APPLIED SURFACE SCIENCE
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2023
·
IF 6.7
Guangda Zhou,Xiaoli Yan,Tianyu Zhang,Kui Wang,Jingtao Zhang,Junjie Guo
The rational design and construction of the hierarchical porous structure of carbon framework to support transition metal-based catalysts is critical to increase their active sites density and facilitate mass/electron transport. Herein, we report a novel nanocapsules with cobalt core and nitrogen-doped carbon shells (Co@NC) supported on MOFs-derived hierarchical porous carbon framework. The rational hierarchical porous carbon framework with controllable size and micropore/mesoporous ratio was achieved by one-step pyrolysis of Zn(acac) 2 ·phen ligand and ZIF-67 precursor, which is beneficial for the mass transport in the oxygen reduction reaction (ORR). The 0.4Co@NC-900 electrocatalyst display a distinguished ORR activity in the pH-universal range, with a half-wave potential of 0.91 V in alkaline and 0.76 V in acid electrolytes. The excellent ORR performance of our electrocatalyst can be attributed to its optimized micropore/mesoporous ratio of carbon framework with efficient mass transport, together with the graphitized carbon shell on Co nanoparticles which not only enhances the electron/proton transport, but also suppresses the chemical corrosion of the Co nanoparticles. Impressively, the Zinc-air battery as air electrode offers peak power density of 203 mW cm −2 and long-term stability of 130 h, showing an excellent battery performance. This study offers a fresh method of constructing ORR catalysts with increased activity and durability over a universal pH range.
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高影响因子
Green Energy & Environment
·
2020
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IF 6.395
Qiongguang Li,Yanhong Wang,Jing Yu,Menglei Yuan,Qiangqiang Tan,Ziyi Zhong,Fabing Su
To mitigate the massive volume expansion of Si-based anode during the charge/discharge cycles, we synthesized a superstructure of Si@Co–NC composite via the carbonization of zeolite imidazolate frameworks incorporated with Si nanoparticles. The Si@Co–NC is comprised of Si-nanoparticle core and N-doped/Co-incorporated carbon shell, and there is void space between the core and the shell. When using as anode material for LIBs , Si@Co–NC displayed a super performance with a charge/discharge capacity of 191.6/191.4 mA h g −1 and a coulombic efficiency of 100.1% at 1000 mA g −1 after 3000 cycles, and the capacity loss rate is 0.022% per cycle only. The excellent electrochemical property of Si@Co–NC is because its electronic conductivity is enhanced by doping the carbon shell with N atoms and by incorporating with Co particles, and the pathway of lithium ions transmission is shortened by the hollow structure and abundant mesopores in the carbon shell. Also, the volume expansion of Si nanoparticles is well accommodated in the void space and suppressed by the carbon host matrix. This work shows that, through designing a superstructure for the anode materials, we can synergistically reduce the work function and introduce the confinement effect , thus significantly enhancing the anode materials' electrochemical performance in LIBs.
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ELECTROCHIMICA ACTA
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2025
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IF 5.6
Haoqi Liang,Yutong Yang,Yijia Wang,Zejun Deng
Escalating aquatic contamination by toxic heavy metal ions (HMIs) urgently requires field-deployable electrochemical sensors surpassing traditional methods. This work proposed a controllable synthesis of cobalt-embedded nitrogen-doped carbon/carboxyl-functionalized multi-walled carbon nanotube (Co@NC/CMWCNTs) composites through in situ growth of ZIF-67 on CMWCNTs, followed by optimized carbonization. CMWCNTs-directed morphological evolution was systematically demonstrated, revealing that with increasing CMWCNT ratios, the ZIF-67 crystallite size underwent an initial increase and later decay, and after carbonization, a unique knot-like interpenetrating architecture was formed with CMWCNTs as bridges and Co@NC as nodes. This synergistic structure significantly enhanced electrical conductivity and electrocatalytic activity, as evidenced by electrochemical characterization. Compared to the glassy carbon electrode (GCE), the Co@NC/CMWCNTs/GCE sensor exhibited a 12-fold reduction in charge transfer resistance (28.3 Ω vs. 346.8 Ω), a 21% larger electroactive surface area, and rapid heterogeneous electron transfer kinetics of 3.8 × 10⁻³ cm s -1 . The composite sensor allowed simultaneous detection of Cd²⁺, Pb²⁺, Cu²⁺, and Hg²⁺ in 0.1 M NaAc-HAc buffer (pH 4.5) with high sensitivities (169.7, 199.0, 135.9 and 108.0 μA·μM⁻¹ cm -2 ), low detection limits (40.0, 40.5, 87.5 and 106.2 nM) and observed cross-interference within 10%. This work establishes a materials design paradigm for MOF-derived electrochemical sensors for low-cost on-site environmental monitoring of HMIs.
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Journal of Water Process Engineering
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2023
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IF 7
Juan Miao,Peipei Wang,Xinquan Zhou,Ning Zhang,Ruichang Zhang,Xuefeng Wei,Shuge Peng
Loading metal on N-doped C material is an effective way of improving the activation efficiency of heterogeneous catalysts for persulfate. Many studies have explored the intrinsic relationship between material modification and enhanced activation efficiency from various aspects. In this study, a cobalt oxide/polypyrrole (Co 3 O 4 /PPy) derived Co/NC composite catalyst has been synthesized and used for the activation of PMS. The mechanism study showed that Co/NC can enhance the oxidation efficiency of the reaction system by improving the conversion efficiency of PMS to free radicals . Furthermore, the mechanism of the effect of physicochemical properties of Co/NC (electron transfer capacity, functional bonds, structural texture, etc.) on the conversion of PMS to free radical was explored by regulating the ratio of PPy and metal Co. This study can provide a new catalyst synthesis strategy for the efficient formation of free radicals in heterogeneous persulfate activated systems.
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Science China-Materials
·
2022
·Vol. 66
·期 1
·169-178
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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.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Runmin Huang,Dan Liao,Zhenhua Liu,Jingang Yu,Xinyu Jiang
Construction of high-sensitive analytical platform to monitor organic pollutants in the environment is of significance. Nitrophenol is toxic organic pollutant, causing serious damage to biosphere. Herein, a simple self-assembled method was proposed to design a novel heterostructure (MXene/ ZIF) composed of Nb 2 CT X and Zn-Co-ZIFs derived bimetallic Zn, Co embedded N-doped carbon (Zn-Co-NC) nanocage. The Nb 2 CT X / Zn-Co-NC composite modified electrodes were applied for the electrochemical detection of 4-nitrophenols (4-NP). SEM images revealed that the insertion of Zn-Co-NC can effectively avoid Nb 2 CTx from restacking. EDS and XPS demonstrated the successful synthesis of bimetallic Zn, Co embedded N-doped carbon nanocage. Excellent conductivity and large specific surface area of Nb 2 CTx as well as superior catalytic activity of Zn-Co-NC nanocage enhance the electrochemical performance of Nb 2 CTx/ Zn-Co-NC sensor. Under optimal conditions, the achieved wide linear range was 1 μM to 500 μM. The low detection limit of 0.070 μM with high sensitivity of 4.65 μA μM −1 cm -2 was obtained. Furthermore, the Nb 2 CTx/ Zn-Co-NC sensor holds outstanding selectivity and stability. Therefore, the innovative structure and excellent properties of MXene/ ZIF make them alternative materials for various electrochemical sensors for the detection of other toxic organic pollutants.
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ChemCatChem
·
2021
·Vol. 13
·期 24
·5166-5177
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IF 5.686
Chuanhui Li,Ye Meng,Song Yang,Hu Li
Graphical Access to bio-nitrogenous chemicals : A Co-embedded N-doped carbon nanocatalyst can efficiently promote Leuckart-type reductive amination of biomass-derived carbonyls to prepare N-formyl compounds, which benefits from the synergy of its Co NPs and N base sites. The initial formation of the C−N bond occurs between carbonyls and H 2 NCHO rather than HCOONH 4 . It is of great significance to develop non-precious metal catalysts with excellent catalytic activity, stability, and acid resistance for biomass valorization. Herein, catalytic amination of biomass carbonyl compounds was achieved via a Leuckart-type reaction over Co nanoparticles (NPs) embedded N -doped carbon catalyst, which was prepared by thermolysis of ZIF-67 precursor at different temperatures in the N 2 atmosphere. The Co/NC-800 catalyst exhibited excellent catalytic activity and recyclability in furfural reductive amination to mono-substituted formamide, which was attributed to the synergistic catalytic action of Co NPs and nitrogen base sites of the catalyst. The reductive amination mechanisms were elucidated by theoretical calculations, and showed that the initial formation of C−N bond was derived from the condensation of furfural and formamide, followed by dehydration to form C=N double bond, which was then reduced by hydrogen species Co−H − and NH + . The developed catalytic system was applicable to different carbonyls for the synthesis of corresponding N -formyl compounds with up to 99 % yield.
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CARBON
·
2022
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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.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 56
·12882-12890
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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.
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PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2026
·
IF 4.6
Yu Wang,Danyang Wu,Jiao wu,Xizhen Zhang,Yongze Cao,Baojiu Chen
We breakthrough the conventional high-temperature paradigm for synthesizing transition metal catalysts by discovering 500 °C as a critical metastable window in ultrafast (>1500 °C/s) Joule heating synthesis. This kinetically confined thermal shock at precisely 500 °C uniquely terminates metal aggregation while locking abundant pyridinic-N sites (2.86 at.%) that effectively anchor highly dispersed Fe and Co species, simultaneously sculpting a defect-rich carbon matrix. This unique combination, inaccessible in traditional pyrolysis, unlocks exceptional synergistic activity. Consequently, the 500 °C-engineered NC-FeCo catalyst achieves an oxygen reduction record: half-wave potential (0.92 V) surpassing Pt/C (0.85 V) and 1500 °C-treated analogs (0.85 V), while delivering near-theoretical 4e − selectivity (<1.2% H₂O₂), negligible decay (ΔE = 3 mV/5000 cycles), and superior methanol tolerance. Our work establishes sub-second 500 °C thermal shock as an innovative platform for metastable dual-metal electrocatalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Shunli Li,Chenxi Xu,Qiulan Zhou,Zhen Liu,Zhixiong Yang,Yu Gu,Yaping Ma,Weijian Xu
Designing high-efficiency catalysts with earth-abundance elements for overall water splitting (OWS) in alkaline electrolyte has been unsettled owing to the non-negligible overpotential of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). An electrocatalyst with decent HER and OER activities in the same electrolyte is crucial for sustainable energy storage and conversion device. In this work, a nitrogen-doped porous carbon confined yolk/shell OWS catalyst of WC/Co 3 W 3 N/Co@NC has been prepared via calcination polyhedron encapsulation structure PW 12 @ZIF-8 @ZIF-67 generated by the epitaxial method. Because of the optimized chemical composition , the derived WC/Co 3 W 3 N/Co@NC multisite catalyst has outstanding OWS performance in 1 M KOH solution. For example, to reach a current density of 10 mA cm -2 , it only needs low overpotentials of 141 and 280 mV for the HER and OER, respectively. By using the easy operation and classical bubble extraction method , we find that the Faraday efficiencies of the catalyst for HER and OER are 94.3% and 97.4%, respectively. Moreover, taking advantage of the micropores and mesopores in the yolk/shell structure, it exhibits enhanced stability and promoted diffusion kinetics. This work initiates an effortless approach to the synthesis of the highly efficient yolk/shell carbon-based OWS electrocatalyst .
研究领域:
材料科学
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电化学
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能量转换与存储
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催化
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纳米材料
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可持续能源
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13030-13036
·
IF 3.925
Yu-Hang Zhao,Tao Zhang,Xiao-Feng Wang,Shao-Jie Li,Yu Pan,Yihan Wang,Xue-Zhi Song,Zhenquan Tan
The rational exploration of highly active and low-cost materials for electrocatalytic hydrogen evolution is extremely imperative, but remains challenging as well. Transition metal carbides (TMCs) as highlighted electrocatalysts usually exhibit unsatisfactory activity and stability. In this work, we demonstrate a two-step strategy for electrocatalyst synthesis involving biomass-derived tannic acid (TA) and coordination assembly preparation followed by subsequent high-temperature carbonization. Interestingly, by simply controlling the feed amount of TA, heterostructured nitrogen-doped graphene-coated Mo3Co3C-based tri- and bi-component electrocatalysts (Mo3Co3C/Mo2C/Co@NC and Mo3Co3C/Co@NC) can be obtained with phase regulation and interface engineering. It is observed that the heterostructured materials possess more active sites than that of the TMC-excluding sample (Co@NC). Moreover, the tri-component Mo3Co3C/Mo2C/Co@NC may enhance the intrinsic activity at each active site due to the strong interaction at the Mo3Co3C/Mo2C interface. These advantages allow the Mo3Co3C/Mo2C/Co@NC catalyst to deliver superior electrocatalytic activity and favorable kinetics towards the HER, with a low overpotential of 211 mV and a Tafel slope of 96.0 mV dec−1. Furthermore, it has good long-term stability. This work provides new inspiration for heterostructured TMC-based electrocatalysts with high performance towards promising catalytic applications.
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