KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2023
·Vol. 40
·期 12
·3059-3067
·
IF 2.7
Yin Zihang,He Ruibo,Nie Fei,Wei Zhen,Jia Bo,Feng Qing,Fu Xiaolong,Zhang Wenyan
The oxygen evolution kinetics of industrial copper electrodeposition is slow, resulting in low electrocatalytic activity and high energy consumption. In this work, a quaternary composite of carbon coated active particles containing Mn, Co and Ce were prepared (Mn-Co 3 O 4 /CeO 2 @C), and Ti/Sb-SnO 2 /PbO 2 electrode doped with these active particles was prepared by co-electrodeposition. The microstructure and chemical composition of the electrode was characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and X-ray diffractometry (XRD). Linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS) and Tafel polarization curve (Tafel) were used to study the electrochemical properties of anode materials. The results showed that the doping of Mn-Co 3 O 4 /CeO 2 @C active particles promoted the crystal transition of PbO 2 , decreased the average grain size, and the doping of Ce increases the average valence state of Co. The modified titanium electrode showed excellent catalytic activity of the oxygen evolution reaction (OER) characteristics. The overpotential of the doped Ti/Sb-SnO 2 /PbO 2 anode was only 453 mV when the current density was 20 mA cm −2 in 0.5 M H 2 SO 4 solution, which is 508 mV lower than that of the undoped Ti/Sb-SnO 2 /PbO 2 anode. In simulated copper electro-deposition experiments, the cell voltage was reduced by about 400 mV, compared to the undoped Ti/Sb-SnO 2 /PbO 2 electrode.
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Advanced Composites and Hybrid Materials
·
2022
·Vol. 5
·期 3
·2557-2574
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IF 11.806
Lai Changwei,Guo Yao,Zhao Huihui,Song Haixiang,Qu Xiaoxiao,Huang Mina,Hong Suck Won,Lee Kwan
The double ion-buffering reservoirs of asymmetric supercapacitors (ASC) have drawn enormous interest due to their excellent electrochemical performance. Herein, we have prepared the hierarchical porous sandwich-like Co 3 O 4 -rGO-CNT > N-PEGm (Co 3 O 4 -RGOC, in which rGO was short for reduced graphene oxide and CNT > N-PEGm was modified with methoxypolyethylene glycol by nitrene chemistry) ternary composites via a solvothermal method. Remarkably, the Co 3 O 4 -RGOC composites exhibited unique structural features of the opened honeycomb-like structures as “ion-buffering reservoirs.” Moreover, in Co 3 O 4 -RGOC composites, both the intermediate sandwich layers of rGO sheets and the interpenetrating CNT > N-PEGms can form double conductive networks as express electron transport channels to improve the electronic conductivity by synergistic effect. The promising Co 3 O 4 -RGOC composites can be summarized as capacity of 138.5 mAh g −1 (capacitance of 1420.5 F g −1 ) at 0.5 A g −1 . Furthermore, the 3D rGO-PANI (PANI, polyaniline) aerogels as negative electrode materials also have been prepared by facile in situ polymerization and chemical reduction process. The 3D rGO-PANI presented excellent electrochemical performance of 218.8 F g −1 (capacity of 60.8 mAh g −1 ) at 0.5 A g −1 due to the hierarchical interconnected porous network structures. Finally, the corresponding asymmetric supercapacitors of Co 3 O 4 -RGOC//3D rGO-PANI devices exhibited a high energy density of 41.3 Wh kg −1 at power densities of 775 Wk g −1 with excellent electrochemical performance and long cycle performance. Our work can present a new concept to design the innovative asymmetric supercapacitors with double ion-buffering reservoirs as a combinatorial strategy for useful energy storage and conversion.
Graphical abstract
The novel double “ion-buffering reservoir” asymmetric
supercapacitors are fabricated with the double conductive networks of
battery-type Co 3 O 4 -RGOC ternary composites as positive
electrode and 3D rGO-PANI aerogels as negative electrode for energy storage-conversion application.
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Chemosensors
·
2022
·Vol. 10
·期 7
·260
·
IF 4.229
Zhaoxia Shi,Ling Xia,Gongke Li,Yufei Hu
High purity methyl tert-butyl ether (MTBE) can be used to adjust gasoline octane values. However, an isomer, methyl sec-butyl ether (MSBE), is the main by-product of its industrial production, and this affects the purity of MTBE. Pt/Au NPs@Co3O4composites with a hollow dodecahedron three-dimensional structure were synthesized using ZIF-67 as a template, with Pt and Au nanoparticles (NPs) evenly distributed on the shell of the hollow structure. A CTL sensor was established for the determination of MSBE based on the specificity of Pt/Au NPs@Co3O4. The experimental results showed that Pt/Au NPs@Co3O4had a strong specific cataluminescence (CTL) response to MSBE, with no interference from MTBE. The linear range was 0.10–90 mg/L, the limit of detection was 0.031 mg/L (S/N= 3), the RSD was 2.5% (n= 9), and a complete sample test could be completed in five minutes. The sensor was used to detect MSBE in MTBE of different purity grades, with recoveries ranging from 92.0% to 109.2%, and the analytical results were consistent with those determined by gas chromatography. These results indicate that the established method was accurate and reliable, and could be used for rapid analysis of MTBE gasoline additive.Keywords:Pt/Au NPs@Co3O4;cataluminescence sensor;methyl sec-butyl ether;methyl tert-butyl ether;rapid analysis;gasoline additive
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Wei Li,Wei Li,Kuanchang He,Longxiang Tang,Qian Liu,Kui Yang,Yi-Di Chen,Xin Zhao,Kai Wang,Hui Lin,Sihao Lv
Cobalt-based catalysts have been widely explored in the degradation of organic pollutants based on peroxymonosulfate (PMS) activation. Herein, we report an MXene nano-Co 3 O 4 co-catalyst enriched with oxygen vacancies (O v ) and steadily fixed in nickel foam (NF) plates, which is used as an efficient and stable PMS activator for the removal of 1,4-dioxane (1,4-D). Ti originating from MXene was doped into the Co 3 O 4 crystal, generating large amounts of O v , which could provide more active sites to enhance PMS activation and facilitate the transformation of Co 2+ and Co 3+ , causing a high stability. As a result, the 1,4-D removal efficiency of the NF/MXene-Co 3 O 4 /PMS system ( k app : 2.41 min −1 ) was about four times higher than that of the NF/Co 3 O 4 /PMS system ( k app : 0.62 min −1 ). In addition, singlet oxygen was the predominant reactive oxygen species . Notably, the 1,4-D removal of the NF/MXene-Co 3 O 4 /PMS system was over 95% after 20 h operation in the single-pass filtration mode with only 3.72% accumulative Co leaching, showing excellent stability and reusability of NF/MXene-Co 3 O 4 . This work provides a defect engineering strategy to design a robust and stable catalytic system for water treatment , which expands the application of MXene in the field of environmental remediation.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Wenyang Fu,Zhongzheng Hu,Yingying Du,Pei Su,Yi Su,Qizhan Zhang,Minghua Zhou
The electrochemical reduction of nitrate to ammonia (ERNA) has become a green treatment technology for nitrate wastewater. However, strong adsorption for product caused high activation energy for product desorption in scaling relations, blocking activity of electrocatalyst in ERNA. Density functional theory (DFT) calculations indicated that constructing dual active sites (Cu and Co 3 O 4 ) could achieve strong adsorption of nitrate (−2.91 eV) with low desorbing energy barrier of ammonia (0.13 eV), breaking scaling relations. This dual active sites Co 3 O 4 /Cu electrode achieved a high ammonia yield rate of 684 µg mg cat − 1 h −1 with 94.6% faradic efficiency, surpassing single active site Co 3 O 4 and Cu electrodes. For mechanism, In-situ electrochemical characterization found the vital intermediates of *NH and *NH 2 , demonstrating that indirect reduction was the main pathway on Co 3 O 4 /Cu electrode. Thus, it is believed that building dual active sites on electrode is a reliable strategy to enhance ERNA for purifying industrial wastewater polluted by nitrate.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuxin Li,Li Liu,Wei Li,Yeqing Lan,Cheng Chen
In this study, a novel Co 3 O 4 -La 2 O 2 CO 3 @C composite was fabricated via the calcination of Co-La bimetallic MOFs at 500 °C, and was employed to efficiently activate peroxymonosulfate (PMS) for simultaneous oxidation of roxarsone (ROX) and adsorption of concomitant inorganic arsenic. Approximately 100% of ROX (50 μmol L −1 ) was degraded by PMS (0.5 mmol L −1 ) activated with Co 3 O 4 -La 2 O 2 CO 3 @C (0.2 g L −1 ) at initial pH 6 within 10 min. Meanwhile, the produced inorganic arsenic was almost completely adsorbed within 90 min. The maximum adsorption capacity of As(V) by Co 3 O 4 -La 2 O 2 CO 3 @C was determined to be high up to 275.4 mg g −1 . Co 3 O 4 -La 2 O 2 CO 3 @C also exhibited superior stability. During 6 rounds, the degradation efficiency of ROX and the removal efficiency of the total As maintained almost 100% and more than 97%, respectively. SO 4 − and OH were confirmed to be the reactive oxygen species (ROS) in charge of the degradation of ROX and the conversion of As(III) to As(V). The investigation of the adsorption mechanism revealed that the As species were combined with La species via ligand and anion exchange, resulting in the formation of La-O-As bond. Furthermore, the practical application potential of Co 3 O 4 -La 2 O 2 CO 3 @C in the ROX degradation and the in-situ adsorption of the released arsenic were further evaluated in a continuous flow column reactor. The Co 3 O 4 -La 2 O 2 CO 3 @C composite as catalyst and adsorbent may offer a feasible strategy for the implementation of organoarsenic degradation and produced inorganic arsenic adsorption.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xingqi Huang,Lingce Kong,Wenming Chen,Haibo Wang,Jingjing Zhang,Zhimeng Gao,Yi Xin,Wencai Xu,Yanjun Zuo
Pelargonic acid vanillylamide (PAVA), a capsaicin-type dacryagogue agent utilized for anti-terrorism and riot control, possesses a low stimulus threshold. This characteristic can lead to environmental contamination following its application and may easily result in secondary stimulation to personnel. The synthesized cobalt-doped Co 3 O 4 /Ti 3 C 2 @C nanocomposite is applied to activate peracetic acid (PAA) and degrade PAVA. A carbon layer was coated on the surface of Ti 3 C 2 -MXene nanosheets to solve the problem of poor oxygen resistance in MXenes; thus, preventing a remarkable loss of surface reactivity. The BET surface area of Co 3 O 4 /Ti 3 C 2 @C was enlarged to 149.6 m 2 /g, substantially larger than that of Ti 3 C 2 (13.0 m 2 /g) and Co 3 O 4 (56.4 m 2 /g). The enhanced BET surface area and more active sites confer remarkable PAA activation and catalytic degradation properties toward PAVA. With 0.5 mg/mL of Co 3 O 4 /Ti 3 C 2 @C and 0.35 mM of PAA, 100 mg/L of PAVA was completely degraded in 60 min. Factors such as initial pH, PAVA concentration, catalyst dosage, and PAA concentration on PAVA degradation were systematically evaluated. Additionally, the nanocomposite's reusability and stability were confirmed through recycling tests. Radical quenching experiments and electron paramagnetic resonance analysis demonstrated that the acetylperoxy radical (CH 3 CO 3 ) was the primary species responsible for PAVA degradation. This study offers an example of the application of MXene and transition metal-activated PAA in wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Huan Xu,Dan Zhang,Minmin Liu,Daixin Ye,Shengjuan Huo,Wei Chen,Jiujun Zhang
Designing cost-effective and robust bifunctional electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is highly desired in hydrogen production from overall water splitting, but still suffers great challenges due to the sluggish catalytic OER/HER kinetics. In this paper, a surface/defect engineering strategy is developed to synthesize three-dimensional (3D) carbon foam (CF)-supported unique hierarchical Co 3 O 4 nanowires@NiO nanosheets core–shell nanostructured catalyst (NiO@Co 3 O 4 /CF) with rich oxygen-vacancies as a novel bifunctional catalyst for alkaline water splitting electrolysis. Benefited from the synergy of the 3D hierarchical core–shell structure and rich oxygen vacancies , the as-obtained NiO@Co 3 O 4 /CF shows both excellent OER ( η 200 = 325 mV, η 500 = 374 mV) and HER ( η 10 = 104 mV) activities with low Tafel slopes (64.26 mV dec −1 for OER and 109.14 mV dec −1 for HER, respectively) and outstanding stability. A simple overall water splitting electrolysis cell assembled by this bifunctional NiO@Co 3 O 4 /CF as both OER and HER catalysts requires only a cell voltage of 1.53 V to obtain the current density of 10 mA cm −2 and displays a long-term stability. This work has successfully developed an approach for rational design and novel synthesis of metal oxide hybrids as bifunctional electrocatalysts with high activity and stability for overall water splitting.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lei Yuan,Na Xin,Yu Liu,Weidong Shi
Research on environmentally friendly energy storage devices is an important strategy to solve the energy crisis and environmental pollution. Herein, a novel self-supporting electrode based on multi-dimensional Co 3 O 4 /NiCo 2 O 4 hierarchical flakes coating on graphene/carbon sphere (rGO/CS) conductive substrate is reasonably designed. Firstly, a simple hydrothermal method is used to synthesize NiCo 2 O 4 with both flake and nanoneedle morphology on the rGO/CS substrate. Subsequently, Co 3 O 4 /NiCo 2 O 4 @rGO/CS is obtained by in-situ growth of metal organic frameworks polyhedrons on the surface of NiCo 2 O 4 flakes followed by calcination. In the unique structure, benefitting from the synergy between the substrate and multi-element transition metal oxides, the integrated film shows good conductivity, high specific surface area and abundant active sites. Thus, the binder-free electrode exhibits an ultra-high specific capacitance of 3876.6 F g −1 (538.4 mA h g −1 ) at 1 A g −1 . A hybrid supercapacitor is assembled with activated carbon as the negative electrode and Co 3 O 4 /NiCo 2 O 4 @rGO/CS as the positive electrode, the device shows a highest energy density of 56.5 Wh kg −1 at a power density of 800 W kg −1 . After 6000 charge–discharge cycles, 92.5% of the initial capacitance can be still maintained, indicating its good application prospects in energy storage materials.
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RSC Advances
·
2020
·Vol. 10
·期 64
·38906-38911
·
IF 3.119
Changshui Wang,Jiahui Zhang,Zenong Zhang,Guancheng Ren,Dandan Cai
Controllable structure and defect design are considered as efficient strategies to boost the electrochemical activity and stability of catalysts for the oxygen evolution reaction (OER). Herein, oxygen defect hollow Co3O4/nitrogen-doped carbon (OV-HCo3O4@NC) composites were successfully synthesized using tannic acid-modified ZIF-67 (TAMZIF-67) as the precursor through a one-step pyrolysis. Tannic acid provides abundant oxygen during the pyrolysis process of the modified ZIF-67, which can contribute to the formation of oxygen defects and the construction of a hollow structure. The existence of oxygen defects is shown by X-ray photoelectron spectroscopy and electron paramagnetic resonance, whereas the hollow structure is confirmed by transmission electron microscopy. The optimized OV-HCo3O4@NC shows good electrocatalytic activity and exhibits a low overpotential of 360 mV at a current density of 10 mA cm−2 in 0.1 M KOH due to the hollow structure, abundant oxygen defects, and good electrical conductivity. This work provides valuable insights into the exploration of promising OER electrocatalysts with oxygen defects and special structures.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuxin Li,Li Liu,Zeming Wang,Lixiang Zhou,Yeqing Lan,Cheng Chen
4-aminophenylarsonic acid ( p -ASA) is usually employed as feed antibiotics which can kill bacteria, protozoa and spirochetes. When p -ASA is released into the environment by biological metabolism, it could be broken down to produce hypertoxic inorganic arsenic, including arsenite (AsO 3 3- ) and arsenate (AsO 4 3- ). In this study, cobalt and lanthanum composites loaded on rice straw biochar labelled as Co 3 O 4 -La 2 CO 5 @RSBC was obtained. The material was used as an efficient catalyst for peroxymonosulfate (PMS) activation and adsorbent to achieve the simultaneous degradation of p -ASA and adsorption of arsenic. 100% decomposition of p -ASA (50 μmol L -1 ) could be realized within 30 min, coupled with nearly complete removal of inorganic arsenic during 80 min at initial pH = 7. Co 3 O 4 -La 2 CO 5 @RSBC also possessed superior reusability and stability. Even in the third cycle, more than 95% of p -ASA was decomposed and meanwhile 92.5% of inorganic arsenic was removed. No cobalt ions were detected, and the concentration of lanthanum ions in the three cycles ranged from 8.05 to 9.90 mg L -1 , which was much lower than those reported in previous studies. A series of the material characterizations, electron paramagnetic resonance technology and scavenger tests were utilized to unveil the possible catalytic mechanism and the transformation pathways of p -ASA and arsenic. It was confirmed that 1 O 2 , O 2 ∙ - , OH ∙ , and SO 4 ∙ - generated from the PMS activation were responsible for the degradation of p -ASA and the oxidation of As(III) to As(V). Meanwhile, As(V) was rapidly adsorbed by Co 3 O 4 -La 2 CO 5 @RSBC. This study provides us with a novel and efficient approach to control p -ASA pollution in aqueous solution.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Haitao Li,Qiang Gao,Guanshuai Wang,Bo Han,Kaisheng Xia,Chenggang Zhou
As one of the newly emerging heterogenous catalysts for peroxymonosulfate (PMS) activation, complex hollow structured nanoreactors with multilevel interiors can significantly enhance the catalytic performance and manifest great potentiality in organic pollutant degradation. Herein, a novel yolk–shell structured CoTiO 3 @Co 3 O 4 nanoreactor was synthesized via a simple self-template method using amorphous TiO 2 nanospheres as template and CoCl 2 ·6H 2 O as cobalt source, respectively. Owing to the remarkable structural advantages and unique space confined effect, the as-synthesized CoTiO 3 @Co 3 O 4 nanoreactor exhibited a high efficiency for PMS activation, enabling 100% removal of rhodamine B (RhB; 50 mg L −1 ) in a short period of time, with a rate constant (0.1993 min −1 ) much higher relative to those of CoTiO 3 (0.0246 min −1 ) and Co 3 O 4 (0.0150 min −1 ). Moreover, this catalyst showed a low cobalt leaching (0.080 mg L −1 ) while keeping almost unchanged catalytic activity in the cyclic degradation processes. Based on ESR analysis and quenching experiments, the possible catalytic mechanism was proposed. The mineralization degree was found to be 79.5% in the RhB degradation process via TOC analysis. LC/MS was employed to identify the intermediates and corresponding degradation pathway was elucidated. Besides, CoTiO 3 @Co 3 O 4 nanoreactor was revealed to be also highly efficient in activating PMS for degradation of several other recalcitrant organic pollutants. This work may be suggestive to the design and synthesis of advanced complex hollow nanoreactors for environmental remediation.
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危险品化学品经营许可证（带存储）