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Materials Advances · 2020 ·Vol. 1 ·期 1 ·54-60 · IF 0

FeNiMo trimetallic nanoparticles encapsulated in carbon cages as efficient hydrogen evolution reaction electrocatalysts

Ziqi Zhang,Linchuan Cong,Zhuochen Yu,Lina Qu,Miaomiao Qian,Weimin Huang

Hydrogen is one of the most desirable alternatives to fossil fuels due to its renewability and large energy density. The electrocatalytic hydrogen evolution reaction (HER) is drawing more and more attention since it can produce H2 powered by renewable energy. Therefore, efficient and durable electrocatalysts are an urgent need. On the one hand, the high price and low reserve of noble metals hinder their further applications. On the other hand, various non-noble metal electrocatalysts cannot achieve satisfactory stability and efficiency. Thus, this paper reports a cheap and feasible way to synthesize a carbon cage-encapsulated FeNiMo compound. It exhibits the desired overpotentials of 199 mV at 10 mA cm−2 in an alkaline solution and 246 mV at 10 mA cm−2 in an acidic solution. Besides, it exhibits similar current density loss to commercial Pt/C after 10 000 CV cycles, which suggests satisfactory durability.

研究领域: 材料科学 · 能源化学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Caged biomass carbon with anchoring MoO2/NC Nanospheres: Synergistic enhancement of potassium ion storage and electrochemical performance

Mengmeng Yang,Qingquan Kong,Wei Feng,Weitang Yao,Qingyuan Wang

Due to its relatively high theoretical capacity and low cost, transition metal oxides are considered as candidate anodes for potassium ion batteries (KIB). However, poor recyclability due to inherently large volume changes hinders their application. Therefore, we use Ganoderma spores as the carbon matrix to synthesize MoO 2 /N/C composites through simple complexation reactions. It was found that the synergistic effect of cage-like biomass carbon and molybdenum oxide can promote the transfer and adsorption of potassium ions, thereby improving the storage capacity of potassium ions. On the one hand, the introduction of a small amount of MoO 2 greatly enhances the potassium storage capacity of biomass carbon materials. On the other hand, the porous cage-like carbon structure effectively buffers the volume change during the MoO 2 potassium storage process and provides more diffusion paths for K + . In addition, the stable double-walled cage structure provides the possibility for the composite material to achieve good long-cycle performance. Specifically, MoO 2 /N/C composites provided a high reversible specific capacity of 422 mAh g −1 (after 200 cycles) at 200 mA g −1 , and coulombic efficiency was greater than 98%. The composites still provided a high capacity of 316 mAh g −1 after 500 cycles at 500 mA g −1 . At the same time, after 1500 cycles at 2000 mA g −1 , the capacity was maintained at 248 mAh g −1 . Verify the possibility of its practical application by assembling a full battery, meanwhile, through first-principles calculations, the reasons for the excellent potassium storage performance of MoO 2 /N/C electrodes are discussed.

CAS / MDL: 62-31-7
研究领域: 材料科学 · 电化学 · 能源存储
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Highly dispersed Co/Fe bimetal in carbonaceous cages as heterogeneous Fenton nanocatalysts for enhanced sulfamethoxazole degradation

Dong-Hua Xie,Pu-Can Guo,Keng-Qiang Zhong,Guo-Ping Sheng

A self-assembly strategy was presented for the synthesis of highly dispersed Co/Fe bimetallic carbon cages (CoFe50@C) through thermal morphology-controlled transformation of Fe doping dual metal-organic frameworks (MOFs). Taking advantage of the well dispersibility, synergetic effects between Fe and Co species, and enhanced graphitization degree of carbon, CoFe50@C exhibited a high removal efficiency of 98% in 180 min for sulfamethoxazole (SMX). The synergistic effect between Co and Fe species played an important role in promoting the reduction of Co(III) to Co(II) and the adsorption of H 2 O 2 molecules, thus enhancing the generation of hydroxyl radicals (HO•), which had been demonstrated by density functional theory (DFT) calculations. Meanwhile, the graphitized carbon cages could prevent the loss of bimetallic active component and promote the electron transfer during catalytic reaction . This work provides a new type of highly dispersed Co/Fe bimetal carbon cages as heterogeneous Fenton nanocatalyst for the degradation of organic contaminants.

研究领域: 环境科学 · 材料科学 · 催化化学
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NANOTECHNOLOGY · 2021 ·Vol. 33 ·期 6 ·065409 · IF 3.874

ZIF-67-derived N-doped double layer carbon cage as efficient catalyst for oxygen reduction reaction

Wenwen Zhang,Ximeng Zhao,Weixing Niu,Hang Yu,Tongtao Wan,Guihua Liu,Dongsheng Zhang,Yanji Wang

The slow kinetic of oxygen reduction reaction (ORR) hampers the practical application of energy conversion devices, such as fuel cells, metal-air batteries. Here, an efficient ORR electrocatalyst consists of Co, Ni co-decorated nitrogen-doped double shell hollow carbon cage (Ni–Co@NHC) was fabricated by pyrolyzing Ni-doped polydopamine wrapped ZIF-67. During the preparation, polydopamine served as a protective layer can effectively prevent the aggregation of Co and Ni nanoparticles during the pyrolysis process, and at the same time forming a carbon layer to grow a double layer carbon cage. This unique hollow structure endows the catalyst with a high specific surface area as well as more exposed active sites. Also benefited from the synergistic effect between Ni and Co nanoparticles, the Ni–Co@NHC catalyst leads to an outstanding ORR performance of half-wave potential (E1/2, 0.862 V), outperforms that of commercial Pt/C catalyst. Additionally, when Ni–Co@NHC was used in the cathode for the zinc-air battery, the cell exhibits high power density (108 mW cm−2) and high specific capacity (806 mAh g−1) at 20 mA cm−2 outperforming Pt/C. This work offers a promising design strategy for the development of high-performance ORR electrocatalysts.

研究领域: 材料科学 · 电化学 · 能源转换技术
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ChemCatChem · 2023 ·Vol. 15 ·期 5 ·e202201615 · IF 4.5

Hollow Carbon Cages Derived from Polyoxometalate-Encapsuled Metal-Organic Frameworks for Energy-Saving Hydrogen Production

Huijie Cao,Tianran Wei,Qian Liu,Shusheng Zhang,Yongji Qin,Hao Wang,Jun Luo,Xijun Liu

Graphical Nano-structured materials for glycerol/glucose oxidation reaction : Herein, hollow-structured PW-NiCo-NC was synthesized from a POMOF precursor as a highly efficient and stable electrocatalyst for HER and glycerol/glucose oxidation reaction. Furthermore, it exhibits energy-efficient catalytic hydrogen production activity in an OWS cell assisted by glycerol/glucose oxidation reaction. The electrocatalytic conversion of water-to-hydrogen powered by renewable energy is one of the promising strategies to unravel the energy and environment crises. However, a such process usually costs large energy consumption owing to the low efficiency of anodic oxygen evolution reaction (OER), which is another vital half reaction of the overall water splitting (OWS) system. Herein, we designed and fabricated hollow nitrogen-doped carbon nanocages loaded with Ni 3 N and Co nanoparticles derived from polyoxometalate-encapsuled metal-organic frameworks. The catalyst exhibited appealing dual functions for both OER and hydrogen evolution reaction (HER), outperforming the Ni-free and solid samples. Notably, the designed catalyst also showed much enhanced electrochemical performance for glycerol/glucose oxidation reaction when compared with OER. The home-made two-electrode electrolyzer, coupled HER with polyalcohol or glucose oxidation reaction, only needs cell voltages of 1.125 and 1.557 V to reach 10 mA cm −2 , respectively, which are much smaller than that in 1 M KOH (2.087 V), demonstrating a large amount of energy saving for hydrogen production.

研究领域: 材料科学 · 能源化学
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ACS Nano · 2022 · IF 18.027

Pseudocapacitive Vanadium Nitride Quantum Dots Modified One-Dimensional Carbon Cages Enable Highly Kinetics-Compatible Sodium Ion Capacitors

Jun Yuan,Min Qiu,Xiang Hu,Yangjie Liu,Guobao Zhong,Hongbing Zhan,Zhenhai Wen

The kinetics incompatibility between battery-type anode and capacitive-type cathode for sodium ion hybrid capacitors (SIHCs) seriously hinders their overall performance output. Herein, we construct a SIHCs device by coupling with quantum grade vanadium nitride (VN) nanodots anchored in one-dimensional N/F co-doped carbon nanofiber cages hybrids (VNQDs@PCNFs-N/F) as the freestanding anode and the corresponding activated N/F co-doped carbon nanofiber cages (APCNFs-N/F) as cathode. The strong coupling of VN quantum dots with N/F co-doped 1D conductive carbon cages effectively facilitates the ion/electron transport and intercalation–conversion–deintercalation reactions, ensuring fast sodium storage to surmount aforesaid kinetics incompatibility. Additionally, density functional theory calculations cogently manifest that the abundant active sites in the VNQDs@PCNFs-N/F configuration boost the Na+ adsorption/reaction activity well which will promote both “intrinsic” and “extrinsic” pseudocapacitance and further improve anode kinetics. Consequently, the assembled SIHCs device can achieve high energy densities of 157.1 and 95.0 Wh kg–1 at power densities of 198.8 and 9100.5 W kg–1, respectively, with an ultralong cycling life over 8000 cycles. This work further verified the feasibility of kinetics-compatible electrode design strategy toward metal ion hybrid capacitors.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 电化学能源存储
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

CoNi nano-alloys modified yolk-shell structure carbon cage via Saccharomycetes as carbon template for efficient oxygen evolution reaction

Guangyao Hou,Xin Jia,Hongjun Kang,Xianshu Qiao,Yang Liu,Yang Li,Xiaohong Wu,Wei Qin

ABSTRACT Developing efficient and stable OER catalysts is conducive to improving hydrogen production efficiency and achieving “carbon neutrality” goal. Herein, a CoNi nano-alloys modified yolk-shell carbon cage (CoNi/NC-YS) catalyst was synthesized through a green synthesis method, which shows an outstanding OER activity with a low overpotential of 292 mV at 10 mA·cm −2 , and a robust OER catalytic stability. The experimental and density functional theory (DFT) results demonstrate that the hydrophilic yolk-shell CoNi/NC-YS catalyst with large specific area contributes to exposing more active sites, and increases the reaction contact area between catalysts and electrolyte. Meanwhile, CoNi nano-alloys can regulate the electronic configuration of CoNi/NC-YS catalyst and optimize Gibbs free energies for water adsorption, accelerating OER process in alkaline media and showing an outstanding OER performance. This work can provide a low-cost and green strategy to construct nano-alloys modified yolk-shell OER catalysts for renewable energy systems.

研究领域: 材料科学 · 能源科学 · 催化化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Methanol-induced assembly and pyrolysis preparation of three-dimensional N-doped interconnected open carbon cages supported FeNb2O6 nanoparticles for boosting oxygen reduction reaction and Zn-air battery

Lu Zhang,Ling-Ling Liu,Jiu-Ju Feng,Ai-Jun Wang

Three-dimensional (3D) hollow carbon is one of advanced nanomaterials widely applied in oxygen reduction reaction (ORR). Herein, iron niobate (FeNb 2 O 6 ) nanoparticles supported on metal-organic frameworks (MOFs)-derived 3D N -doped interconnected open carbon cages (FeNb 2 O 6 /NICC) were prepared by methanol induced assembly and pyrolysis strategy. During the fabrication process, the evaporation of methanol promoted the assembly and cross linkage of ZIF-8, rather than individual particles. The assembled ZIF-8 particles worked as in-situ sacrificial templates, in turn forming hierarchically interconnected open carbon cages after high-temperature pyrolysis. The as-made FeNb 2 O 6 /NICC showed a positive onset potential of 1.09 V and a half-wave potential of 0.88 V for the ORR , outperforming commercial Pt/C under the identical conditions. Later on, the as-built Zn-air battery with the FeNb 2 O 6 /NICC presented a greater power density of 100.6 mW cm −2 and durable long-cycle stability by operating for 200 h. For preparing 3D hollow carbon materials, this synthesis does not require a tedious removal process of template, which is more convenient than traditional method with silica and polystyrene spheres as templates. This work affords an exceptional example of developing 3D N -doped interconnected hollow carbon composites for energy conversion and storage devices.

研究领域: 材料科学 · 电化学 · 能源转换与存储
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CARBON · 2020 · IF 8.821

Synthesis of porous nitrogen doped carbon cage from carbide for catalytic oxidation

Jun Wang,Zhe Yang,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng,Shaobin Wang

Nitrogen doped porous carbon cage materials are successfully synthesized using a chemical vapor deposition (CVD) method. Several carbides are selected as templates and in situ removed by CCl 4 . NaNO 3 is then used to create porous structure , and a very large surface area (SSA) (1224 m 2 g -1 ) could be obtained. The obtained materials can activate peroxymonsulfate (PMS) for degradation of various organic pollutants effectively. By NaNO 3 , the nitrogen doping styles could be regulated and the percentage of graphitic N and C O group could be increased, which will alter the PMS-based oxidation from a radical pathway to a non-radical dominated process. This study provides a novel way for synthesis of carbocatalysts, which should have great potential in environmental remediation.

CAS / MDL: 108-95-2 497-19-8
研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

3-D nitrogen-doped carbon cage encapsulated ultrasmall MoC nanoparticles for promoting simultaneous ZnIn2S4 photocatalytic hydrogen generation and organic wastewater degradation

Sijia Liu,Xifei Zhou,Junxian Qin,Chaohai Wei,Yun Hu

Simultaneous redox reactions on photocatalysts make it possible to use wastewater for hydrogen production . The controlled synthesis of ultrasmall metal carbides effectively enhances the photocatalytic efficiency under this system. Here, we report a new type of cocatalyst in which a three-dimensional (3-D) nitrogen-doped carbon cage (NGC) of metal–organic framework derivatives encapsulates ultrasmall MoC nanoparticles (MoC@NGC), promoting simultaneous degradation of organic pollutants and hydrogen production by ZnIn 2 S 4 (ZIS). Characterization analyses showed that MoC accelerated the separation of the photogenerated carrier and effectively reduced the overpotential of hydrogen evolution , while NGC promoted the good dispersion of MoC particles and provided sufficient sites. The MoC@NGC/ZIS composite exhibited a high hydrogen (H 2 ) evolution rate of 1012 µmol g –1 h −1 , which exceed that of ZIS loaded with platinum. In the coupled system, where the electron donor was replaced with rhodamine B (RhB), the mechanism analysis showed that RhB and the as-generated intermediates consumed holes and facilitated hydrogen evolution. In addition, we designed a combined photocatalytic anoxic and oxic sequence process to achieve the recovery of hydrogen energy during the treatment of dye wastewater. This study provides a new way for cooperation between energy development and environmental protection.

研究领域: 材料科学 · 环境科学 · 能源 · 化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Degradation of Cephalosporin C using MOF-derived Fe-Co bimetal in carbon cages as electro-Fenton catalyst at natural pH

Yaoyu Zhou,Jianlong Wang

Developing high performance electrocatalysts for effective antibiotics elimination for heterogeneous electro-Fenton (Hetero-EF) process is still a challenge. This work synthesized iron/cobalt bimetallic N doped graphitic carbon cages (Fe x Co@NC) from ZIF-8@ZIF-67-Fe dual MOF composite for Cephalosporin C (CEP-C) degradation in the Hetero-EF system at a wide pH range. Results indicated that CEP-C degradation rate and total organic carbon (TOC) removal efficiency by Fe 40 Co@NC catalyst were as high as 82.45% (60 min) and 61.35% (240 min) at natural pH, respectively. The unique structure with FeCo bimetal encapsulated inside the N doped graphitic carbon cages enabled Fe 40 Co@NC to show excellent catalytic reactivity for H 2 O 2 activation. The generated M (•OH) and •OH all contributed to CEP-C degradation. The synergistic effects of Co 0 /Co 2+ /Co 3+ and Fe 0 /Fe 2+ /Fe 3+ cycles made Fe 40 Co@NC catalyst to continuously activate H 2 O 2 . Moreover, Fe 40 Co@NC catalyst showed good stability in consecutive cycles, and could still remain excellent reactivity when applied for CEP-C degradation from the real CEP-C fermentation residue supernatant. Furthermore, a possible CEP-C degradation pathway was proposed based on the identified intermediates.

CAS / MDL: 75-05-8 64-18-6
研究领域: 环境科学 · 化学工程 · 材料科学 · 催化
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