化工新型材料

化工新型材料 ›› 2023, Vol. 51 ›› Issue (6) : 186-190. DOI: 10.19817/j.cnki.issn1006-3536.2023.06.034

科学研究

Pd-P/g-C₃N₄催化剂的优化制备及在甲酸分解制氢中的应用

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Preparation of Pd-P/g-C₃N₄ catalyst and its application in hydrogen production by formic acid decomposition

Xia Yuanyu, Wang Yusheng, Pei Yujie, Xie Pinhong, Li Qiming, Li Fang

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Received
2022-02-17
Issue Date	Revised Date
2023-07-07	2022-02-17

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摘要

以氮化碳(g-C₃N₄)为载体,采用液相还原法制备了一系列Pd-P/g-C₃N₄催化剂用于甲酸分解制氢,通过优化还原温度和活性组分负载量可以显著提高催化剂性能。采用X射线衍射仪、透射电子显微镜和X射线光电子能谱仪对催化剂的晶相结构、微观形貌、活性组分分布以及价态进行分析,并通过甲酸分解制氢实验测试了催化剂的甲酸分解制氢活性。结果表明:使用次磷酸钠还原剂需要在较高还原温度(90℃)才能实现Pd-P活性组分在 g-C₃N₄载体表面的高度分散,获得较小的纳米粒子,过高或过低的还原温度都不利于制备高性能催化剂。当Pd负载量为8.0%(质量分数)时,2-Pd-P/g-C₃N₄催化剂表现出最佳催化性能,通过动力学研究和Arrhenius方程计算得到该催化剂的甲酸分解活化能为33.83kJ/mol。

Abstract

A series of Pd-P/C₃N₄ catalysts for hydrogen production from formic acid were prepared by liquid-phase reduction method using carbon nitride (g-C₃N₄) as the carrier.Here the catalytic activity of the catalysts was significantly improved by optimizing the reduction temperature and loading amounts of active components.The crystal structure,microstructure,active component distribution and valence state of the catalysts were analyzed by X-ray diffractometry (XRD),transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS).The activity of the catalyst for hydrogen production from formic acid decomposition was tested by formic acid decomposition experiment.The results showed that the reducing agent based on sodium hypophosphite needed a high reduction temperature (90℃) to achieve the high dispersion of the Pd-P active component on the surface of carbon nitride carrier,and to obtain small nanoparticles.Too high or too low reduction temperature was not conducive to the preparation of high-performance catalysts.When the Pd loading was 8.0% (mass fraction),the 2-Pd-P/g-C₃N₄ catalyst showed the best catalytic performance,and the activation energy of the catalyst for formic acid decomposition was 33.83kJ/mol calculated by the kinetic study and the Arrhenius equation.

关键词

甲酸 / 还原 / 催化剂 / 制氢

Key words

formic acid / reduction / catalyst / hydrogen production

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Pd-P/g-C₃N₄催化剂的优化制备及在甲酸分解制氢中的应用[J]. 化工新型材料, 2023, 51(6): 186-190 DOI:10.19817/j.cnki.issn1006-3536.2023.06.034

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参考文献

原文顺序 | 出版日期 | 本文引用

[1] 孙志聪,孟庆磊,马荣鹏,等.功能化氮化碳对Pd基甲酸分解制氢催化剂性能的促进作用[J].应用化学,2020,37(10):1187-1194.
[2] 马通祥,高雷章,胡蒙均,等.固体储氢材料研究进展[J].功能材料,2018,49(4):4001-4006.
[3] 杨静怡.储氢材料的研究及其进展[J].现代化工,2019,39(10):51-55.
[4] Wang C,Astruc D.Recent developments of nanocatalyzed liquid-phase hydrogen generation[J].Chemical Society Reviews,2021,50(5):3437-3484.
[5] 郭晓彤.钯基催化剂催化甲酸基体系脱氢的研究[D].济南:山东大学,2019.
[6] Fellay C,Dyson P J,Laurenczy G.A viable hydrogen-storage system based on selective formic acid decomposition with a ruthenium catalyst[J].Angewandte Chemie International Edition,2008,47(21):3966-3968.
[7] 王嘉琦,王秋颖,朱桐慧,等.甲烷重整制氢的研究现状分析[J].现代化工,2020,40(7):15-20.
[8] 李洪亮,潘哆吉,马维清.甲醇裂解制氢纯度控制与影响因素[J].化工管理,2020(33):128-129;133.
[9] 李建国,刘义,钟玉发,等.甲醇水蒸气重整制氢工艺现状及发展[J].石油化工技术与经济,2019,35(6):53-56.
[10] 高大伟.甲酸/氨硼烷制氢催化剂的构建与性能研究[D].长春:长春工业大学,2019.
[11] 石林,任小荣,张洪波,等.甲醇裂解制氢方法的研究进展[J].山东化工,2018,47(1):37-38.
[12] 杨青.甲醇制氢在工业应用中的工艺改良研究[J].云南化工,2019,46(9):162-163.
[13] 蔡翊宇.氮化碳负载钯纳米粒子催化甲酸分解和硝基化合物加氢[D].上海:上海交通大学,2014.
[14] Aldosari O.Hydrogen storage in formic acid as a renewable energy source using heterogeneous catalysis[J].Turkish Journal of Chemistry,2019,43(4):995-1005.
[15] 陈小芬,郭敏学,贾立山.氮修饰碳黑负载PdCu合金催化甲酸分解制氢性能研究[J].化工学报,2021,72(7):3637-3647.
[16] Gu X J.Synergistic catalysis of metal-organic framework-immobilized Au-Pd nanoparticles in dehydrogenation of formic acid for chemical hydrogen storage[J].Journal of the American Chemical Society,2011,133(31):11822-11825.
[17] Qing Y B.Gold supported on zirconia polymorphs for hydrogen generation from formic acid in base-free aqueous medium[J].Journal of Power Sources,2016,328:463-471.
[18] 马尚坤,刘艳,王少君,等.氮化碳负载AuPd纳米催化剂甲酸分解制氢性能[J].化学研究与应用,2020,32(6):1088-1093.
[19] 焦晓新,郑潇潇,张鸿斌,等.P促进Pd/C高效催化甲酸制氢的研究[J].厦门大学学报(自然科学版),2015,54(5):707-712.
[20] 王瑞斌.Pd-Co@Pd核壳催化剂催化甲酸脱氢的机理研究[D].长春:吉林大学,2020.
[21] 朱明兰.三维g-C₃N₄及其复合光催化剂的制备和产氢性能研究[D].北京:北京化工大学,2020.
[22] 武德伟.g-C₃N₄纳米管复合材料的光催化性能研究[D].南京:南京邮电大学,2020.
[23] Zhou X,Huang Y,Xing W,et al.High-quality hydrogen from the catalyzed decomposition of formic acid by Pd-Au/C and Pd-Ag/C[J].Chemical Communications,2008(30):3540-3542.
[24] 肖顺远,辛悦,邓庆芳.氮化碳负载AgPd合金催化剂的甲酸分解制氢性能[J].化工时刊,2019,33(2):8-9.