Molecular Catalysis
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2026
·
IF 4.3
Peiran Liu,Kang Wang,Xitao Wang
For propane dehydrogenation (PDH), cobalt-based catalysts are attractive candidates to replace Pt- and Cr-based systems, yet their practical application is hindered by rapid deactivation through sintering and coke deposition. In this work, we report a hybrid synthesis strategy to fabricate a Co–Al 2 O 3 catalyst (Co-Al 2 O 3 -INC) with atomically-dispersed Co 2+ sites strongly anchored in the γ-Al 2 O 3 . In contrast to an impregnated catalyst (Co-Al 2 O 3 -IMP) that forms reducible Co 3 O 4 clusters and suffers severe deactivation, the Co-Al 2 O 3 -INC catalyst exhibits high stability with propane conversion decreasing only marginally from 27.8% to 23.5% over 5 h. Extensive characterization confirms that the atomic dispersion of tetrahedral Co 2+ sites and the resulting strong metal–support interaction effectively suppress cobalt reduction and sintering, leading to significantly reduced coke formation. This study underscores the critical role of stabilizing isolated active sites via tailored synthesis for achieving highly stable PDH catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Chuang Li,Senqing Fan,Jiaojiao Chen,Yu Chen,Mingxia Yang,Jiaxin Meng,Haijie Qing,Yangchao Liu,Zeyi Xiao
An electrocatalytic membrane structured reactor with a stainless steel membrane as the Co3O4 catalyst carrier (Co3O4@SS EMSR) has been fabricated for benzyl alcohol oxidation coupled with hydrogen evolution. The structural characterization shows that the Co3O4 catalyst with the average size of 20 nm has been immobilized in the membrane pores. The electrochemical characterization indicates that the electrochemical active surface area can be increased and faster electron transfer can be achieved. During the process of benzyl alcohol oxidation coupled with hydrogen evolution by Co3O4@SS EMSR via flow-through mode, the benzyl alcohol conversion of 99% and the selectivity of benzoic acid of 97.7% with the Faraday efficiency of 95.9% for benzoic acid production can be achieved. The hydrogen production from the experiments is approximately consistent with the theoretically calculated hydrogen production, and a Faraday efficiency of 99% for hydrogen evolution can be achieved. The cell voltage during benzyl alcohol oxidation coupled with hydrogen evolution under the flow-through mode is reduced by 850 mV, and energy consumption is reduced by 2.03 kWh NmH2–3 under the condition of a current density of 2.6 mA cm–2, compared with those of hydrogen production by water electrolysis with the oxygen evolution reaction.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Zhaohui Yin,Sisi He,Yuwei Li,Wenjing Dai,Hong Wang,Runhe He,Kui Tang,Yiming Xiao,Songbo Wang,Jian Gao,Lei Zhang,Jianxin Li,Na Tang,Zhen Yin
Self-supported carbon electrodes have been intensively explored in the fields of materials chemistry, energy storage, and conversion due to the unique features of carbon materials. Herein, we report a facile strategy to construct a freestanding carbon membrane (CM) electrode consisting of a microfiltration CM and two-dimensional (2D) ultrathin Co3O4 nanosheets (NSs), which is successfully applied as an efficient and binder-free carbon electrode in the electrochemical applications of enzyme-free glucose detection and supercapacitors. Owing to the inherent structural merits, including the three-dimensional (3D) interconnected porous network in the membrane, structural integrity, high conductivity, and the well-dispersed and in situ growth of 2D Co3O4 NSs, the obtained Co3O4 NSs/CM demonstrated superior electrochemical performances and excellent long-term operation stability. Our present work paves the path to fabricate low-cost and efficient carbon electrodes with a rational structure design for multifunctional materials.
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APPLIED PHYSICS LETTERS
·
2023
·Vol. 122
·期 12
·
IF 4
Zhu Guozhen,Yang Qihao,Che Renchao
Co 3 O 4 /NiO@C (CNOT@C) microspheres were synthesized via a facile solvothermal method and annealing treatment under an argon atmosphere. A high initial reversible specific capacity of 1469.7 mA h g −1 of CNOT@C was attained due to its high specific surface area from its unique triangular hollow tube morphology. These triangular hollow tubes relieved volume expansion from repeated cycling processes, with CNOT@C attaining a high reversible specific capacity of 694.9 mA h g −1 after 1000 cycles at 6000 mA g −1 . Furthermore, excellent rate performance of CNOT@C was achieved due to its carbon layer coating, exhibiting a reversible specific capacity of 429.8 mA h g −1 at 10 000 mA g −1 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Lu Cui,Di Wu,Xiaomei Liu,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
In this study, free-standing Co 3 O 4 -CuO/CF electrodes are synthesized via an electrodeposition-annealing process and then protected by dip-coated carbon nanotubes (CNTs). The obtained Co 3 O 4 -CuO@CNTs/CF is employed as cathode to activate peroxymonosulfate (PMS) for the degradation of Bisphenol A (BPA) in an electrochemical system. The electrochemical assistant (EA) plays a critical role to accelerate metal redox by donating electrons sustainably, and the fast regeneration of Co 2+ /Cu + could be achieved to promote chemical-catalysis for PMS activation, which is proved via the pre-electroreduction treatment. The rate constant of Co 3 O 4 -CuO@CNTs/CF/PMS system with EA is ∼ 4.4 times compared to the system without EA. It also exhibits an excellent stability, which could still remove over 90% of BPA after eight cycles in 45 min. In addition, the coating of CNTs could decrease leaching of metals effectively. According to quenching tests and electron spin-resonance spectroscopy (ESR), the presence of EA could enhance the radical route by producing more SO 4 •− and •OH greatly, which is also proved by much faster degradation of carbamazepine (CBZ) and atrazine (ATZ) than that without EA. This work reveals activation mechanism of PMS in the electrochemical system, and provides an effective strategy to achieve the fast metal redox cycle for effective and long-term pollutant degradation.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yuanzhong Li,Liling Li,Yufa Feng,Huize Wang,Jinyun Liao,Jianwei Ren,Weiyou Zhou,Mingyang He,Hao Li
Engineering and fabricating cost-effective and high-performing bifunctional catalysts for ammonia borane (AB) hydrolysis and methanolysis is paramount for their commercial availability. A series of rattle-structured CuO/Co 3 O 4 @C microsphere bifunctional catalysts for AB hydrolysis and methanolysis were produced using a simple hard template etching approach. The CuO/Co 3 O 4 @C-4 (4 refers to designed the mole ratio of Cu/Co) exhibits the best activity with TOF of 18.8 and 26.8 mol H2 ·mol cat -1 ·min −1 for AB hydrolysis and methanolysis, respectively. It is discovered that the excellent performance is mainly attributed to its unique rattle structure and the synergetic effect between Co 3 O 4 and CuO . Kinetic isotope effect (KIE) experiments and infrared spectroscopy were applied to investigate AB hydrolysis and methanolysis reaction mechanisms. A suggested mechanism for AB methanolysis on rattle-structured CuO/Co 3 O 4 @C-4 is proposed based on the experiment results. This work could provide useful guidance for the construction of high-performance bifunctional catalysts for AB hydrolysis and methanolysis for hydrogen production.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 31
·10869-10875
·
IF 4
Xianxian He,Hongfei Liu,Jiangzhou Qin,Zhaodong Niu,Jincheng Mu,Baojun Liu
The electrochemical reduction of nitrate (NO3−) to ammonia (NH3) has emerged as an attractive approach for selectively reducing NO3− to highly value-added NH3 and removing NO3− pollutants simultaneously. In this work, a heterostructured Co/Co3O4 electrocatalyst anchored on N-doped carbon nanotubes was prepared and applied for the NO3− reduction towards NH3 under alkaline conditions. The catalyst achieves outstanding performance with up to 67% NH3 faradaic efficiency at −1.2 V vs. Hg/HgO and 8.319 mg h−1 mgcat−1 yield at −1.7 V vs. Hg/HgO. In addition, it also exhibits good long-term stability. 15N isotopic labelling experiments prove that the yielded NH3 is derived from NO3− species. In situ electrochemical Raman spectra revealed that the structure of the as-prepared catalyst showed outstanding stability and identified possible intermediates during the electrocatalytic NO3− reduction reaction (NO3RR).
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Shengji Wu,Yalun Ma,Wangsheng Yu,Hui Wang,Wei Yang,Lei Che,Zhongxi Han
How to enhance the SO 2 tolerance of transition metal oxide-supported activated carbon is one of the hottest issues in the field of mercury capture from flue gas. Addition of a foreign metal ion to prepare bimetallic adsorbent is a common method of improving the SO 2 tolerance of adsorbent. However, this approach suffers from high cost and a complex preparation process. In this study, CeO 2 - and Co 3 O 4 -supported activated carbon ( m %CeO 2 /AC and m %Co 3 O 4 /AC), with various loading values of active center, were prepared by an incipient wetness impregnation method, and their SO 2 tolerances were compared. The mercury removal performance and SO 2 tolerance of both CeO 2 /AC and Co 3 O 4 /AC could be remarkably improved through increasing the loading amount of the active center. Co 3 O 4 /AC exhibited high affinity with SO 2 , and the chemisorbed oxygen in Co 3 O 4 would be largely consumed, when SO 2 was present in the flue gas, resulting in a significant decrease of mercury removal efficiency. The mercury removal efficiencies of 20%CeO 2 /AC, 40%CeO 2 /AC and 60%CeO 2 /AC were 86.1%, 93.7% and 93.7%, respectively, during removal of mercury from flue gas at 150 °C in the presence of SO 2 . 20%CeO 2 /AC was the optimal adsorbent for mercury capture from flue gas, owing to its excellent mercury removal efficiency, strong SO 2 tolerance and relatively lower cost. The mercury species formed over spent 20%CeO 2 /AC were HgO and HgSO 4 . The HgO was generated through the reaction of mercury and chemisorbed oxygen, while the formation of HgSO 4 was due to the reaction between mercury, SO 2 and chemisorbed oxygen. The regeneration investigation indicated that the activity of spent 20%CeO 2 /AC could be almost fully recovered through a temperature-programmed decomposition and desorption process. The present study showed that the SO 2 tolerance of CeO 2 /AC could be easily improved through regulation of the loading amount of the active center.
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Environmental Science-Nano
·
2022
·Vol. 9
·期 11
·4162-4176
·
IF 9.473
Qiuxia Liu,Yuelong Wang,Meicheng Wen,Yunlong Guo,Yupeng Wei,Guiying Li,Taicheng An
Formaldehyde has strong carcinogenic and cancer-promoting effects, and its removal from indoor air is still challenging. Transition metal oxides such as cobalt(II,III) oxide (Co3O4) are potential catalysts to eliminate formaldehyde. However, the inherent low activity of Co3O4 at room temperature has greatly limited its utilization for indoor air purification. In this work, an extremely facile and mild method was designed to prepare a Au@Co3O4 core–shell nanocomposite catalyst, and its catalytic and photocatalytic activities for formaldehyde oxidation were determined both under dark conditions and visible-light irradiation. This material exhibited not only high catalytic formaldehyde oxidation efficiency in the absence of light but also significantly promoted photocatalytic formaldehyde oxidation activity under visible-light irradiation. Electron paramagnetic resonance and in situ diffuse reflectance infrared Fourier transform spectroscopy were applied to identify the reactive oxygen species and the produced degradation intermediates which adsorbed onto the surface of the catalyst during the oxidation process. It was found that the enhanced catalytic activity of the Au@Co3O4 nanocomposite catalyst under visible-light irradiation was mainly attributed to the promotion of oxygen and formaldehyde activation by the photogenerated carriers, facilitating the formation of dioxymethylene and thereby accelerating the key step of the generation of formic acid and carbonate species. This fundamental study provides evidence for a catalytic mechanism of the photocatalytic degradation of formaldehyde and a basis for the rational design of catalysts that efficiently eliminate indoor formaldehyde through full use of visible light.
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COMBUSTION SCIENCE AND TECHNOLOGY
·
2022
·
IF 2.133
Fanggang Zhang,Yilun Liang,Juan Wang
Nano-sized Co3O4 is an effective catalyst for fuel oxidation due to its high capacity of oxygen storage, and it is thus frequently applied in improving the oxidation performance of hydrocarbon fuels. In our present work, attempts were made to study the catalytic performance of Co3O4 for the oxidation of liquid fuels over a wide temperature range. Neat n-decane and n-decane/1,2,4-trimethylbenzene mixtures were chosen because they are typical liquid hydrocarbon fuels. The evidences from this study suggest that the temperatures of both fuel ignition and full conversion are significantly decreased by Co3O4 catalyst. CO2 is the only product detected in the catalytic oxidation, which also proves the complete oxidation of the liquid fuels. Furthermore, to explore the possible reaction pathways on the catalyst surface, temperature-dependent and time-dependent in situ DRIFTS were employed to identify surface species and analyze catalytic mechanism. Various surface intermediates including bidentate, monodentate carbonate species, carboxylate species and molecular adsorbed n-decane have been observed. The experimental results indicate that n-decane oxidation over Co3O4 proceeds via the Mars-van Krevelen mechanism where lattice oxygen plays a critical role in the fuel oxidation.
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Bo Li,Huan-Yan Xu,Yu-Long Liu,Li-Min Dong,Sridhar Komarneni
Due to the in-situ generation of reactive oxygen species (ROS), sulfate radical-based advanced oxidation processes (SR-AOPs) have emerged for the oxidative degradation of organic contaminants. Developing highly efficient heterogeneous catalysts is of great importance for SR-AOPs. In this work, an urchin-like Co 3 O 4 nanocatalyst with oxygen vacancies (V O ) was elaborately fabricated and employed for enhanced peroxymonosulfate (PMS) activation to degrade the high-concentration active dye crystal violet (CV). The obtained sample was characterized by field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and N 2 adsorption/desorption isotherms. Characterization results indicated that this unique V O -rich urchin-like Co 3 O 4 nanocatalyst was endowed with a larger surface area and abundant reactive sites for PMS adsorption and activation. The experimental results of CV degradation showed that nearly complete removal of 100 mg L −1 CV could be realized within 30 min of reaction time under neutral conditions at room temperature, and the degradation process followed retarded-first-order kinetics. Electron paramagnetic resonance (EPR) spectra accompanied by quenching experiments of radicals demonstrated that the contribution of ROS to CV degradation followed this sequence: 1 O 2 > ▪OH > SO 4 ▪- > O 2 ▪- . The degradation pathways of CV were proposed by a combination of density functional theory (DFT) calculations along with frontier orbit theory while the toxicity of intermediate products was evaluated by quantitative structure-activity relationship (QSAR) prediction.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 15
·7202-7211
·
IF 3.925
Zijing Wang,Shixiang Lu,Wenguo Xu,Ziwen Wang,Hao Zuo
Stable electrode materials with suitable electrochemical performance and high specific power are essential for the application of supercapacitors. A combination of La2O3, Co3O4, and graphene on nickel foam (LCGN) was prepared by hydrothermal synthesis and heat treatment to construct a three-dimensional flower-like structure. The synergistic effect between La2O3, Co3O4, and graphene dramatically improves the electrode stability. Owing to the special three-dimensional flower-like structure that improves ion diffusion and prevents structural collapse during charging and discharging, the prepared LCGN composite exhibits an excellent specific capacitance of 2945.11 F g−1 (2.95 F cm−2) at a current density of 1 A g−1 and excellent rate retention of 79.20% at 30 A g−1. Moreover, the LCGN//LCGN symmetric supercapacitor shows excellent performance with a specific capacitance of 403.92 F g−1 at 1 A g−1, with power density and energy density (12 000 W kg−1 at 53.9 W h kg−1), reflecting its industrial potential. Under the condition of 10 A g−1 current density, the capacitance retention rate is still extremely high, 89.3% after 30 000 continuous charge and discharge cycles, which certifies the promising potential of LCGN for high-performance energy storage devices.
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