attributed to the alkali metal oxide modified cerium oxide and carbon dioxide induced oxygen vacancies to promote the dehydrogenation of ethylbenzene.What is the implication of the main finding?The proposed ODH strategy by using oxygen vacancies enriched catalysts offers an important insight into the efficient dehydrogenation of ethylbenzene at mild conditions.AbstractOxidative dehydrogenation (ODH) is an alternative for styrene (ST) production compared to the direct dehydrogenation process. However, ODH with O2or CO2suffers from either over-oxidation or endothermic property/low ethylbenzene conversion. Herein, we proposed an ODH process with a CO2-O2mixture atmosphere for the efficient conversion of ethylbenzene (EB) into styrene. A thermoneutral ODH is possible by the rationalizing of CO2/O2molar ratios from 0.65 to 0.66 in the temperature range of 300 to 650 °C. K modification is favorable for ethylbenzene dehydrogenation, and 10%K/CeO2achieved the highest ethylbenzene dehydrogenation activity due to the enhanced oxygen mobility and CO2adsorbability. The catalyst achieved 90.8% ethylbenzene conversion and 97.5% styrene selectivity under optimized conditions of CO2-4O2oxidation atmosphere, a temperature of 500 °C, and a space velocity of 5.0 h−1. It exhibited excellent catalytic and structural stability during a 50 h long-term test. CO2induces oxygen vacancies in ceria and promotes oxygen exchange between gaseous oxygen and ceria. The ethylbenzene dehydrogenation in CO2-O2follows a Mars-van Krevelen (MvK) reaction mechanism via Ce3+/Ce4+redox pairs. The proposed ODH strategy by using oxygen vacancies enriched catalysts offers an important insight into the efficient dehydrogenation of ethylbenzene at mild conditions.Keywords:ethylbenzene;oxidative dehydrogenation;ceria;CO2

研究领域: 化学工程 · 催化科学
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CATALYSIS LETTERS · 2017 ·Vol. 148 ·期 1 ·181-193 · IF 2.799

CO Oxidation over Nanostructured Ceria Supported Bimetallic Cu–Mn Oxides Catalysts: Effect of Cu/Mn Ratio and Calcination Temperature

Lin Jin,Guo Yafei,Chen Xiao,Li Changhai,Lu Shouxiang,Liew Kim Meow

Abstract Nanostructured CeO 2 supported CuO–MnO 2 (CuMn/Ce) catalysts were synthesized by wet co-impregnation method and compared with CuO/CeO 2 and MnO 2 /CeO 2 catalysts on CO oxidation. The former shows significantly higher catalytic activity toward CO oxidation than the bimetallic oxides catalysts with minimum T 50 . Dual synergistic effects in the interfaces of CuO–MnO 2 and CuO–CeO 2 shall be responsible for the higher oxidation performance of CuMn/Ce catalyst. As Cu/Mn mass ratio varies from 1/0.2 to 1/9, CO oxidation activities of the catalysts present unimodal distribution, and the catalyst with Cu/Mn = 1/1 shows the highest performance (T 50  = 45.8 °C; Ea = 24.11 kJ mol −1 ). Cu acts as CO dissociative adsorption sites, and Mn–Ce supplies activated O species from gas molecule and lattice oxygen, which are both indispensable for improving utilization efficiency of the reactants in the dual redox processes. The catalytic performance of catalyst is also vitally correlated with calcination temperature (160–320 °C). The optimum calcination temperature of CuMn/Ce catalyst is 320 °C. Catalyst characterization results indicate that the pretreatment at 320 °C is decent to obtain desired metal oxides along with fine texture properties. Graphical Abstract

研究领域: 催化化学 · 材料科学 · 环境化学
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MATERIALS TECHNOLOGY · 2024 · IF 2.9

Enhancement of oxygen-deficient mediated oxidative stress by zinc-doped vanadium oxides against Candida albicans

Li Liu,Siyu Li,Detai Shi,Wei Zhu,Shuangshuang Zhang,Chengzhi Zhou,Tiangui Zhao,Xiaolong Li,Qifu Bao,Jianer Zhou

In this study, hydrothermal-calcination method was employed to synthesize pure vanadium oxide and zinc doped vanadium oxide powders. The crystal structure, morphology, chemical state and light absorption properties of the powders were also thoroughly analyzed. The antimicrobial effect against Candida albicans was evaluated by the circle of inhibition method and plate colony counting method. This study reveals the antibacterial mechanism of oxygen defects generating reactive oxygen species, leading to oxidative stress damage. This study not only demonstrates the potential of vanadium oxides as an efficient antimicrobial agent, but also provides a strong experimental basis and theoretical support for the design and optimization of novel antimicrobial materials by modulating the defect engineering of the materials. This finding provides a new perspective for the development of antimicrobial strategies against microorganisms and has important application prospects for the clinical treatment of Candida albicans infections.

研究领域: 微生物学 · 材料科学 · 医学
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 30 ·11949-11956 · IF 8.262

Electrodeposited SiO2 film: a promising interlayer of a highly active Ti electrode for the oxygen evolution reaction

Lian-Kui Wu,Xin-Yu Liu,Ji-Ming Hu

Ti-supported IrO2 or RuO2 oxide coated electrodes are widely used for the oxygen evolution reaction (OER) in acidic media. Electrocatalytic activity and long-term stability need to be further improved for these types of electrodes. A highly porous and well-adhered electrodeposited SiO2 (e-SiO2) film is proposed as the interlayer in this work to meet the above-mentioned requirements. The results show that the active oxide fully fills in the porous network throughout the whole thickness of the e-SiO2 film, to form “total-depth” highly porous oxide electrocatalytic coatings. For this reason, more than 1 order of magnitude higher apparent activity towards the OER at the Ti/e-SiO2/IrO2 (or RuO2) electrode is achieved compared to that of the conventional Ti/IrO2 or Ti/RuO2 electrode. Literature survey indicates that these novel electrodes are one of the most active Ti electrodes ever reported. The service life of this type of electrode is also obviously enhanced due to the “inter-locking” structure formed between the active oxide layer and e-SiO2 film.

研究领域: 电化学 · 材料科学
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ChemSusChem · 2018 ·Vol. 11 ·期 22 ·3965-3974 · IF 7.411

Interfacial CoOx Layers on TiO2 as an Efficient Catalyst for Solvent-Free Aerobic Oxidation of Hydrocarbons

Hai Wang,Liang Wang,Jian Zhang,Chengtao Wang,Ziyu Liu,Xinhua Gao,Xiangju Meng,Seung Jo Yoo,Jin-Gyu Kim,Wei Zhang,Feng-Shou Xiao

Graphical Ready layer one : A newly synthesized catalyst with layered cobalt oxide on the surface of titania (layer-CoO x /TiO 2 ) is highly selective towards the aerobic oxidation of C−H bonds in a series of hydrocarbons. In-depth structural and functional characterization reveal that the layer-CoO x /TiO 2 readily reacts with O 2 for the adsorption and activation of C−H bonds. Construction of efficient interfaces to improve the performance of supported metal catalysts is a challenging but effective technique. A newly synthesized catalyst with layered cobalt oxide on the surface of titania (layer-CoO x /TiO 2 ) is highly selective towards the aerobic oxidation of C−H bonds in a series of hydrocarbons under sustainable conditions. The layer-CoO x /TiO 2 easily outperforms the state-of-the-art noble metal catalysts and homogeneous cobalt salts used in industry. In-depth structural and functional characterization reveal that the layer-CoO x /TiO 2 readily reacts with O 2 for the adsorption and activation of C−H bonds. The layered structure of CoO x can maximize the interfacial effect of CoO x /TiO 2 leading to a good performance for the oxidation of C−H bonds.

研究领域: 催化化学 · 材料科学
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