JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Yujie Wang,Chen Yan,Yu Bingliang,Yaru Yang,Ningru Wang,Jingren Yang,Bin Li,Yanwei Li,Xing Xu
Developing efficient and eco-friendly technologies for treating the antibiotic wastewaters is crucial. At present, the catalysts with metal-nitrogen (M-N x ) coordination showed excellent Fenton-like performance but were always difficult to realize practical antibiotics degradation because of their complicated preparation methods and inferior stability. In this work, the Co-N x configuration was facilely reconstructed on the surface of Co 3 O 4 (Co-N x /Co 3 O 4 ), which exhibited superior catalytic activity and stability towards various antibiotics. DFT results indicated that stronger ETP oxidation will be triggered by the electron-donating pollutants since more electrons can be easily migrated from these pollutants to the Co-N x /Co 3 O 4 /PMS complex. The Co-N x /Co 3 O 4 /PMS system could maintain superior oxidation capacity, high catalytic stability and anti-interference due to (i) the strong nonradical ETP oxidation with superior degradation selectivity in Co-N x /Co 3 O 4 /PMS system, and (ii) the synchronously enhanced radical oxidation with high populations of non-selective radicals generated via activating PMS by the Co-N x /Co 3 O 4 . As a result, the synergies of synchronously enhanced dual oxidation pathways guaranteed the self-cleaning properties, maintaining 98 % of activity after eight cycles and stability across a wide pH range. Basically, these findings have significant implications for developing technologies for purifying antibiotic wastewater.
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 20
·11991-11997
·
IF 3.269
Liang Jiang,Peng Zhou,Zehui Zhang,Quan Chi,Shiwei Jin
The application of earth-abundant transition metal catalysts in the mild and selective synthesis of secondary amines via the reductive amination method is very challenging. In this regard, we have developed a new method for the reductive amination of carbonyl compounds with nitro compounds over a heterogeneous Co–nitrogen (Co–Nx) catalyst under mild conditions (110 °C and 10 bar H2). This method afforded the corresponding secondary amines with the yields of 43.7–100% at 110 °C and under 10 bar H2 pressure. Kinetic studies revealed that the hydrogenation of imines was the rate-determining step with much higher activation energy than the first step of the hydrogenation of nitro compounds. To the best of our knowledge, no such non-noble heterogeneous catalyst that shows very high catalytic activity under mild conditions (110 °C and 10 bar H2) has been reported to date. This promising cheap heterogeneous catalyst allows an efficient domino reductive amination of carbonyl compounds with nitro compounds.
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高影响因子
ACS Nano
·
2021
·
IF 15.881
Ting Huang,Yingjie Sun,Jianghua Wu,Jia Jin,Chaohui Wei,Zixiong Shi,Menglei Wang,Jingsheng Cai,Xing-Tao An,Peng Wang,Chenliang Su,Ya-yun Li,Jingyu Sun
Although lithium–sulfur (Li–S) batteries have long been touted as next-generation energy storage devices, the rampant dendrite growth at the anode side and sluggish redox kinetics at the cathode side drastically impede their practical application. Herein, a dual-functional fibrous skeleton implanted with single-atom Co–Nx dispersion is devised as an advanced modificator to realize concurrent regulation of both electrodes. The rational integration of single-atomic Co–Nx sites could convert the fibrous carbon skeleton from lithiophobic to lithiophilic, helping assuage the dendritic formation for the Li anode. Meanwhile, the favorable electrocatalytic activity from the Co–Nx species affording a lightweight feature effectively enables expedited bidirectional conversion kinetics of sulfur electrochemistry, thereby inhibiting the polysulfide shuttle. Moreover, the interconnected porous framework endows the entire skeleton with good mechanical robustness and fast electron/ion transportation. Benefiting from the synergistic effects between atomically dispersed Co–Nx sites and three-dimensional conductive networks, the integrated Li–S full batteries can achieve a reversible areal capacity (>7.0 mAh cm–2) at a sulfur loading of 6.9 mg cm–2. This work might be beneficial to the development of practically viable Li–S batteries harnessing single-atom mediators.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Ming Zeng,Haiting Shi,Wenhui Cui,Xianyan Wu,Shuaitong Liang,Wei Wang,Nishonov Akbarjon,Zhiwei Xu
Non-precious metal catalysts have emerged as the leading candidate to replace platinum-based catalysts due to their cost-effectiveness. However, the sluggish oxygen reduction kinetics and inadequate durability limit their application in zinc-air battery technology. Herein, we demonstrate a facile strategy to construct a hierarchical architecture of N-doping γ-graphyne-supported carbon nanotubes encapsulating cobalt nanoparticles (Co@N-CNT/N-GY). This unique structure prevents the aggregation and exfoliation of nanoparticles, thereby enhancing the catalysts durability. Synchrotron radiation absorption spectroscopy confirms the presence of Co-N x coordination in Co@N-CNT/N-GY, which contributes to promote the oxygen reduction reaction. Density-functional theory calculations further reveal that nitrogen doping in carbon nanotubes induces substantial charge redistribution among adjacent carbon atoms, facilitating the formation of the OOH* intermediate and lowering the overall Gibbs free energy barrier. Moreover, the open-pore architecture of N-doping γ-graphyne promotes the rapid diffusion of dissolved oxygen and creates abundant gas-liquid-solid interfaces, thereby boosting the Oxidation-reduction reaction (ORR) kinetics. As a result, the Co@N-CNT/N-GY catalyst delivers a high specific capacity (723 mAh g −1 ) and excellent power density (135.86 mW cm −2 ) when employed in a zinc-air battery. This study provides valuable insights for designing the γ-graphyne-supported non-precious metal ORR electrocatalyst with high activity and durability.
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高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jian Tang,Yujie Wang,Jun Ma,Yujie Chen,Ming Chen
In this study, we selected rice straw, wheat straw and corn cob as raw materials to successfully prepare cobalt-nitrogen co-doped biomass-based carbon nanotubes composites (BM@CoNCNTs) with Co-N x sites highly dispersed on porous biochar carrier, which could effectively activate peroxymonosulfate (PMS) to remove tobacco mosaic virus (TMV) in water. Particularly, BM@CoNCNTs-CC, with its confined carbon nanotubes and high-density Co-N x sites, enhanced the Co 2+ /Co 3+ cycle and direct adsorption of PMS to generate Co(IV)=O and 1 O 2 , playing a dominant role. This led to the effective disruption of TMV coat protein and degradation of its genome within 5 min, achieving up to 6 log 10 removal efficiency. Additionally, BM@CoNCNTs-CC/PMS system maintained efficient catalytic removal performance even in complex water matrices (river water and tap water). Overall, our research not only elucidates the production of efficient biomass-based catalysts for environmental remediation, but also highlights the application potential of biomass-based carbon nanotubes composites enriched with Co-N x sites.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·740-751
·
IF 12.732
Lichong Peng,Yaxin Sun,Shiquan Guo,Congju Li
Oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) involve proton coupled electron transfer reaction (PCET), resulting in sluggish redox kinetics. At present, the development of high-efficiency bifunctional oxygen electrocatalysts is still a puzzling challenge. Herein, we propose a scalable strategy for embedding and beading ZIF-derived hollow Co–Nx nanocube cage dispersion implanted with porous carbonized nanofibers (EH/PCNFs and BH/PCNFs) through electrospinning and annealing. The cobalt species prevent themselves from agglomerating during the annealing process through the “fence” effect of the non-volatile Zn species, thereby synergizing with ligand volatilization to facilitate the formation of Co–Nx nanocube cages. Benefiting from the ultralong interconnected multi-layered carbon nanofiber matrix, the hollow Co–Nx nanocube cages can change the charge density and electron distribution of the carbon nanofiber matrix, endowing the carbonized nanofiber carrier with special surface polarization and accelerating the electrocatalytic kinetics. Remarkably, the integrated Li–O2 batteries (LOBs) based on BH/PCNFs and EH/PCNFs electrodes exhibit significantly decreased charge/discharge polarization (0.79 V) and a long-term cyclability (147 cycles) under a cut off capacity of 500 mA h g−1 at 200 mA g−1. This work might be beneficial for the practically viable design and manufacture of dual-function oxygen electrocatalysts.
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高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Mingzhu Wang,Shuyu Yue,Xingyun Zhao,Yaoyan Wu,Yaohui Zhang,Yaqian Dong,Tiehua Ma
Developing highly efficient and durable trifunctional electrocatalysts is essential for advancing technologies related to water splitting, oxygen reduction, and hydrogen storage, which are critical for energy conversion and storage. In this study, we encapsulated Co-MOFs on the surface of Mo2C hollow spheres and achieved the Co@NC/Mo2C composite material through high-temperature annealing. In the optimal catalyst, Co@NC/Mo2C-0.1, Co@NC nanosheets were uniformly distributed on the Mo2C hollow spheres, and the BET surface area was well maintained. Compared to Co nanoparticles, Co-Nx in Co@NC/Mo2C-0.1 exhibited a greater modulation effect on the electronic structure of Mo2C. Density functional theory (DFT) calculations showed that the Co@NC/Mo2C heterostructure effectively lowered the energy barrier for the hydrogen evolution reaction (HER) on Mo2C and enhanced the performance of the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) through electronic coupling. Specifically, for Co@NC/Mo2C-0.1, at a current density of 10 mA cm–2, the half-wave potential for ORR was 0.86 V, the overpotential for OER was 349 mV, and the overpotential for HER was 158 mV. Additionally, this catalyst exhibited exceptional stability across all three reactions, making it an ideal candidate for sustainable energy technologies.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Hao Han,Xiaomei Wang,Xu Zhang
Reasonable design and construction of efficient and stable catalysts with abundant metal-N x active sites are the focus of oxygen reduction reaction (ORR) research. In this work, a type of catalyst with isolated single-atomic Co sites embedded in the ultra-thin pore walls of hierarchically ordered porous N-doped carbon (ISA-Co/HOPNC) by a simple single template pyrolysis strategy has been successfully synthesized. The interconnected macropores introduced by the silica colloidal crystal template (CCT) not only improve the mass transmission of molecules and ions to achieve the accessibility of internal Co-N x active sites, but also promote the complete removal of inactive Co species nanoparticles (NPs) inside the catalyst. Removal of inactive Co species NPs that form mesopores in the ultra-thin walls of the macropores increases the specific surface area to expose more active sites. In comparison with the commercial 20 wt% Pt/C, the optimal ISA-Co/HOPNC-0.3 catalyst shows comparable ORR activity, but much higher methanol tolerance and cycle stability. The remarkable ORR performance of ISA-Co/HOPNC-0.3 can be attributed to the numerous exposed single-atomic Co-N x active sites, as well as the high surface area and efficient mass transport from the 3D hierarchically ordered porous structure.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Qianer Xu,Haifeng Zhou,Qunli Tang,Aiping Hu,Yali Xu,Yuping Shen,Chao Kang,You Zhou,Xiaohua Chen
Sluggish reaction kinetics of lithium-sulfur (Li-S) battery is the key issue affecting cycle capacity and rate performance. Highly conductive and catalytically active sulfur host is still a research hotspot in recent years. Herein, the sulfur host of Co nanoparticles anchored on the Co-N x active centers grafted nitrogen-doped graphene (Co/Co-N x @NG) with high catalytic activity and electrical conductivity was prepared via a simple and feasible in situ method. The cobalt-based nanocatalytic center exhibits efficient sulfur conversion efficiency. Moreover, the Co-N x coordination group is beneficial to inhibit the agglomeration of cobalt nanoparticles to form large particles and further improve the catalytic activity. In addition, the graphene structure formed at low temperature based on the two-dimensional guide of dicyandiamide in combination with the catalytic graphitization of cobalt nanoparticles has excellent electrical conductivity. Owing to the high catalytic activity, appropriate adsorption ability, and excellent electrical conductivity, the Co/Co-N x @NG applied as sulfur cathode matrix exhibits high capacities of 1300.3 mA h g −1 at 0.1 C and 884.2 mA h g −1 at 2 C, and good cycling stability with a capacity decay of only 0.069% per cycle at 2 C for 705 cycles.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 32
·期 12
·e4570
·
IF 3.581
Xiaobin Dong,Chaoyue Zhao,Qingxin Guan,Wei Li,Xiufang Xu
Industrial production of vinyl chloride through acetylene hydrochlorination is a dominating technique in coal-rich areas, but its development is severely restricted by the use of toxic mercury chloride (HgCl 2 ) catalyst. Inspired by the fact that doped carbon materials active in acetylene hydrochlorination often have good performance in the oxygen reduction reaction, a series of cobalt and nitrogen co-doped porous carbon catalysts prepared by pyrolysis of bimetallic ZIFs based on ZIF-8 and ZIF-67 under N 2 were applied in acetylene hydrochlorination. The catalytic activities of the co-doped catalysts varied with Co addition, and the highest acetylene conversion could be up to 83% with a space velocity of 2.6 ml g −1 min −1 at 220°C when a small amount of cobalt was introduced. Results of several characterizations confirmed the existence of Co–N x in the co-doped carbons, pointing out that this coordination structure makes the catalysts have better ability to adsorb and activate C 2 H 2 . Density functional theory calculation finally proved that C atom adjacent to the N atom in Co–N 4 structure is the primary active site in co-doped catalysts with high activity. We also conclude that the decreased N content caused by Co 2 N decomposition and the coordination structure change of Co–N x should be responsible for the gradually worsening performances of the carbon catalysts with further Co addition. Our study provides a new route for improving the performance of N-doped carbon material in acetylene hydrochlorination and thus enhances its potential for practical application.
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高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wenfei Dong,Guo Chen,Mengyao Ding,Haiyan Cao,Gaoya Li,Meiqing Fang,Wenbing Shi
Nanozyme-based sensing strategy for glucose generally involves a two-step H 2 O 2 -bridged cascade reaction . However, this two-step cascade reaction always shows a limited detection efficiency for glucose, which hardly makes simply operation, rapid detection, and sensitivity all promised. Herein, a novel strategy for one-step glucose detection was proposed based on the efficiently competitive relationship between glucose oxidase catalyzed glucose oxidation and oxidase nanozyme catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB) colorimetric oxidation. As a proof of concept, Co-Nx sites on porous carbon (Co-Nx/PC) derived from ZIF-67 was selected as the oxidase nanozyme with O 2 -sensitive nature, which can activate O 2 to produce 1 O 2 for TMB colorimetric oxidation. In the presence of glucose, the competitive reaction of glucose oxidase catalyzed glucose oxidation occurs, which will obviously inhibit the Co-Nx/PC catalyzed TMB colorimetric oxidation to construct method for glucose detection. The usage of the same reactant O 2 and the production of suppressive H 2 O 2 cause a dual effect to this inhibition. In addition, the available pH range of Co-Nx/PC overlaps with that of glucose oxidase, promising a one pot reaction . The proposed method with Co-Nx/PC as oxidase nanozyme based on one-step competitive strategy for glucose detection possesses high detection efficiency with convenience (one-pot), rapidness (total reaction time of 10 min) and sensitivity (LOD of 0.31 μM) all promised, which is superior among the methods based on two-step one-pot or two-pot cascade strategy. The strategy can be successfully applied into the blood glucose detection in human serums with satisfactory results. Also, the strategy can be scalable to other oxidase nanozyme like Mn 3 O 4 .
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Yunyun Dong,Lin Gu,Chenghuan Wang,Yuchang Du,Wang Bo,Hongmei Du,Yanlan Wang,Jinsheng Zhao
The preparation of non-noble metal catalysts with performance in the oxygen reduction reaction (ORR) comparable or superior to platinum-based catalysts remains challenging. In the present study, hexaazatriphenylenehexacarbonitrile (HAT-CN), which is rich in both cyano groups and pyrazine units, was used as the precursor and then cyclotrimerized into a covalent triazine-based framework with a macrocyclic structure containing abundant complexation sites for transitional metal ions. Subsequently, a series of non-platinum Co N C type catalysts (HAT-CN-Co/C) were prepared, and then pyrolyzed at different temperatures (700 °C, 800 °C, and 900 °C). The pyrolysis treatment endowed the catalysts with activated Co-N x sites, large pore sizes and high specific surface areas, which can promote oxygen transfer and accelerate the ORR catalytic process. It is found that the catalyst (HAT-CN-Co/C-800) obtained from pyrolysis at 800 °C possessed the best ORR activity and followed the four- electrons transfer pathway; the onset potential of ORR was determined as 0.972 V vs reversible hydrogen electrode (RHE), very close to that of Pt/C (0.993 V vs RHE), and the half-wave potential (0.895 V vs RHE) was significantly higher than that of Pt/C (0.859 V vs RHE). Furthermore, the HAT-CN-Co/C-800 catalyst showed good durability (83.2 % current retention after 28000 s) and significant methanol tolerance with good application potential as a substitute for the platinum-based ORR catalyst in fuel cell.
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高影响因子
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