ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Liyuan Guo,Nengneng Xu,Tuo Lu,Qin Cao,Momo Safari,Jong Min Kim,Yongxia Wang,Jinli Qiao
The rational design of bifunctional electrocatalysts with abundant active sites and efficient charge/mass transport is crucial for Zn-air batteries. Here, we report a scalable electrospinning strategy to fabricate Co/N-doped carbon nanofibers (CNFs) with a beaded architecture derived from ZIF-67@PAN precursors. By precisely tuning the ZIF-67 loading, the intercluster spacing along the fibers can be controlled, yielding well-dispersed Co nanoparticles and Co-N x moieties after pyrolysis. Critically, vertically stacked nanofibrous membranes enable scalable manufacturing. The optimized Co/Co-N x -C@CNF-1.5 exhibits superior bifunctional activity (Δ E = 0.815 V), benefiting from balanced active-site density, rapid electron transport, and hierarchical porosity. Density functional theory calculations further reveal the microscopic origin that an appropriate spacing enables moderate electronic coupling between adjacent Co-based active sites, thereby optimizing the adsorption energetics of oxygen intermediates and facilitating ORR/OER kinetics. As an air cathode, the liquid Zn-air battery delivers a peak power density of 406.5 mW cm −2 , an energy density of 976 Wh kg −1 , and a long cycling stability of ∼2143 h. The quasi-solid-state device also shows high power output, stable operation, and excellent flexibility. This work demonstrates a general electrospinning-pyrolysis approach to engineer MOF-derived self-supporting electrodes, bridging high-performance electrocatalysis with practical energy storage applications.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yang Li,Yihao Jing,Yiguo Zhao,Wentao Li,Jing Li,Yuqing Song,Yue Yang,Tingting Feng,Gen Peng,Zhenpeng Huang,Ting Yang,Qi Zhou
In this study, novel Co-embedded hollow N -doped carbon polyhedrons, derived from ZIF-8@ZIF-67 core–shell structure, were synthesized and used for activating peroxymonosulfate (PMS) towards efficient bisphenol A (BPA) degradation. The contents of different N species, especially Co-N x and graphitic N sites, were tuned by different calcination temperatures (800, 900, and 1000 °C). Characterization results demonstrated that hollow polyhedron with high graphitization degree and abundant porosity anchored numerous Co nanoparticles, which could enhance the catalytic performance. Compared to other as-prepared catalysts, Co/HNCP-900 (pyrolyzed at 900 °C) showed a more outstanding performance of PMS activation towards BPA degradation, and 95.1 % of BPA (20 mg/L) could be removed within 3 min. Abundant Co-N x sites were a critical factor to induce the reaction process. Based on trapping, radical scavenger, and electrochemical analysis experiments, a nonradical process (singlet oxygen and direct electron transfer) was proposed to play the dominant role in BPA degradation. Benefiting from the nonradical process, BPA degradation efficiency almost remained stable either in a wide pH range (2.5–8.0) or in the presence of coexisting ions and natural organic matter. The findings of this study will elucidate a new opportunity for improving environmental remediation.
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高影响因子
Materials Today Sustainability
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2022
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IF 7.244
X. Zhang,J. Xu,L. Wu
Fuel cells and metal-air batteries attracted extensive research attention owing to high power density, renewability, and environmental friendliness. Hence, developing heteroatom-doped pyridinic N abundant porous carbon materials with large surface area have an extensive effect on oxygen reduction reaction (ORR) for fuel cell and metal-air battery. Herein, high content of pyridinic N porous carbon-supported Co/Co-N x nanoparticles were synthesized as ORR catalysts by carbonizing complexes of hexamethylenetetramine (HMT) and Co(NO 3 ) 2 ·6H 2 O with silica template. The HMT-Co@SiO 2 -900 with high content of pyridinic N, large specific surface area, and porous structure exhibits a more positive half-wave potential (0.85 V) than 20% Pt/C and the outstanding performance oxygen evolution reaction behavior. The low Tafel slope of HMT-Co@SiO 2 -900 revealed the faster reaction kinetics during ORR. The HMT-Co@SiO 2 -900 zinc-air battery showed a high excellent cyclic stability in continuous charge/discharge cycles for 420 times at 10 mA/cm 2 . This research provides an efficient strategy for the preparation of pyridinic N porous electrocatalyst by the reduction of diffusion restriction and exposure of active sites.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meiling Liu,Liping Wang,Qilong Fan,Ningning Xiao,Zhiwen Chen,Yingying Dong,Chuanliang Zhao,Yongxia Sun,Xing Xu,Wendong Wang
Nitrogen (N)-doping has been reported effective to reinforce catalysis in advanced oxidation processes (AOPs) due to the formation of N-related active sites. Although several documents have reported that transition metal-nitrogen (metal-N x ) sites could work as reactive centers, the catalytic mechanism was hardly elucidated. In this study, N-doped cobalt oxide (N-CoO x ) was initiatively prepared via calcination in ammonia atmosphere to construct cobalt-nitrogen (Co-N x ) sites. The emergence of Co-N x sites effectively improved peroxymonosulfate (PMS) activation efficiency (above 5.8 times), leading to higher pollutant decomposition rate (95.8 % at 30 min) and kinetics constant (above 4.1 times). N introduction changed main facets of material and elevated adsorption energy (E ads ) (from −1.81 eV to −3.71 eV) between catalyst and PMS. Co atoms at Co-N x sites could donate larger quantity of electrons (from 1.088 e to 1.583 e) to PMS, therefore, contributed to stretching and breaking O–O bonds of PMS molecules to form reactive species. As a result, both radical and electron transfer pathway (ETP) were enhanced in the oxidation processes. Ultimately, the catalytic membrane coated with N-CoO x maintained 100 % treatment towards continuous antibiotic wastewater at environmentally relevant concentration (μg/L), realizing purification as well as separation of catalyst. This work systematically elaborates the superiority of Co-N x sites and unravels the underlying mechanism to inspire further study to metal-N x tailored catalysis.
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高影响因子
ACS Omega
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2023
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IF 4.1
Peipei Liu,Meiling Fan,Yapeng Cheng,Hongfei Pan,Jin Liu,Haining Zhang
Porous carbon materials with nitrogen-coordinated transition metal active sites have been widely regarded as appealing alternatives to replace noble metal catalysts in oxygen-based electrochemical reaction activities. However, improving the electrocatalytic activity of transition-metal-based catalysts remains a challenge for widespread application in renewable devices. Herein, we use a simple one-step pyrolysis method to construct a Co nanoparticles/Co–Nx-decorated carbon framework catalyst with a near-total external surface structure and uniform dispersion nanoparticles, which displays promising catalytic activity and superior stability for oxygen reduction reactions in both alkaline and neutral electrolytes, as evidenced by the positive shift of half-wave potential by 44 and 11 mV compared to 20% Pt/C. Excellent electrochemical performance originates from highly accessible Co nanoparticles/Co–Nx active sites at the external surface structure (this is, exposing active sites). The thus-assembled liquid zinc–air battery using the synthesized electrocatalyst as the cathode material delivers a maximum power density of 178 mW cm–2 with an open circuit potential of 1.48 V and long-term discharge stability over 150 h.
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PubMed
高影响因子
Journal of Materials Chemistry A
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2024
·Vol. 12
·期 27
·16863-16876
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IF 10.7
Katam Srinivas,Hesheng Yu,Zhuo Chen,Anran Chen,Ming-qiang Zhu,Yuanfu Chen,Chengtao Yang
The urgent demand for stable and highly efficient bifunctional electrocatalysts for the oxygen reduction/evolution reactions (ORR/OER) is pivotal in advancing energy conversion and storage technologies. Herein, we introduce a metal–organic framework (MOF)-derived bifunctional electrocatalyst Fe3Co-NC@900, featuring synergistically coupled dual single-atom sites (Fe/Co–Nx) and core–shell Co3Fe7@C nanoparticles. Leveraging the synergistic interactions of Fe–Nx sites with associated Co–Nx sites and core–shell nanoparticles within the MOF-derived nitrogen-doped mesoporous sheets and nanotubes, Fe3Co-NC@900 demonstrates outstanding ORR and OER performance, outpacing the Fe-NC@900 catalyst fabricated without Co incorporation. Specifically, it demonstrates superior ORR performance with a higher half-wave potential (E1/2) of 0.88 V and a small Tafel slope of 62.1 mV dec−1, surpassing the Pt/C benchmark (E1/2 of 0.82 V) and Fe-NC@900 (E1/2 of 0.788 V). Additionally, it demonstrates noteworthy OER performance, requiring a 1.572 V overpotential at 10 mA cm−2 current density, resulting in a significant bifunctional activity with a potential gap (ΔE) of 0.692 V, surpassing the Pt/C + Ir/C combination (ΔE = 0.748 V). Moreover, serving as a bifunctional air electrode, Fe3Co-NC@900 exhibits excellent performance in lab-made Zn–air batteries, with outstanding open circuit voltage, specific capacity, and cycling stability (>650 cycles), outpacing the Pt/C + Ir/C-based battery.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Jiahui Xu,Jia-qi Bai,Wenjie Si,Yunhai Zhang,Jiazhao Tan,Mengdie Cai,Qin Cheng,Song Sun
Non-noble metals have attracted worldwide attention for the catalytic hydrogenation of halonitrobenzene due to their high activity, low price, and abundance on Earth. However, the construction of effective and stable non-noble-metal catalysts for the selective hydrogenation of halonitrobenzene to haloaniline by a simple method remains challenging. Herein, we report a facile one-pot method for the synthesis of N,S-co-doped mesoporous carbon-supported non-noble-metal catalysts through carbonization of a mixture of metallic precursors and 2-aminothiazole in molten ZnCl2. The prepared Co-NSPC catalyst showed excellent activity and selectivity with a turnover frequency of 84.4 h–1 in the hydrogenation of p-chloronitrobenzene to p-chloroaniline. Furthermore, Co–Nx was found to be the main active site for this reaction on the basis of characterization and experimental data, and the introduction of S promoted the formation of Co–Nx sites. Moreover, the Co-NSPC-800 catalyst can be reused at least four times and applied to the hydrogenation of 10 kinds of halogenated nitrobenzenes with excellent selectivity.
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高影响因子
Materials Today Physics
·
2019
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IF 0
X. Wu,S. Chen,Y. Feng,Q. Yuan,J. Gao,Y. Chen,Y. Huang,Y.-B. He,W. Gan
The development of bifunctional cathode catalysts with advantages such as high activity, low cost, and high durability is highly desirable and challenging for zinc-air batteries (ZABs) in energy applications . In this work, a novel type of bifunctional catalyst (CoP x /Co-N x -C@CNT) simultaneously effective for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) was prepared via a simplified all-in-one phosphorization-carbonization synthesis, which is distinctively different from the previously reported carbonization and postphosphorization route. With the integration of efficient catalytic factors such as Co-N x -C–coordinated moieties, cobalt phosphide, graphitic carbon shells, as well as a supportive and conductive matrix, the as-prepared CoP x /Co-N x -C@CNT exhibits high catalytic activity for ORR and OER in 0.1 M KOH, with an output positive onset potential of 0.92 V vs reversible hydrogen electrode (RHE) for ORR and a low potential of 1.69 V vs RHE at 10 mA cm −2 for OER. Remarkably, the assembled liquid and all-solid-state ZAB based on the as-prepared CoP x /Co-N x -C@CNT showed superior cycling performance than the results of its Pt/C-based counterparts and some recently reported cobalt phosphide–based ZABs. The good flexibility and reversibility of the all-solid-state ZAB also verified its feasibility in applications such as wearable electronics .
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