Journal of CO2 Utilization
·
2022
·
IF 8.321
Jian-Lei Qi,Qin-Qin Xu,Dan Zhou,Jian-Zhong Yin
Supported single-atom catalytic materials (SACMs) have aroused extensive interest due to their remarkable properties. Herein, a novel method was proffered to prepare Co-NC SACMs using custom-designed N-doped carbon (NC) as support, CoCl 2 as the precursor in supercritical CO 2 with appropriate co-solvent. It was found that when ethanol was used as co-solvent, nanoparticles were obtained while only Co single-atom was obtained when N, N-Dimethylformamide (DMF) was used as co-solvent. Both the theoretical loading and the deposition time influenced the Co loading a lot, and the maximum Co loading was as high as 1.71 wt%. Strong acid, strong alkali, corrosive solvent, and high-temperature treatment were avoided in the whole process. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray photoelectron spectroscopy (XPS), Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES), and Energy Dispersive X-ray spectroscopy (EDX) were conducted to confirm the existence and uniform distribution of Co atoms over the N-doped carbon materials. The conversion rate of 90.0% and selectivity of 86.0% were obtained for the solvent-free selective oxidation of benzyl alcohol to benzaldehyde at 70 °C and 1 h using the Co-NC SACMs.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
npj Clean Water
·
2023
·Vol. 6
·期 1
·1-11
·
IF 11.4
Li Chao,Li Jiale,Huang Niu,Kong Xin Ying,Xiao Qingyi,Huang Yingping,Wong Po Keung,Ye Liqun
Advanced oxidation technology based on peroxonosulfate (PMS) has attracted extensive attention in water treatment research due to its fast reaction speed and wide pH range adaptability. Cobalt-based catalysts are considered to be one of the most effective reagents for PMS activation in various PMS activation methods. However, Co-ion leaching and difficulty in recovery have greatly hindered its practical applications. Herein, we developed a robust membrane constructed by nitrogen-doped carbon nanotubes embedded with cobalt nanoparticles (Co-NC) to concurrently address the Co-ion leaching and recovery issues. Based on our customization, continuous water flow reactor, the Co-NC membrane exhibited excellent catalytic activity and stability, in which it demonstrated a remarkable sterilization efficiency of 99.9999% against E. coli , and it retained a superior stability of 96.29% after 40 repeated cycles. Fewer attempts to put such efficient heterogeneous advanced oxidation processes (AOPs) into practical application, to mimic real-life applications, the performance of the Co-NC/PMS system was extended to the water taken from Qiuxi River. Remarkably, there is no deterioration in performance over 12 h of continuous real sewage processing. Mechanistic studies revealed that abundant high-valence metals (Co IV =O) were generated in the system, which can attack and penetrate into the cell membrane to destroy its intracellular defense system. This work provides useful insights into designing robust membranes with superior efficiency and stability for PMS-based advanced oxidation technology.
研究领域:
环境科学
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水处理技术
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材料科学
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催化
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微生物学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yonghong Wang,Kaixin Wang,Xinru Zhang,Jinping Li
Carbon molecular sieve (CMS) membranes are widely used for the separation of similar molecular kinetic diameter gas. However, their performance is limited by a large amount of discontinuous porous structures and a few adsorption affinity sites. Herein, we first prepared magnetic Co@NC@ZIF-8 nanoparticles , followed by introducing it into the polyimides matrix to design precursor membrane with vertical nanochain-like particle distribution by magnetic field induction. Afterwards, hybrid carbon molecular sieve (HCMS) membranes were prepared by pyrolyzing precursor with high-temperature under N 2 atmosphere, which had ordered microporous architecture and Co-N-C structure. Resultant HCMS membranes prepared by magnetic field induction had excellent gas separation performance, whose CO 2 , N 2 and CH 4 permeabilities were 27,050, 2614 and 622 Barrer, with CO 2 /N 2 , CO 2 /CH 4 and N 2 /CH 4 selectivities of 10.4, 43.5 and 4.2 respectively. These values far exceeded 2019 CO 2 /CH 4 and 2008 N 2 /CH 4 upper bounds as well as approached 2008 CO 2 /N 2 upper bound. The superior performance resulted from the vertically ordered nanochain-like channels for gas transport, which dramatically shortens the transport path of gas molecules to intensify shape sieving potential. Moreover, the Co-N-C structure on the wall of channels could facilitate CO 2 transport due to the π complexation. Additionally, a large quantity of nitrogen sites in the carbonized Co@NC@ZIF-8 enhance CO 2 adsorption selectivity owing to the acid-base interaction. More remarkably, after 30-day aging testing, it was found that HCMS membranes prepared by magnetic field induction had exceptional aging resistance compared to the pristine CMS membranes and one without magnetic field induction under the same aging environments.
研究领域:
材料科学
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化学工程
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膜技术
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气体分离
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yan Chen,Yufan Liu,Huizhen Jin,Xinyue Wang,Guowen Wang,Hongchao Ma,Vadivel Subramaniam,Krishnamoorthy Ramachandran,Xinghui Liu
Antibiotic drugs are biotoxic and difficult to degrade, causing irreversible effects on aquatic environment and human health. The photoelectrocatalytic (PEC) process is regarded as a promising strategy for simultaneously addressing environmental pollution and the energy crisis. Herein, a plum tree-type composite semiconductor photoanode MnOx@Co/NC-x with core-shell heterostructures was constructed to evaluate the PEC activity for sulfamethoxazole (SMX). The synergistic effects of Co nanoparticles, a high content of graphitic N, an open framework, and interfacial structures played a decisive role in improving the PEC activity of the MnOx@Co/NC-x system. The engineered micro-nano structure significantly improved the specific surface area and conductivity of electrode materials, and promoted the diffusion of electrolyte. Among them, MnOx@Co/NC-500 photoanode exhibited the best performance (reached 98.92% in 50 min), cyclic stability and repeatability. The results showed that it was feasible to construct a high-performance heterostructural interface for pollutant treatment based on micro-nano structure regulation and valence band matching.
研究领域:
环境催化
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材料化学
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环境污染治理
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纳米材料
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电化学
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光化学
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药物降解
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Xiangrong Zeng,Hongyu Xiao,Yaxuan Lei,Sifei Ye,Peng Liu,Zhuohua Kong,Yangping Wen,Guixia Tan,Xia Gong,Mingfang Li
The simultaneous electrochemical detection of catechol (CC) and hydroquinone (HQ) isomers is hindered by overlapping voltammetric signals, creating a persistent sensitivity-selectivity-accuracy paradox. Herein, we present a synergistic sensing platform integrating BC-Co@NC nanoarchitectures (engineered via topotactic carbonization to form 3D hierarchical pores with atomically dispersed Co-N 4 sites) and a first- and second-derivative voltammetry cascade (FS-DVC) optimized by Savitzky-Golay algorithm. This dual-engine strategy achieves 152 mV interpeak separation, ultra-low limits of detection (0.09 nM for CC, 0.12 nM for HQ), a linear range spanning four orders of magnitude (0.3-500 μM), and robust performance in environmental matrices (95.2-99.1% recoveries in agricultural water/soil). This work establishes a new paradigm for electrochemical isomer discrimination through the synergistic fusion of tailored material design and advanced signal mathematics.
研究领域:
电化学
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纳米材料
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分析化学
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信号处理
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环境监测
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产品关联
DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Bin Li,Biao Ma,Mengying Wei,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Recycle of the spent lithium-ion batteries (LIBs) can reuse the toxic heavy metals for the synthesis of useful materials. In this study, the cobalt metal is obtained by recycling the cathodes of spent LIBs, which is then used as cobalt source for the synthesis of highly porous Co-NC composites. Attributing to the addition of EDTA-2Na and NaNO 3 as chelate agent and activation agent respectively, very large surface areas (>3700 m 2 /g) and highly porous structure can be achieved. These composites can activate peroxymonosulfate (PMS) effectively for the degradation of bisphenol A (BPA) in aqueous solution. The optimized Co-NC/PMS system also shows good performance in a wide pH range and great tolerance to different inorganic ions and NOMs. Radical scavenging experiments and EPR results prove that 1 O 2 is the only functional reactive oxidation species (ROS) for BPA degradation. A generation route of PMS – *OH – *O – 1 O 2 for 1 O 2 is also simulated and proved by DFT calculation. This work provides a novel way to synthesize effective catalysts for PMS activation from the environmental wastes.
研究领域:
环境科学
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材料科学
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催化
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废物管理
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaoli Peng,Long Yuan,Shilan Li,Shengdong Jing,Yaozhu Tian,Zhu Luo,Yufei Zhang,Haosen Fan
Lithium‑sulfur batteries (LSBs) have attracted much attention due to their high theoretical energy density (2600 Wh kg −1 ) and low cost of sulfur cathodes. However, their practical application is hindered by the significant polysulfide shuttle effect and sluggish redox kinetics. To address these challenges, a Co-NC/Nb 2 O 5 heterostructure was successfully prepared through high-temperature annealing of a ZIF-67 precursor followed by hydrothermal growth of Nb 2 O 5 nanocrystals on the surface of Co -embedded and N-doped carbon polyhedrons (Co-NC). The unique structure features a hierarchical conductive framework with uniformly dispersed Nb 2 O 5 nanoparticles and defect-rich carbon matrix, which synergistically enhances sulfur utilization and ion diffusion. Numerous dangling bonds and defective sites exist on the Nb 2 O 5 surfaces, and its Lewis acidic site (Nb 5+ ) can inhibit the solvation and shuttling of LiPSs through strong chemical interactions with the S atoms of polysulfides via Nb-O-S bonds. The catalytic and adsorption mechanisms were explained by density functional theory (DFT) calculations and experimental results. Consequently, LSBs cells equipped with Co-NC/Nb 2 O 5 modified separators demonstrated exceptional electrochemical performance with a rate capability that provides a reversible capacity of 761.8 mAh g −1 at 3 °C. The composite of MOF-derived hollow carbon polyhedra decorated with Nb 2 O 5 nanoparticles ensured fast electron transfer, achieving a reversible capacity of 731.4 mAh g −1 after 500 cycles at 1C and 501.6 mAh g −1 after 1000 long cycles at 2C, with a capacity decay rate of only 0.03 % per cycle. Excellent electrochemical performance was maintained with a high sulfur loading cycling performance of 5 mg cm −2 at a low electrolyte/sulfur condition of 7 μL mg −1 . This work provides new insights into the development of high energy density LSBs and the advancement of next generation energy storage systems through precise electronic structure design at the heterojunction interface.
研究领域:
储能材料
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电化学
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纳米材料
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表面化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 1
·169-178
·
IF 8.64
Wei Haisheng,Song Huaxing,Ren Yujing,Yan Xiaorui,Fang Geqian,Wang Wenhua,Ren Wanzhong,Zhu Mingyuan,Lin Jian
Metal-organic frameworks (MOFs) derived Co-based catalysts have received extensive attention in the chemoselective hydrogenation of nitroarenes, while they usually require a lot of solvent during the synthesis and identification of active species. This study explores a solid-phase synthesis strategy to obtain MOF precursors without using any solvent, which is then foamed and pyrolyzed to synthesize the Co@NC-X catalyst. It was found that a nitrogen-doped graphene shell can well encapsulate the Co nanoparticles. The resulting catalyst, which was pyrolyzed at 800°C, exhibited ~100% conversion for the hydrogenation of 3-nitrostyrene and >99% selectivity to 3-vinylaniline. This catalyst also showed excellent stability and good substrate universality for the hydrogenation of extensive substituted nitroarenes. Various characterizations revealed a positive relationship between the catalytic performance and the content of Co—N species tuned by pyrolysis temperature. This work provides a novel and green strategy to design an efficient Co-based catalyst for chemoselective hydrogenation.
研究领域:
催化
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材料科学
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化工
·
绿色化学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 56
·12882-12890
·
IF 4.857
Qiongguang Li,Yanhong Wang,Qiangqiang Tan,Ziyi Zhong,Fabing Su
Graphical Hollow core–shell anode : An SnO 2 @C@Co-NC anode material with hollow core–shell structure was structurally designed and synthesized by a heteroatom-doping and multiconfinement approach. This material can efficiently alleviate the volume expansion of the SnO 2 -based anode materials and exhibits much-enhanced electrochemical performance, including high rate performance and cycle stability, as well as superior capacity. To overcome the drawbacks of the structural instability and poor conductivity of SnO 2 -based anode materials, a hollow core–shell-structured SnO 2 @C@Co-NC (NC=N-doped carbon) composite was designed and synthesized by employing the heteroatom-doping and multiconfinement strategies. This composite material showed a much-reduced resistance to charge transfer and excellent cycling performance compared to the bare SnO 2 nanoparticles and SnO 2 @C composites. The doped heteroatoms and heterostructure boost the charge transfer, and the porous structure shortens the Li-ion diffusion pathway. Also, the volume expansion of SnO 2 NPs is accommodated by the hollow space and restricted by the multishell heteroatom-doped carbon framework. As a result, this structured anode material delivered a high initial capacity of 1559.1 mA h g −1 at 50 mA g −1 and an initial charge capacity of 627.2 mA h g −1 at 500 mA g −1 . Moreover, the discharge capacity could be maintained at 410.8 mA h g −1 after 500 cycles with an attenuation rate of only 0.069 % per cycle. This multiconfined SnO 2 @C@Co-NC structure with superior energy density and durable lifespan is highly promising for the next-generation lithium-ion batteries.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TRANSITION METAL CHEMISTRY
·
2025
·
IF 1.7
Wang Yuqin,He Lizi,Han Ning,Li Lishuang,Wang Meiyang
It is of great practical significance to explore and prepare cheap, high-performance, and stable catalysts for oxygen reduction reaction (ORR), but it is still in progress at present. Herein, a straightforward evaporation–pyrolysis strategy is designed for the preparation of 3D porous electrocatalysts (denoted as \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) , which represented carbonization products at °C) made of carbon nanoparticles combined with metallic Fe-Co-doped N-enriched bridged carbon nanotube by carbonization of a pristine ZIF8 as highly efficient and durable ORR electrocatalysts. The obtained Fe–Co–NC structure possesses 3D open porous texture, abundant active sites, desired nitrogen bonding type, and high specific surface area, providing them with excellent ORR activity. The optimal performing \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) catalyst presents an outstanding ORR performance in terms of a high onset potential ( \(\textrm{E}_{\text{ onset } }\) ) of 0.96 V (vs. RHE) and half-wave potential ( \(\textrm{E}_{1 / 2}\) ) of 0.86 V (vs. RHE), respectively, possible to rival those of the commercially available \(\textrm{Pt} / \textrm{C}\) in an alkaline electrolyte solution. Besides, the \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) catalyst manifests better stability than those of commercially available \(\textrm{Pt} / \textrm{C}\) , which is of importance for the optimization and characterization of novel electrocatalysts originated from non-precious metals.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Le Zhou,Xin Zhang,Yu Han,Xin Li,Ze-Quan Zeng,Hai-Kui Zou,Yong Luo
The Co@NC catalyst exhibits significant protic solvent preference for hydrogenation of nitriles to primary amines. However, the effect of mixed protic solvents on catalytic hydrogenation has received little attention. Herein, the synergetic solvent effect has been proposed to accelerate the hydrogenation of adiponitrile (ADN) to hexamethylenediamine through H 2 O-ethanol hydrogen bond networks on Co@NC catalyst. Experimental screenings on solvents showed that ADN conversion in H 2 O-ethanol was 1.6 ~ 5.1 times greater than in single solvents. Kinetic models in H 2 O/ethanol ( v W = 0.6), H 2 O, and ethanol showed that the solvents effected on H 2 transformation dominated the reaction. Isotope labelling and kinetic experiments revealed that H 2 O and ethanol acted as co-catalysts through exchanging and transferring hydrogen via hydroxyl groups. Density functional theory calculations confirmed that the energy barrier for proton transfer mediated by H₂O–ethanol was reduced by 0.18 eV compared to proton transfer mediated by H₂O–H₂O dimers.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 9
·090514
·
IF 4.316
Xiaochao Liu,Siyuan Peng,Xiaoxiao Li,Chao Liu,Jinming Zeng,Xiaopeng Qi,Tongxiang Liang
The development of low-cost, high catalytic activity oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalysts is the key to promoting the development of zinc-air batteries. In this paper, a simple one-step pyrolysis method was used to successfully synthesize a binary FeCo–Co/NC catalyst with FeCo and Co nanoparticles encapsulated in N-doped carbon nanotubes. This structure exhibits great characteristics: it has a variety of active species (FeCo, Co, NC), and there is close combination between these active species (FeCo, Co, NC). Electrochemical studies have shown that the initial potential of FeCo–Co/NC during ORR process is 0.93 V, the half-wave potential is 0.808 V, and the limiting current density is 4.94 mA cm−2. In the OER process, at an anode current density of 10 mA cm−2, an overpotential of only 353 mV is shown; a lower Tafel slope and good durability are also observed. Moreover, the zinc-air battery in preparation can be cycled for as long as 2000 times. This provides a new method for the preparation of high-efficiency dual-function electrocatalysts for OER and ORR.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）