Journal of Energy Chemistry
·
2020
·
IF 7.216
Kuncan Wang,Wen Li,Junjie Huang,Jiale Huang,Guowu Zhan,Qingbiao Li
The extraction of metallic nanoparticles from perovskite-type oxides (ABO 3 ) under mild reducing conditions is a novel way to prepare well-dispersed supported catalysts (B/AO δ ). Herein, we found that the encapsulated PdO in perovskite LaCoO 3 (PdO@LaCoO 3 ) could facilitate the phase transformation of the perovskite structure at a low temperature owing to both strong H 2 spillover of Pd and intimate interaction between the encapsulated PdO and LaCoO 3 . The pure LaCoO 3 without PdO was relatively inert to CO 2 hydrogenation (CO 2 conversion <4%). In contrast, PdO@LaCoO 3 exhibited excellent CO 2 methanation performance with 62.3% CO 2 conversion and >99% CH 4 selectivity. The characterization results demonstrated that the catalytically active Co 2 C was in-situ formed by carburization of the extracted Co 0 during CO 2 methanation for the PdO@LaCoO 3 sample. Whereas, the LaCoO 3 with surface supported PdO (PdO/LaCoO 3 ) showed a weak interaction and remained a perovskite structure with few Co 2 C active centers after the catalytic reaction, which was similar to the parent LaCoO 3 . Accordingly, the PdO/LaCoO 3 showed an inferior catalytic performance with 31.8% CO 2 conversion and 87.4% CH 4 selectivity. Therefore, the designed encapsulation structure of PdO within perovskite is critical to extract metallic NPs from perovskite-type oxides, which has the potential to prepare other integrated nanocatalysts based on perovskite-type oxides.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Renjing Zhang,Yanjian Wan,Jiali Peng,Gang Yao,Yunhong Zhang,Bo Lai
In this study, LaCoO 3 /Al 2 O 3 (LCA) was utilized as a heterogeneous catalyst to activate peroxymonosulfate (PMS) to degrade atrazine (ATZ). The structural properties of the catalysts were characterized by SEM, EDS, XRD, XPS and TPD. The effects of some key parameters (i.e., loadings of LCA, ATZ concentration, catalyst dosage, PMS concentration, initial pH and coexisting ions) were optimized. In addition, under the optimal conditions of 100 mg/L 23LCA, 100 mg/L PMS and initial solution pH 6.8, the removal rate and mineralization efficiency of ATZ (5 mg/L) reached 100% and 30.8%, respectively. The superiority of the 23LCA/PMS system was verified by two controlled experiments. After three cycles of experiments, the degradation effect of ATZ was within an acceptable range. The degradation intermediates of ATZ were detected by UPLC-QTOF-MS/MS, and the possible degradation pathway of ATZ was proposed. In addition, the presence of SO 4 − and HO was identified by quenching experiments and SO 4 − was verified as the predominant radical. Finally, based on the comprehensive analysis, a reasonable reaction mechanism of the 23LCA/PMS system was proposed. In a word, these results indicate that LCA can act as a highly efficient heterogeneous catalyst to activate PMS to degrade ATZ in water.
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CHEMOSPHERE
·
2023
·
IF 8.8
Yansong Ma,Biao Ma,Di Wu,Jun Wang,Yang Li,Xiaobin Fan,Qing Xia,Fengbao Zhang,Wenchao Peng
Perovskite materials are reported to be effective in peroxymonosulfate (PMS) based Fenton-like reactions, the leaching rates of chalcogenide materials in perovskite materials are however serious, thus leading to bad performance in long-term stability. In this study, an O-doped MoS 2 is synthesized to composite with LaCoO 3 , and the high catalytic activity of LaCoO 3 is well preserved with greatly decreased Co leaching. During the BPA degradation with PMS as oxidant, ∼100% degradation can be achieved in 20 min and this degradation efficiency can be maintained for ∼45 h in a simulated fixed bed reactor, which is almost 3 times longer than the pure LaCoO 3 . With the compositing of O-doped MoS 2 , the leached Co was greatly decreased and the dominated reactive oxidation species (ROS) transformed from SO 4 •– into O 2 •– with longer lifespan, thus resulting in the better stability. This study could promote the application of perovskite materials in the real industrial wastewater treatment .
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PubMed
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Junjie Huang,Kuncan Wang,Xintong Huang,Jiale Huang
With the assistance of nitrate additives (KNO 3 , NaNO 3 , Ca(NO 3 ) 2 or Mg(NO 3 ) 2 ), perovskite LaCoO 3 , which has a 3D porous structure and relatively high surface area (around 20 m 2 /g) was successfully synthesized at 500 °C via a sol-gel process. The results of thermal gravimetric analysis indicated that nitrates (especially NaNO 3 and KNO 3 ) acted as combustion aids, which significantly lowered down the crystallization temperature of LaCoO 3 by intensifying the decomposition of organic ingredients. Unlike other researches, the metal ions from the nitrate additives did not dope into the crystal lattice of perovskite and it was found that the remained nitrate additives would dramatically inhibit the LaCoO 3 catalytic activity on benzene oxidation. However, after removal of these remained nitrate additives by rinsing with deionized water, LaCoO 3 derived from our proposed salt-assisted sol-gel method exhibited an excellent catalytic activity.
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RSC Advances
·
2019
·Vol. 9
·期 61
·35646-35654
·
IF 3.049
Caiyun Wang,Lirong Zeng,Wei Guo,Cairong Gong,Jing Yang
In this study, a series of perovskite oxides LaCo1−xPtxO3−δ (x = 0, 0.02, 0.04, 0.06, and 0.08) were prepared by the citric acid–ethylenediaminetetraacetic acid (CA–EDTA) complexing sol–gel method and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Then, the samples were investigated as OER and HER bifunctional electrocatalysts in alkaline media. Compared with other catalysts, LaCo0.94Pt0.06O3−δ had good stability and presented more activity at a lower overpotential of 454 mV (at 10 mA cm−2), a lower Tafel slope value of 86 mV dec−1 and a higher mass activity of 44.4 A g−1 for OER; it displayed a lower overpotential of 294 mV (at −10 mA cm−2), a lower Tafel slope value of 148 mV dec−1 and a higher mass activity of −34.5 A g−1 for HER. The improved performance might depend on a larger ECSA, faster charge transfer rate and higher ratio of the highly oxidative oxygen species (O22−/O−). Furthermore, the eg orbital filling of Co approaching 1.2 in the B site might play a leading role.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 16
·8554-8560
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IF 3.269
Kuiyuan Wang,Jinzhu Song,Xijian Duan,Jianshuai Mu,Yan Wang
Perovskite LaCoO3 materials (LCO NPs) were prepared and found to possess both peroxidase-like and catalase-like catalytic activities. The LCO NPs can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 generating a blue color change under acidic conditions or decompose H2O2 under alkaline conditions with the generation of oxygen. Catalytic kinetics together with the possible mechanism of the peroxidase-like activity was investigated. The peroxidase-like catalytic properties of LaCoO3 nanoparticles were found to originate from their ability of accelerating electron transfer. Then based on their peroxidase properties, LCO NPs were applied to determine dopamine by using the colorimetric method with the dopamine-dependent successive inhibition reaction. The linear range of dopamine sensing was found to be 0.5–20 μM and the detection limit (LOD) was also discussed. The standard addition experiments were further performed with recoveries between 95.4% and 103.6%, and all the relative standard deviations (RSDs) were below 4.0%. The determination of dopamine therefore showed high accuracy and efficiency and has potential for the diagnosis of dopamine-related diseases.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Bang Xiao,Anqi Jiao,Yiran Zhang,Lin Yang,Xuteng Zhao,Chunping Wu,Dongdong Guo,Reggie Zhan,He Lin
NH 3 detection is of great significance for precise control of the SCR system. In this paper, mixed potential type ammonia sensor using LaCo 1-x Fe x O 3 sensing electrode, YSZ electrolyte, and Pt reference electrode was developed. LaCo 1-x Fe x O 3 sensing materials were made by flame spray pyrolysis technique, and Fe B-site substitution was implemented to enhance the sensing performance. It was observed that in the concentration range of 20–70 ppm at 475 °C, the sensor using LaCo 0.9 Fe 0.1 O 3 as sensing electrode exhibited the highest sensing signal and sensitivity to ammonia among the LaCo 1-x Fe x O 3 -SE sensors (x = 0, 0.05, 0.1, 0.2, 0.3). A sectional linear relationship between the response value change( Δ V ) of that sensor and the logarithm of ammonia concentration within the range of 2–15 ppm and 15–70 ppm was noticed, and the sensitivities were 17.52 and 87.22 mV/decade, respectively. Its lower detection limit reached 2 ppm at 475 °C. Its excellent sensing properties are ascribed to enriched oxygen vacancies and high electrocatalytic performance of the perovskite electrode. Moreover, the sensor exhibited good selectivity against CH 4 , CO, NO, NO 2 , and good stability against oxygen and water vapor concentration fluctuation. Besides, the sensing response to 50 ppm ammonia has been tested for 22 days and only a slight fluctuation within 7 % was observed. Furthermore, the mixed potential sensing mechanism of the sensor was discussed.
研究领域:
化学传感器
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材料科学
·
环境监测
·
催化
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Nanoenergy Advances
·
2026
·Vol. 6
·期 3
·20
·
IF 4.2
Qilan Shangguan,Huiying Qiu,Yanzhi Sun,Pingyu Wan,Yang Tang,Yongmei Chen
In this study, an electrochemical system for methane conversion was developed, employing Ni- and Ce-doped LaCoO3perovskite as the anode catalyst in an Na2CO3electrolyte. Structural characterization revealed that the La1−yCeyCo1−xNixO3(x = 0–0.5, y = 0–0.12) synthesized by the sol–gel method maintains the perovskite structure, but is rich in oxygen vacancies. Electrochemical studies revealed that the performance of methane activation is related to the presence of Ni(III) in the catalyst, and reactive oxygen species (•OH and HOO−) are provided through water oxidation reactions (WOR) in the Na2CO3electrolyte. The electrocatalytic performance of the synthesized La0.92Ce0.08Co0.5Ni0.5O3during methane conversion was verified in an electrolysis cell, and ethanol and acetic acid were identified as the methane conversion oxygenates. Under ambient conditions, the formation rate of ethanol reached 577.0 μmol gcat−1h−1at 0.90 V (vs. Ag/AgCl) in 0.5 mol L−1Na2CO3. The catalyst was found to retain structural integrity and sustain catalytic activity over multiple reaction cycles.
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Molecular Catalysis
·
2023
·
IF 4.6
Jiahao Chen,Yiqing Zeng,Shule Zhang,Zhaoxiang Zhong,Qin Zhong
Interface interaction existed in the multicomponent determines the catalytic performance of composite catalysts. Herein, a Co 3 O 4 -LaCoO 3 (Co-La) composite catalyst with strong spinel-perovskite interface interaction was successfully synthesized via a one-pot sol-gel method for the catalytic oxidation of toluene. The activity test results showed that the optimal 1Co 3 O 4 –4LaCoO 3 (1Co-4La) catalyst exhibits much higher catalytic activity (T 90 = 215 °C, GHSV = 50,000 h −1 ) than Co 3 O 4 (T 90 = 295 °C), LaCoO 3 (T 90 = 256 °C) and 1Co 3 O 4 /4LaCoO 3 (1Co/4La) (prepared by mechanical ball-milling, T 90 = 285 °C). Characterizations revealed that the strong spinel-perovskite interface interaction generated between the Co 3 O 4 spinel and LaCoO 3 perovskite in 1Co-4La facilitates the transfer of interfacial electrons, contributing to the exposure of surface active Co 3+ and the enhanced oxidation ability of surface active Co 3+ on 1Co-4La. In addition, the reactive lattice oxygen of surface Co 3+ –O on 1Co-4La effectively promotes the decomposition of toluene into CO 2 , enabling the low-temperature oxidation of toluene through the Mars-van Krevelen (MvK) mechanism. This work provides insight into the promotional effect of multicomponent interface interaction on enhancing catalytic performance of spinel-perovskite composite catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Dihao Bai,Haixia He,Ziheng Wang,Huiyu Dong,Lei Sun,Xiangjuan Yuan
Herein, perovskite LaCoO 3 composites with different Co/La molar ratios (denoted as LC x O) were synthesized and exploited to activate peracetic acid (PAA) for naproxen (NPX) degradation. Comprehensive characterizations were employed to elucidate the physicochemical properties, morphology, and surface functionalization of LC x O composites. Notably, as the Co/La ratio decreased from 1.0 to 0.25, the LC x O composites exhibited reduced particle agglomeration, increased specific surface area, and elevated oxygen vacancies (O V ) content. Amongst, LC 0.25 O (Co/La = 0.25) exhibited the highest catalytic efficiency for PAA activation, achieving complete NPX degradation within 3 min, with a rate constant of 0.3764 min −1 , approximately four times greater than that of LC 1.0 O (0.09545 min −1 ). Mechanistic investigations through quenching experiments, EPR, XPS, and EIS characterizations demonstrated that both Co and O V jointly facilitated the generation of reactive species, including CH 3 C(O)OO • , • OH and singlet oxygen, in LC 0.25 O/PAA system. Additionally, DFT calculations and transformation product (TP) identification were used to propose the NPX degradation pathway, revealing the oxidation preferentially occurred in the electron-rich sites. Ecotoxicity assessment using ECOSAR suggested an overall increase in the toxicity of TPs due to the intactness of naphthalene ring. Moreover, LC 0.25 O exhibited excellent reusability and stability, maintaining 100 % NPX degradation efficiency over four consecutive cycles. The fixed-bed column experiments demonstrated consistent NPX removal efficiency above 90 % during continuous operation for 30 h, highlighting the robust potential of LC 0.25 O/PAA system for practical applications. This study offers new insights into the development of highly efficient and low-cobalt-content catalysts for PAA activation.
研究领域:
环境科学
·
催化化学
·
材料科学
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Weiyu Wang,Qian Zhang,Jiajun Wan,Jie Liu,Lei Wang,Maoshuai He
Owing to its remarkable energy density and specific capacity, lithium-sulfur (Li-S) battery has emerged as one of the most promising energy storage devices. Nevertheless, the shuttle effect and the sluggish conversion of polysulfides significantly impede the practical application of Li-S batteries. Hence, a LaCoO 3 functional material with a unique honeycomb structure was designed as an efficient polysulfide converter. The honeycomb-structured LaCoO 3 not only exhibits strong bonding energy towards polysulfides but also possesses abundant adsorption sites on its surface. The LaCoO 3 material also shows excellent catalytic properties to quickly convert the adsorbed and aggregated polysulfides, effectively suppressing the shuttle effect. Moreover, the honeycomb structure of LaCoO 3 can facilitate the rapid wetting and infiltration of the electrolyte. Consequently, the Li-S cell with LaCoO 3 functionalized separator provides an areal specific capacity of 3.10 mAh cm −2 after 150 cycles under high sulfur loading of 6.52 mg cm −2 . Moreover, under practical conditions where the electrolyte content is as low as 7 μL mg −1 and the sulfur loading is 7.96 mg cm −2 , the Li-S battery equipped with LaCoO 3 -separator can still provide an areal specific capacity of 5.93 mAh cm −2 after 50 cycles.
研究领域:
储能技术
·
材料科学
·
电化学
·
纳米材料
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高影响因子
JOURNAL OF CHEMICAL SCIENCES
·
2022
·Vol. 134
·期 2
·1-12
·
IF 2.15
Li Wenyu,Zhu Yumei,Guo Wei,Xu Hanwen,Gong Cairong,Xue Gang
This report designed a Pt/LaCoO 3 composite electrocatalyst for electrochemical water splitting: LaCo 0.94 Pt 0.06 O 3 was prepared via the sol-gel method and then dealt with a heat treatment in 10% H 2 /Ar atmosphere at 350 °C. The XRD, HRTEM, SEM and XPS results show that the Pt nanoparticles (NPs) exsolve from the perovskite lattice and are homogeneously distributed on the surface. The HER and OER performance of the samples was tested in 1 mol·L -1 KOH solution and the findings illustrate that compared with LaCo 0.94 Pt 0.06 O 3 , Pt/LaCoO 3 owes better OER and HER performance. The improved performance could be up to the higher ratio of oxygen vacancies and improved charge transfer. Furthermore, the synergistic effect between Pt NPs and the LaCoO 3 matrix may also take a leading part in the future. Graphical abstract Figure SEM images of the samples: (a) LaCo 0.94 Pt 0.06 O 3 ; (b) Pt/LaCoO 3 . After the exsolution, the Pt/LaCoO 3 is well-developed with smooth surface and some nanoparticles are homogeneously distributed on the surface of the samples. The exsolved Pt nanoparticles can accelerate the electron exchange process between the matrix and its adsorbed intermediates, and ultimately promote the electrochemical reaction kinetics.
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