NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 13
·5949-5957
·
IF 3.591
Xuexia Liu,Shuaihui Li,Limin Liu,Zhijun Wang
The development of active and stable carbon nanomaterials as electrocatalysts for the oxygen reduction reaction (ORR) remains a significant challenge. Herein, we report a one-step pyrolysis process to design hierarchical micro/mesoporous N-doped carbon (m-NC) materials using low-cost folic acid precursors. The optimal m-NC material carbonized at 750 °C (m-NC-750) displays a splendid ORR electrocatalytic activity and perfect stability in an alkaline medium (0.1 mol L−1 KOH). Notably, the current density of m-NC-750 can reach 4.35 mA cm−2 at 0.85 V, which surpasses that of commercial Pt/C (20 wt%). The higher electrocatalytic activity and activation of oxygen is due to the porous structures facilitating ion diffusion and the graphitic N dopant providing more active sites. In addition, the graphite N dopant of the m-NC material possesses the lowest energy barrier of reactions based on density functional theory (DFT) calculations, which effectively boosts the ORR of the as-prepared materials. This simple and economical method provides a facile way of designing high-performance carbon electrocatalysts for the ORR.
研究领域:
材料科学
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电化学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Pengcheng Wang,Qingqing Jiang,XingYu Li,Xuedong Wang,Juncheng Hu
Generally, researchers focus on the regulation of metal sites rather than surrounding nonmetals in photothermal CO 2 hydrogenation reaction. Herein, concerning the role of non-metallic N species, a series of Co/NC-T catalysts have been fabricated via high-temperature pyrolysis of Zeolitic Imidazolate Frameworks-67. The CO 2 conversion rate shows a consistent tendency with the ratio of graphitized-N species while the product selectivity is closely related to the coordination state of Co-N x species. Co/NC-800 catalyst achieves high CO 2 conversion rate of 758 mmol g cat -1 h -1 with CH 4 selectivity of 99.6 %. After adding extra graphitized-N species, the CO 2 conversion rate could further enhance to 80.2 % for N-Co/NC-2. The role of N species in photothermal CO 2 hydrogenation reaction has been investigated in details, providing new insights for the design of metal organic frameworks derived metal/N-doped carbon catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 8
·E240
·
IF 3.12
Zhengzheng Xie,Xiaohong Shang,Kaibing Xu,Jianmao Yang,Bin Hu,Pengfei Nie,Wenwen Jiang,Jianyun Liu
The ginkgo leaf-derived graphitic-N-doped porous carbon was fabricated by one-step carbonization in the presence of KOH agent. The morphology, surface functional groups, element state and porous structure of the obtained carbon were investigated systematically. Compared with the carbon samples by ginkgo-leaf carbonization and KOH post-activation (two-step), the one-step activated porous carbon exhibits high graphitic-N content and good electric conductivity. The conductive-agent-free carbon sheet was made successfully and the resultant carbon electrode possesses good conductivity and excellent electrochemical properties, with the specific capacitance of 176.1 F g−1. When being applied for capacitive deionization, the desalination amount of the electrode arrived at 16.5 mg g−1. Meanwhile, the salt adsorption rate is very rapid, with the average salt adsorption rate reaching 1.5 mg g−1 min−1. This work provides an easy and environmentally benign route for the synthesis of the conductive carbon from natural raw materials for highly efficient capacitive deionization.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Junjie Zhang,Pei Chen,Wenran Gao,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Graphitic N-rich graphene (GNG) was prepared through a melamine-cyanurate (MC) supramolecule induced method by pyrolyzing the precursor of graphene oxide@melamine cyanurate composite (GO@MC). The fabricated sample at 800 °C (GNG8) possessed the high graphitic N content of 4.18%, which exhibited excellent capability to peroxymonosulfate (PMS) activation for degradation of organic pollutants. Results of electron paramagnetic resonance (EPR) spectra coupled with quenching experiments and density functional theory (DFT) calculations revealed that the graphitic N in graphene was the intrinsic active site for the cleavage of O-O bond in PMS to produce singlet-oxygen ( 1 O 2 ), responsible for organics degradation. Furthermore, the GNG/PMS system could work in a wide temperature range (5–45 °C), and the common matrix species of Cl − , NO 3 − , HCO 3 − and HA had negligible effect on the degradation performance. This study provided a facile strategy for the preparation of highly graphitic N doped graphene catalysts to powerfully degrade organic pollutants, and deep understand of the catalytic mechanism of GNG for PMS activation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
HongWei Li,Peng Guo,BoYu Huang,Dong Ji,GuiXian Li,XinHong Zhao
Rational modulation of metal-support interaction (MSI) is pivotal yet challenging for developing high-performance electrocatalysts. Herein, we demonstrate a promoter engineering strategy to precisely tune the N configuration in ZIF-8-derived carbon supports for boosting Pd-catalyzed methanol oxidation reaction (MOR). Structurally diverse organic promoters (urea, dicyandiamide, sucrose, xylitol) impregnated in ZIF-8 pores regulate pyrolysis behavior, yielding N-doped carbons with optimized porosity, graphitization, and N-configuration. Among them, urea-modified support (NC–U) demonstrates the highest surface area (925 m 2 g −1 ) and graphitic-N content (40.4 %), facilitating uniform dispersion of ultrasmall Pd nanoparticles (2.71 nm) and electron transfer to enrich metallic Pd 0 (75.2 %). The resulting Pd/NC-U delivers exceptional MOR activity (5570.7 mA·mg −1 Pd ) and stability (87.4 % retention after 500 cycles), outperforming unmodified Pd/NC by 1.32-fold. Besides, operando SERS reveals a CO-free pathway on all catalysts, with Pd/NC-U initiating HCO 3 − /CO 3 2− formation at the lowest potential (0.4 V vs. RHE). This work establishes promoter-mediated N-configuration control as a robust route to tailor MSI for efficient alcohol electrooxidation.
研究领域:
材料科学
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电催化
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纳米技术
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Peng Guo,HongWei Li,BoYu Huang,Dong Ji,GuiXian Li,XinHong Zhao
Despite nitrogen-doped carbons (NC) enhancing metal–support interactions (MSI) in electrocatalysts, how specific N-configurations (pyridinic, pyrrolic, and graphitic) synergistically govern methanol oxidation reaction (MOR) pathways over Pd surfaces remains unknown. Herein, we hypothesize that precise thermal programming of ZIF-8 pyrolysis can tailor synergistic pyridinic-pyrrolic-graphitic N-triads to simultaneously enhance activity, CO tolerance, and stability. Guided by DFT predictions, Pd/NC-T catalysts (T = 700–1100) were synthesized, where in situ pyrolysis controls N-configurations (validated by XPS) and wet impregnation immobilizes ultrafine Pd nanoparticles (3.6 ± 0.8 nm). Furthermore, experimental and theoretical analyses reveal that pyrrolic-N facilitates the adsorption of methanol on Pd, while pyridinic-N suppresses the CHO* → CO* reaction pathway, thus enhancing the catalyst’s tolerance to poisoning, and graphitic-N prevents support dissolution and collapse during the electrocatalytic reaction, thus mitigating active site loss. Notably, Pd/NC-900 achieves 4195.0 mA·mg–1Pd in the alkaline electrolyte, maintaining 80.5% of its initial current density after 500 cycles at 200 mV/s, highlighting its exceptional catalytic activity and long-term stability. This work offers profound insights into the intricate MSI, serving as a crucial framework for guiding the future design and advancement of MOR electrocatalysts.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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表面化学
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能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 82
·51831-51837
·
IF 3.108
Yunrui Zhang,Haihong Niu,Xiangjie Zhang,Junxiu Pan,Yang Dong,Haijun Wang,Yongjun Gao
A kind of magnetic N-containing carbon material was synthesized by a simple method using sustainable N-acetyl-D-glucosamine (NAG) and iron nitrate as the raw materials. In C–H oxidation reactions such as the epoxidation of stilbene and styrene, and the oxidation of ethylbenzene, the carbon catalyst exhibited excellent catalytic activity and selectivity for the target products. The superparamagnetic properties at room temperature facilitated catalyst recycling and reusability when it was used as a catalyst. The relationship between the catalytic results and the N 1s XPS analysis indicated that the graphitic N species located in the carbon skeleton was the key accelerating factor which promoted the catalytic C–H oxidation. Density functional theory (DFT) calculations further indicated that the iron species were not an essential factor but they acted as promoters for the catalytic performance of the catalyst. This study will expand the application of biomass-based heteroatom-containing compounds.
研究领域:
材料科学
·
催化
·
可持续化学
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无机化学
·
理论化学
✓ 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）