APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Ao-tian Gu,Xiao-jun Dai,Pei Liu,Jian Chen,Lei-Lei Gu,Peng Wang,Chun-hui Gong,Yi Yang
MOF-derived CuO/Co 3 O 4 heterojunctions were constructed for efficient PMS activation. • The interfacial built-in electric field induces directional electron transfer from Co to Cu. • High-valent metal species and non-radical pathways dominate BPA degradation. • Enhanced PMS adsorption promotes O − O bond cleavage and a non-radical pathway. Efficient removal of phenolic endocrine disruptors, such as bisphenol A (BPA), remains a significant challenge in complex aquatic environments. In this study, a CuO/Co heterojunction catalyst (CuCo-NC X ) was developed by anchoring Co 3 O 4 nanoparticles onto MOF derived CuO/carbon composites for the high-performance activation of peroxymonosulfate (PMS). The CuCo-NC/PMS system exhibited superior catalytic activity, achieving a 97.8% removal of BPA within 40 min, with a corresponding apparent rate constant of 0.1111 min −1 . Furthermore, it demonstrated exceptional anti-interference capability and selectivity in complex aqueous matrices containing various co-existing anions and natural organic matter. Density functional theory (DFT) calculations and systematic characterization revealed that a built-in electric field (BIEF) formed at the CuO/Co 3 O 4 interface strongly drives directional electron transfer from Co sites to Cu sites. During the catalytic process, the electron-rich Cu acts as an electron reservoir, significantly promoting the Co redox cycle through an electron feedback effect, which induces the generation of high-valent metal species (HVMs) and optimizes the PMS activation pathway. This study not only develops a high-performance catalytic platform for eliminating endocrine disruptors but also provides new insights into modulating heterogeneous catalytic pathways via interfacial BIEF. Download: Download high-res image (198KB) Download: Download full-size image
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Materials Today Chemistry
·
2023
·
IF 7.3
H. Chai,R. Li,L. Gao,H. Niu,J. Jin
The phase interface properties of the p-n junction may profoundly affect its photoelectrochemical (PEC) water oxidation performance. Here, we introduced a non-conjugated polymer functional layer (poly(diallyl-dimethylammonium chloride, PDDA) between the interfaces of the p-n junction (Co 3 O 4 /Gd–Fe 2 O 3 ) to tune the interfacial properties . First, the PDDA modulates the band structure so that the composite photoanode (Co 3 O 4 /PDDA/Gd–Fe 2 O 3 ) has an enlarger band bending than the p-n junction. Then, PDDA passivates the surface trap, which synergizes with Co 3 O 4 to provide more active sites for water oxidation. Furthermore, PDDA improves the PEC water oxidation kinetics. Specifically, PDDA extracts holes and adsorbs water oxidation reactants, thus it efficiently transfers photogenerated holes to Co 3 O 4 , promoting the water oxidation reaction in the positive direction. With these positive modulations, PDDA can further enhance the PEC water oxidation performance of the p-n junction. This conceptual work provides insight into the role of the non-conjugated polymer in PEC water splitting .
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Catalysts
·
2023
·Vol. 13
·期 3
·529
·
IF 3.9
Linshuang Xue,Chenyi Yuan,Shipeng Wu,Zhen Huang,Zhen Yan,Stéphane Streiff,Hualong Xu,Wei Shen
Coalbed methane is a significant source of methane in the atmosphere, which is a potent greenhouse gas with a considerable contribution to global warming, thus it is of great importance to remove methane in coalbed gas before the emission. Exploring the economical non-noble metal catalysts for catalytic methane combustion (CMC) has been a wide concern to mitigate the greenhouse effect caused by the emitted low-concentration methane. Herein, a series of Mn-doped Co3O4catalysts have been synthesized by the environmentally friendly solid-state method. As a result, the Mn0.05Co1catalyst performed the best CMC activity (T90= 370 °C) and good moisture tolerance (3 vol% steam). The introduction of an appropriate amount of manganese conduced Co3O4lattice distortion and transformed Co3+to Co2+, thus producing more active oxygen vacancies. Mn0.05Co1exhibited better reducibility and oxygen mobility. In situ studies revealed that methane was adsorbed and oxidized much easier on Mn0.05Co1, which is the crucial reason for its superior catalytic performance.Keywords:active oxygen;catalytic combustion;low-concentration;methane;Mn-Co3O4;solid-state
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Small
·
2023
·Vol. 19
·期 30
·2300770
·
IF 13.3
Shilin Zhang,Qingjie Wang,Peng Zhang,Jie Wang,Yue Li,Chang Lu,Muhammad Tariq Sarwar,Xiongbo Dong,Qihang Zhao,Aidong Tang,Liangjie Fu,Huaming Yang
To achieve a high separation efficiency of photogenerated carriers in semiconductors, constructing high-quality heterogeneous interfaces as charge flow highways is critical and challenging. This study successfully demonstrates an interfacial chemical bond and internal electric field (IEF) simultaneously modulated 0D/0D/1D-Co 3 O 4 /TiO 2 /sepiolite composite catalyst by exploiting sepiolite surface-interfacial interactions to adjust the Co 2+ /Co 3+ ratio at the Co 3 O 4 /TiO 2 heterointerface. In situ irradiation X-ray photoelectron spectroscopy and density functional theory (DFT) calculations reveal that the interfacial Co 2+ O Ti bond (compared to the Co 3+ O Ti bond) plays a major role as an atomic-level charge transport channel at the p-n junction. Co 2+ /Co 3+ ratio increase also enhances the IEF intensity. Therefore, the enhanced IEF cooperates with the interfacial Co 2+ O Ti bond to enhance the photoelectron separation and migration efficiency. A coupled photocatalysis-peroxymonosulfate activation system is used to evaluate the catalytic activity of Co 3 O 4 /TiO 2 /sepiolite. Furthermore, this work demonstrates how efficiently separated photoelectrons facilitate the synergy between photocatalysis and peroxymonosulfate activation to achieve deep pollutant degradation and reduce its ecotoxicity. This study presents a new strategy for constructing high-quality heterogeneous interfaces by consciously modulating interfacial chemical bonds and IEF, and the strategy is expected to extend to this class of spinel-structured semiconductors.
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Analytical Methods
·
2023
·
IF 3.1
Xuan Zhou,Jiaxin Li,Yuda Hu,Yaohui Wu,Yonghong Wang,Ge Ning
Kanamycin is used widely in livestock farming due to its antimicrobial properties and low cost, but has led to antibiotic residues in food, which can damage human health. Therefore, there is an urgent need for convenient technology that can be used to detect kanamycin rapidly. We found that Co3O4 nanoparticles (NPs) possessed peroxidase-like activity that catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine to change color. Interestingly, a target-specific aptamer could regulate the catalytic activity of Co3O4 NPs and inhibit this effect through aptamer–target binding. On the basis of a colorimetric assay combined with an aptamer-regulatory mechanism, the linear range for quantitative detection of kanamycin was 0.1–30 μM, the minimum limit of detection was 44.2 nM, and the total time needed for detection was 55 min. Moreover, this “aptasensor” displayed excellent selectivity and could be applied to detect KAN in milk samples. Our sensor might have promising applications for kanamycin detection in animal husbandry and agricultural products.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Longwen Chen,Feng Liu,Xiaoqian Li,Qiuzhen Tao,Zhaoqin Huang,Qi Zuo,Yanwu Chen,Tan Li,Mingli Fu,Daiqi Ye
Metal oxide-oxide interface on supported catalyst has been rarely studied due to the complex interfacial structure and synthetic challenge. Herein, different Ag-supported CeO 2 /Co 3 O 4 samples with various covered-state of CeO 2 were prepared for catalytic soot oxidation. In comparison, catalytic activity was significantly improved by grafting CeO 2 on Co 3 O 4 , in which the best performing Ag/CoCe-2 exhibited remarkable catalytic performance towards soot oxidation with a T 50 of 290.5 ℃ under 10 % O 2 /N 2 . Catalyst characterization investigated by Scanning Electron Microscope (SEM), quasi in-situ X-ray Photoelectron Spectroscopy (XPS), in-situ Raman, etc. revealed that this outstanding promotion in catalytic activity can be principally ascribed to the formation of the CeO 2 /Co 3 O 4 interface. An appropriate CeO 2 dosage maximized the contact and interaction between Co 3 O 4 and CeO 2 , resulting in the largest CeO 2 /Co 3 O 4 interface featured with abundant generated superoxide species and activated surface lattice oxygen. Density functional theory (DFT) calculations were also carried out for the oxygen vacancy formation energy, Gibbs free energy, etc. In presence of the CeO 2 /Co 3 O 4 interface, a charge density redistribution around the adsorbed reactants at oxygen vacancies could be formed, owing to the efficient charge transfer enhanced by the electron-appealing effect. The change in electronic structure favored reducing the oxygen vacancy formation energy and boosting the lattice oxygen activation induced by the hybridized Co-O-Ce bonds, finally lowering the adsorption and activation barriers for reactive species and accelerating the reaction kinetics.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Zihao Chen,Senjie Dong,Minghui Wang,Zunpeng Hu,Huiling Chen,Ye Han,Ding Yuan
Constructing three-dimensional (3D) hierarchical heterostructures is an appealing but challenging strategy to improve the performance of catalysts for electrical energy devices. Here, an efficient and robust flexible self-supporting catalyst, interface coupling of ultrathin CoFe-LDH nanosheets and Co3O4 nanowire arrays on the carbon cloth (CC/Co3O4@CoFe-LDH), was proposed for boosting oxygen evolution reaction (OER) in rechargeable liquid/solid Zn–air batteries (ZABs). The strong interfacial interaction between the CoFe-LDH and Co3O4 heterostructures stimulated the charge redistribution in their coupling regions, which improved the electron conductivity and optimized the adsorption free energy of OER intermediates, ultimately boosting the intrinsic OER performance. Besides, the 3D hierarchical nanoarray structure facilitated the exposure of catalytically active centers and rapid electron/mass transfer during the OER process. As such, the CC/Co3O4@CoFe-LDH catalyst achieved excellent OER catalytic activity in alkaline medium, with a small overpotential of 237 mV at 10 mA cm–2, a low Tafel slope of 35.43 mV dec–1, and long-term durability of up to 48 h, significantly outperforming the commercial RuO2 catalyst. More impressively, the liquid and flexible solid-state ZABs assembled by the CC/Co3O4@CoFe-LDH hybrid catalyst as the OER catalyst presented a stable open circuit voltage, large power density, superb cycling life, and satisfactory flexibility, indicating great potential applications in energy technology. This work provides a good guidance for the development of advanced electrocatalysts with heterostructures and an in-depth understanding of electronic modulation at the heterogeneous interface.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Chunmei Li,Sainan Ma,Ming Zhao,Maoxiang Jing,Weiyong Yuan,Changming Li
Hematite (α-Fe2O3) core–cocatalyst shell nanoarchitectures with ultrathin hybrid shells are promising to maximize photoelectrochemical (PEC) water oxidation performance of Fe2O3-based photoelectrodes, but their fabrication presents formidable challenges. For the first time, a wormlike nanostructured α-Fe2O3@Co3O4/graphene quantum dot (GQD) core–hybrid shell nanoarray is synthesized via self-assembly, showing an onset potential of 0.63 V (vs the reversible hydrogen electrode (RHE)) and a photocurrent density of 3.63 mA cm–2 at 1.23 V (vs RHE). This performance is superior to those of reported Fe2O3-based heterojunction photoanodes and among the best reported for Fe2O3-based photoanodes. The outstanding performance is due to the Co3O4/GQD shell significantly promoting charge separation and transfer and hole injection as well as great synergistic effects between GQDs and Co3O4. This work not only fabricates a low-cost photoanode with record-high water oxidation performance and offers scientific insights into the enhancement mechanism but also provides a facile, economical, and universal strategy to self-assemble conformal, ultrathin hybrid shells on three-dimensional (3-D) complex nanostructures, which have broad applications in the fields of energy, environment, and sensing.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qingqing Li,Zhujuan Ren,Yutong Liu,Chibin Zhang,Jiadi Liu,Rong Zhou,Yuanqing Bu,Feifei Mao,Hua Wu
Developing hierarchical and efficient catalysts with multiple active sites to activate peroxymonosulfate (PMS) for the degradation of persistent organic contaminants is crucial, whereas it's still a challenge. Herein, a novel petal-like N -doped porous carbon embedded with ultrafine cobalt oxide nanoparticles (NPs) (named as Co 3 O 4 /NC) was unprecedentedly fabricated via the pyrolysis of N -enriched Co-MOF (named as Co-TA), where the unique hierarchical structure, rich active sites and large specific area were contributed to improve the excellent catalytic activity toward tetracycline hydrochloride (TCH). As expected, the removal efficiency of TCH in Co 3 O 4 /NC/peroxymonosulfate system was 96.4 % within 30 min, extraordinary superior to direct air-calcining nano-Co 3 O 4 , commercial Co 3 O 4 and Co-TA, in which the kinetic constant was 10.4 times higher than pure Co-TA. Besides, above 97 % removal efficiency of TCH was maintained over a wide pH range of 5–9, and 71 % of total organic carbon (TOC) could be eliminated. The TCH degradation was mainly characterized by the coexistence of multiple active substances using EPR analysis, where SO 4 · − and 1 O 2 were the dominant contributors. The degradation pathways of TCH were also clarified based on theoretical calculation and HPLC-TOF-MS 2 data. This work can extend the application of metal–organic frameworks (MOFs)-derived nanocatalysts in the environment field, and may offer a promising metal oxide heterogeneous catalyst for the rapid elimination of persistent organic pollutants by sulfate radical-based advanced oxidation processes (SR-AOPs).
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shaomian Liu,Wenjuan Xue,Yongjun Ji,Wenqing Xu,Wenxing Chen,Lihua Jia,Tingyu Zhu,Ziyi Zhong,Guangwen Xu,Donghai Mei,Fabing Su
Simultaneously improving both NO x conversion and N 2 selectivity in the selective catalytic reduction of NO by CO (CO-SCR) under O 2 -containing conditions is highly challenging because of the competitive reactions of NO x and CO with O 2 . Here, we demonstrate that the interfacial oxygen vacancies (IOVs) generated at the Co 3 O 4 -CeO 2 heterointerfaces by ball-milling-induced strain can remarkably boost both NO x conversion and N 2 selectivity in the temperature range of 100–400 °C. The Co 3 O 4 -CeO 2 -IOV catalyst achieved approximately 100% NO x conversion and 100% N 2 selectivity (200–350 °C, 1–5 vol% O 2 , and 20,000 h −1 ); even under 10 vol% O 2 , it still showed good catalytic performance. The spectroscopy analysis and theoretical calculations reveal that compared with O 2 activation, IOVs are more favorable for the rate-limiting step of NO adsorption and dissociation. This work provides an effective strategy to create IOVs within metal oxide composite catalysts using ball-milling-induced interfacial strain for improving CO-SCR performance.
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Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Ruixiang Wang,Yanyang Wang,Yanhua Lu,Jiangfeng Zheng,Caini Zhong,Jiaming Liu,Jianjun Liu,Shubiao Xia
Constructing advanced nanostructures and combining various active materials are effective strategies to obtain high-performance anode materials for lithium-ion batteries (LIBs). Herein, we report a surface-coordinated polymerization method to synthesize ZIF-67 nanoparticles with a reuleaux tetrahedron morphology, and combine the electrostatic adsorption method and heat treatment, nitrogen-doped hollow porous Co 3 O 4 (HP-Co 3 O 4 /NC) nanoparticles were anchored on reduced graphene oxide (rGO) to obtain HP-Co 3 O 4 /NC@rGO composites. This deliberate structural design can significantly improve the electrochemical performance of lithium (Li) storage. When applied as an anode material in LIBs, HP-Co 3 O 4 /NC@rGO nanocomposite renders a reversible capacity of 809 mAh g −1 after 200 charge/discharge cycles at a current density of 1000 mA g −1 . The excellent electrochemical performance is mainly attributed to the synergistic effect of the hollow nanostructure and graphene network. A hollow nanostructure can provide abundant active sites and enhance structural stability. As a conductive network, graphene tightly wraps Co 3 O 4 , which can not only increase the electronic and ionic transport but also alleviates the volumetric changes of Co 3 O 4 during the charge/discharge process, thereby improving the rate performance and cyclic stability.
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RSC Advances
·
2022
·Vol. 12
·期 17
·10634-10645
·
IF 4.036
Wenhao Jiang,Junli Wang,Xuanbing Wang,Jiang Liao,Jinlong Wei,Ruidong Xu,Linjing Yang
The conventional Pb–Ag alloy possesses a high oxygen evolution reaction overpotential, poor stability, and short service life in acidic solutions, making it an unsuitable sort of anode material for the zinc electrowinning process. Therefore, a layered carbon-covered cobalt tetroxide (Co3O4@C)-reinforced PbO2-coated electrode is fabricated via a facile two-step pyrolysis-oxidation and subsequent electrodeposition process. As a result, the reinforced PbO2-coated electrode exhibits a low OER overpotential of 517 mV at 500 A m−2 and a Tafel slope of 0.152 V per decade in a zinc electrowinning simulation solution (0.3 M ZnSO4 and 1.53 M H2SO4). The reduced overpotential of 431 mV at 500 A m−2 compared to traditional Pb–0.76%Ag alloy leads to improved energy savings, which is attributable to the presence of Co3O4@C to refine the grain size and thus increase the effective contact area. Moreover, the reinforced PbO2-coated electrode has a prolonged service life of 93 h at 20 000 A m−2 in 1.53 M H2SO4. Therefore, an accessible and efficient strategy for preparing a coated electrode to improve OER performance for zinc electrowinning is presented in this research.
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