椰壳炭负载钌催化剂的制备及其催化氨硼烷水解制氢性能

石油炼制与化工 ›› 2023, Vol. 54 ›› Issue (7): 64-70.

椰壳炭负载钌催化剂的制备及其催化氨硼烷水解制氢性能

王小燕,张若凡,司航,王海龙

安徽工业大学化学与化工学院

收稿日期:2023-02-10 修回日期:2023-04-01 出版日期:2023-07-12 发布日期:2023-06-21
通讯作者: 王小燕 E-mail:15883724983@189.cn
基金资助:
安徽省自然科学基金青年基金项目;2022年国家级大学生创新创业训练计划项目;2021年省级大学生创新创业训练计划项目

PREPARATION OF COCONUT SHELL CARBON SUPPORTED RUTHENIUM AS A CATALYST FOR THE HYDROLYTIC DEHYDROGENATION OF AMMONIA BORANE

Received:2023-02-10 Revised:2023-04-01 Online:2023-07-12 Published:2023-06-21
Contact: Xiao-Yan WANG E-mail:15883724983@189.cn

摘要/Abstract

摘要： 以椰壳炭（CSC）为载体，通过浸渍-还原法负载活性组分Ru，制得Ru/CSC催化剂，利用X射线衍射、X射线光电子能谱、透射电镜和N2吸附-脱附等一系列表征手段来探究催化剂的微观结构及形貌；进而考察了光照、金属负载量、反应物浓度、催化剂用量、反应温度等因素对氨硼烷水解制氢反应速率的影响。结果表明：Ru与CSC之间存在金属-载体相互作用；以1.0%Ru/CSC为催化剂催化氨硼烷水解制氢反应，其在可见光照射条件下的催化性能明显优于无光照条件；氨硼烷水解制氢速率与Ru/CSC浓度呈正相关关系，催化剂的界面反应是氨硼烷水解制氢的控速步骤，与氨硼烷浓度无关；以1.0 %Ru/CSC在298 K下光催化氨硼烷水解制氢反应的转化频率（TOF）为334.8min^-1，表观活化能（Ea）为59.9 kJ/mol。

关键词: 钌, 催化剂, 椰壳炭, 氨硼烷, 水解制氢

Abstract: Ru/CSC catalysts were prepared by impregnation-reduction method using the coconut shell carbon (CSC) as support and Ru as active component, and the microstructure and morphology of the catalyst were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, TEM and N2 adsorption-desorption. The effects of light, metal loading, reactant concentration, catalyst dosage, and reaction temperature on the reaction rate of hydrogen production from ammonia borane hydrolysis were investigated. The results showed that there was a metal-support interaction between Ru and CSC, and the catalytic performance of 1.0% Ru/CSC catalyst for the hydrolysis of ammonia borane to hydrogen production under the condition of visible light irradiation was significantly better than that under the condition of no light irradiation. There was a positive correlation between the hydrogen production rate and Ru/CSC concentration. The interfacial reaction of catalyst was the rate-controlling step of hydrogen production from the hydrolysis of ammonia borane, which was independent of the concentration of ammonia borane. The conversion frequency (TOF) and apparent activation energy (Ea) were 334.8min^-1and 59.9 kJ/mol, respectively, for the photocatalytic hydrolysis of ammonia borane to hydrogen at 1.0% Ru/CSC at 298 K.

Key words: ruthenium, catalyst, coconut shell carbon, ammonia borane, hydrolytic dehydrogenation

王小燕张若凡司航王海龙. 椰壳炭负载钌催化剂的制备及其催化氨硼烷水解制氢性能[J]. 石油炼制与化工, 2023, 54(7): 64-70.

参考文献

[1]曹湘洪.能源转型中我国炼油工业面临的挑战与对策[J].石油炼制与化工, 2001, 52(10):1-9
[2]Dunn S.Hydrogen futures: Toward a sustainable energy system[J].International Journal of Hydrogen Energy, 2002, 27(3):235-264
[3]殷朝辉，杨占兵，李帅.氢气分离提纯用钯及钯合金膜的研究进展[J].稀有金属, 2021, 45(2):226-239
[4]赵永志，蒙波，陈霖新，等.氢能源的利用现状分析[J].化工进展, 2015, 34(9):3248-3255
[5]李慧珍，王芃远，陈学年.氨硼烷:一种高性能化学储氢材料[J].科学通报, 2014, 59(19):1823-1837
[6]Hu M G, Geanangel R A, Wendlandt W W.The thermal decomposition of ammonia borane[J].Thermochim Acta, 1978, 23(2):249-255
[7]Wang Ping, Kang XiangDong.Hydrogen–rich boron–containing materials for hydrogen storage[J].Dalton Transactions, 2008, 40(40):5400-5413
[8]马建丽，张晓霞，曹海燕，等.氨硼烷热分解放氢的研究进展[J].化工新型材料, 2016, 44(5):34-36
[9]Sun Daohua, Mazumder V, Metin ?, et al.Catalytic hydrolysis of ammonia borane via cobalt palladium nanoparticles[J].ACS Nano, 2011, 5(8):6458-6464
[10]Yang Kunzhou, Zhou Liqun, Yu Guofeng, et al.Ru nanoparticles supported on MIL-53 (Cr，Al) as efficient catalysts for hydrogen generation form hydrolysis of ammonia borane[J].International journal of hydrogen energy, 2016, 41(15):6300-6309
[11]Li Yuexiang, Wei Zhongyue, Liu Lin, et al.Ag nanoparticles supported on UiO-66 for selective oxidation of styrene[J].Inorganic Chemistry Communications, 2018, 88:47-50
[12]Chandra M, Xu Qiang.Room temperature hydrogen from aqueous ammonia-borane using noble metal nano-clusters as highly active catalysts[J].Journal of Power Sources, 2007, 168(1):135-142
[13]Wang Jun, Qin Yuling, Liu Xiang, et al. In situsynthesis of magnetically recyclable graphene-supported Pd@Co core-shell nanoparticles as efficient catalyst for hydrolytic dehydrogenation of ammonia borane[J].Journal of Materials Chemistry, 2012, 22(25):12468-12470
[14]Shen Junfeng, Yang Lan, Hu Kai, et al.Rh nanoparticles supported on graphene as efficient catalyst for hydrolytic dehydrogenation of amine boranes for chemical hydrogen storage[J].International Journal of Hydrogen Energy, 2015, 40(2):1062-1070
[15]Du Cheng, Ao Qiang, Cao Nan, et al.Facile synthesis of monodisperse ruthenium nanoparticles supported on graphene for hydrogen generation from hydrolysis of ammonia borane[J].International Journal of Hydrogen Energy, 2015, 40(18):6180-6187
[16]Sun Haijie, Liu Xingai, Chen Zhihao, et al.Performance of RuZrO2 catalysts for hydrogen generation from catalytic hydrolysis of ammonia borane[J].Journal of Guangxi Normal University (Natural Science Edition), 2021, 39(3):92-101
[17]孙海杰，刘欣改，陈志浩，等.羟基磷灰石负载催化氨硼烷产氢性能研究[J].江西师范大学学报自然科学版, 2020, 44(04):98-102
[18]Lv Penggang, Liu Dawei, Tian Bin, et al.Preparation of biomass-derived porous carbon supported Ni nanoparticles for CO2 reforming of CH4[J].New Journal of Chemistry, 2020, 44(29):12503-12513
[19]徐晨薇，童倩倩，莫晗，等.纳米催化剂的制备及其催化氨硼烷制氢性能研究[J].湖北大学学报, 2022, 44(5):0562-0570
[20]李鑫恺.以椰壳碳为载体的镁促Ni基CO2甲烷化催化剂的制备和性能评价[D]. 西北大学，2019.
[21]曹画画，沈永淼，施旭升，等.生物质炭负载钌催化剂催化氢化双环戊二烯[J].浙江理工大学学报, 2022, 47(5):746-754