CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Liang Zhang,Jialiang Rui,Yiqian Li,Zhizhi Yang,Shiro Kubuki,Junhu Wang,Bofan Zhang
Precise manipulation of the catalytic spin configuration and delineation of the relationship between spin related properties and oxidation pathways remain significant challenges in Fenton-like processes. Herein, encapsulated cobalt nanoparticles and cobalt-nitrogen-doped carbon moieties, endowed with confinement effects and variations in shell curvature were constructed via straightforward pyrolysis strategies, inducing alterations in magnetic anisotropy, electronic energy levels and spin polarization. The enhanced spin polarization at cobalt sites leads to a reduction in crystal field splitting energy and an increase in electronic spin density. This phenomenon facilitated electron transfer from cobalt orbitals to p z orbitals of oxygen species within peroxymonosulfate molecules, thereby promoting the formation of high-valent cobalt species. The encapsulation effectively stabilized cobalt nanoparticles, mitigating their dissolution or deactivation during reactions, which in turn enhances stability and durability in continuous flow processes. The high-valent cobalt species within the shell exhibit increased exposure and generate localized high concentrations, thereby intensifying interactions with migrating pollutants and enabling efficient and selective oxidation of emerging compounds with elevated redox potentials. This work underscores the profound impact of confined encapsulation curvature and spin polarization characteristics of metal sites on catalytic oxidation pathways and performance, opening novel avenues for spin engineering in practical environmental catalysis.
研究领域:
环境催化
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材料化学
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物理化学
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纳米催化
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污染控制化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
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2024
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IF 5.3
Zhuang Wang,Mian Li,Wenping Cao,Xiangjie Bo
Enhancing catalytic efficiency, achieving controlled synthesis, and lowering production costs are crucial for promoting the use of cobalt oxide (CoOx)/cobalt nitride (CoNx) composites in full water splitting and electrochemical sensing. In this study, a three-dimensional (3D) hierarchically porous material composed of numerous two-dimensional (2D) porous CoOx/CoNx nanosheets (denoted as CoOx/CoNx NSs) was synthesized by using cobalt oxalates (COs) recycled from spent lithium-ion batteries. In a 1.0 M KOH solution, the 2D porous CoOx/CoNx NSs exhibited higher oxygen evolution reaction (OER) electrocatalytic activity than commercial ruthenium oxide (RuO2). Meanwhile, the CoOx/CoNx NSs exhibited a slightly lower hydrogen evolution reaction (HER) electrocatalytic activity than 20 wt % platinum/carbon (Pt/C). Moreover, the CoOx/CoNx NS-based full water-splitting electrolyzer achieved a current density of 10 mA cm–2 at 1.562 V, which was 49 mV more positive than the 1.489 V of the Pt/C||RuO2 benchmark. Furthermore, the 2D porous CoOx/CoNx NSs featured significantly higher HER, OER, and full water-splitting catalytic stability than Pt/C/RuO2. Moreover, the CoOx/CoNx NS-based nonenzymatic electrochemical sensor exhibited advanced glucose detection performance. Particularly, the sensor had a wide linear range of 1.0–10.5 mM), a low detection limit of 5.0 μM), and a fast response time of 0.6 s. The 2D porous CoOx/CoNx NSs exhibited excellent catalytic activity owing to their 3D hierarchically porous architectures, large surface area, good conductivity, uniformly dispersed active sites, and synergistic effects of CoNx and CoO. This study presents an advanced model for recycling Co metal from spent devices and designing advanced Co-based electrocatalysts for water splitting and electrochemical sensing.
研究领域:
材料科学
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环境科学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Li Xu,Daijie Deng,Yuhui Tian,Hongping Li,Junchao Qian,Jianchun Wu,Henan Li
The sluggish kinetics of oxygen reduction reaction (ORR) is the bottleneck for practical applications of zinc-air batteries (ZABs). Developing highly efficient ORR electrocatalysts is of the essence for large-scale applications of ZABs. Herein, we design and synthesize the CoN x /Zn, N co-doped porous carbon structure (CoN x /Zn-NC) by self-polymerization of biomass materials and coupling of nitrogen-rich species with metallic ions. The introduced zinc element can regulate electronic structures of electrocatalysts and construct bimetallic active sites (N-Co/N-Zn species), facilitating the adsorption of reaction intermediates and further enhancing electrocatalytic performance. The porous carbon structure obtained by the self-polymerization of locust bean gum not only disperses active sites but also improves the O 2 and electron transfer efficiency of electrocatalysts. The CoN x /Zn-NC exhibited excellent ORR electrocatalytic performance (E 1/2 = 0.85 V) as well as outstanding stability. Impressively, the ZABs assembled with CoN x /Zn-NC demonstrated a high maximum power density, specific capacitance, and excellent charge/discharge cycling stability for 115 h, surpassing Pt/C catalyst.
研究领域:
材料科学
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电化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Sander Dekyvere,Somboon Chaemchuen,Zhonghui Zheng,Jichao Wang,Meng Liu,Francis Verpoort
Rechargeable zinc-air batteries have a substantial theoretical energy density while potentially being manufactured at a minimized cost. Hence, developing low-cost bifunctional electrocatalysts is of crucial importance. Herein, the synthesis of an electrocatalyst containing zinc/cobalt species encapsulated in a nitrogen-doped carbon matrix modulated with a large number of carbon nanotubes (ZnCo@CN) was developed through a facile thermal method under solvent-free conditions. Using bio-based sucrose in the presence of inorganic catalysts (Zn/Co) resulted in a Zn/Co carbon foam-like structure. Subsequently, the high-temperature treatment with the addition of 2-methylimidazole resulted in a unique material (ZnCo@CN). The incorporation of highly active species dispersed in hierarchical porous carbon presented an excellent bifunctional electrocatalyst for ORR (half-wave potential of 0.85 V) and OER (overpotential of 327 mV). The assembled zinc-air battery with ZnCo@CN as a bifunctional air cathode exhibited an excellent power density of 206 mW cm -2 and an astonishing energy density of 983 Wh Kg -1 .
研究领域:
材料科学
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能源化学
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电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）