Preparation Of Ruthenium-based Nano-composite Catalyst And Study On Its Performance For Dehydrogenation And Hydrogenation

At present,with the rapid development of science and technology,the consumption of fossil fuels is rapidly and increasingly drying up.At the same time,it causes serious pollution to the environment.The large-scale industrial production also brings a large amount of organic wastewater discharge and serious water pollution.Therefore,seeking clean,pollution-free and renewable new energy and efficient treatment of organic dye wastewater is one of the urgent problems to be solved.Ammonia borane（AB）has become one of that ideal hydrogen source at present due to its many advantages such as non-toxicity,stability at normal temperature,high hydrogen storage capacity,etc.but it has the disadvantage of high stability in aqueous solution and being difficult to react,etc.organic dyes also have the problems of good stability in wat and being difficult to degrade under natural conditions,etc.Therefore,appropriate catalyst are needed to accelerate that reaction proces.In this paper,on the basis of previous studies,a series of ruthenium-based noble metal catalysts with high dispersibility and small particle size were prepared by chemical reduction method with the appropriate carrier,in order to reduce metal agglomeration and improve the catalytic performance.The catalytic performance for that generation of hydrogen by the hydrolysis of ammonia borane and the catalytic hydrogenation of organic dye are deeply studied,and the possible catalytic mechanism are preliminarily discussed.The main research contents are as follows:（1）SiO₂@TiO₂@Ru catalyst was prepared by in situ synthesis at room temperature for hydrogenation and dehydrogenation experiments.The morphology,structure and crystal form of the catalyst were characterized by TEM,XPS,XRD and IR.The experimental results show that the Si O₂@Ti O₂@Ru catalyst has excellent catalytic activity.At 298 K,the activation energy of hydrolysis of aminoborane（AB）is Ea=36.75 k J/mol.It shows a high catalytic activity.It still shows a good catalytic activity after five cycles.Moreover,it has an excellent degradation effect on the organic dye p-nitrothiophenol.The degradation rate can reach 98%after reacting for 7 min.（2）N-CS@Ru catalyst was prepared by in-situ synthesis at room temperature.Using 3-aminophenol and formaldehyde as raw materials,without template and surfactant,the preparation method was simple.The N-containing carbon spheres（N-CS）matrix was obtained by calcination.The morphology of the catalyst was characterized by TEM,XPS,XRD and IR.The experimental result show that that catalyst has excellent catalytic performance for both dehydrogenation and hydrogenation.At 298 K,the activation energy ea of ammoniacal borane（AB）hydrolysis is 23.94 k J/mol,and the cycle performance is good.the matrix has excellent catalytic degradation effect for organic dye to nitroaniline.the degradation rate can reach 98%within 10 min.（3）Resorcinol/formaldehyde（RF）resin ball is used as a template,a titanium dioxide layer is coated on the surface of the resorcinol/formaldehyde（RF）resin ball,the RF is coated for the second time,collapse is prevented in the process of matrix calcination,and finally the template is removed to obtain the hollow ball.the method is simple and easy to operate,the template can be removed through high temperature calcination,a hollow Ti O₂ carrier with controllable particle size is obtained,Ru-Pd NPs alloy with small size is uniformly and tightly attached on the hollow Ti O₂ matrix,the inorganic dye potassium ferricyanate and the organic pollutant p-nitroaniline were chosen as the target degradants to study the catalytic performance.The results show that the degradation rate of potassium ferricyanate reaches ninety-seven percent in 20 min and 99%in 8 min.All of them have better catalytic performance than single metal,proving that the synergistic effect between the two metals can significantly improve the activity of the catalyst.