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Title
Hydrogen generation from hydrous hydrazine over Rh/g-C3N4 nanocatalysts
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作者
邱小魁孙佳丽花俊峰郑君宁万超许立信
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Author
QIU Xiao-kui;SUN Jia-li;HUA Jun-feng;ZHENG Jun-ning;WAN Chao;XU Li-xin
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单位
安徽硅宝有机硅新材料有限公司浙江省环境科技有限公司安徽工业大学 化学与化工学院浙江大学 化学工程与生物工程学院南开大学 先进能源材料化学教育部重点实验室
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Organization
GBXF Silicones Co., Ltd
Zhejiang Environment Technology Co., Ltd
School of Chemistry and Chemical Engineering, Anhui University of Technology
College of Chemical Engineering and Biological Engineering, Zhejiang University
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University
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摘要
本研究将三聚氰胺在静态空气中焙烧合成的g-C3N4作为载体,通过简单的浸渍还原法将Rh纳米粒子负载在g-C3N4载体上制备出Rh/g-C3N4催化剂。采用多种表征方法对催化剂的微观结构、组成成分进行研究。此外,还研究了反应温度和NaOH浓度对催化剂催化水合肼分解的影响。研究结果表明,催化剂优异的催化活性源于g-C3N4载体为金属Rh提供了锚定位点,并且载体和金属之间存在强相互作用。催化剂的催化活性随着反应温度的升高而不断提升,当NaOH浓度为0.75 mol/L时Rh/g-C3N4催化剂具有最高的催化活性。Rh/g-C3N4催化剂催化水合肼分解制氢的活化能为30.7 kJ/mol,TOF值为1466.4 h−1,在经过五次循环后,催化剂依旧保持着较好的催化活性,表明催化剂具有良好的循环稳定性。
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Abstract
In this paper, g-C3N4 obtained by calcining melamine at high temperature in static air was used as the carrier, and the precious metal Rh was used as the active component. The Rh nanoparticles were supported on the g-C3N4 support by a simple impregnation reduction method to prepare high activity and high selectivity. Various characterization methods were used to study the microstructure and composition of the catalyst. In addition, the effect of reaction temperature and NaOH concentration on the catalytic decomposition of hydrous hydrazine was also investigated. The results show that the excellent catalytic activity of the catalyst stems from the fact that the g-C3N4 support provides anchor sites for the metal Rh and the support and the strong metal-support interactions. The catalytic activity of the catalyst increases with the increase of the reaction temperature, and the Rh/g-C3N4 catalyst has the highest catalytic activity when the NaOH concentration is 0.75 mol/L. The Rh/g-C3N4 catalyst has an activation energy of 30.7 kJ/mol and TOF value of 1466.4 h−1 for catalyzing the decomposition of hydrous hydrazine for hydrogen production. After 5 cycles, the catalyst still maintains a good catalytic activity, indicating that the catalyst has a good cyclic stability.
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关键词
水合肼g-C3N4Rh分解制氢
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KeyWords
hydrous hydrazine;g-C3N4;rhodium;dehydrogenation
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基金项目(Foundation)
国家自然科学基金青年基金(22108238, U22A20408),安徽省自然科学基金青年基金(1908085QB68),安徽省科技重大专项(201903a05020055),中国博士后面上项目(2019M662060)和特别资助站中项目(2020T130580, PC2022046)资助
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DOI
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引用格式
邱小魁, 孙佳丽, 花俊峰, 郑君宁, 万超, 许立信. Rh/g-C3N4纳米催化剂催化水合肼分解制氢性能研究[J]. 燃料化学学报(中英文), 2023, 51(9): 1313-1320.
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Citation
QIU Xiao-kui, SUN Jia-li, HUA Jun-feng, ZHENG Jun-ning, WAN Chao, XU Li-xin. Hydrogen generation from hydrous hydrazine over Rh/g-C3N4 nanocatalysts[J]. Journal of Fuel Chemistry and Technology, 2023, 51(9): 1313-1320.
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