Cu And Ni-Based Nanocatalytic Materials Derived From Metal-Organic Frameworks For Catalytci Applicaitons

As resource and energy consumption have been close to the environment load limit, resources and energy shortages are becoming a public concern. Thus, how to improve the usage of limited resources and energy has become one of the hotestresearch topic. In recent years, people have tried many ways to solve the resource and energy shortage problems.Developing new technologies and new methods to prepare novel materials to apply in industrial production is believed to be effeciveness for resource and energy conservation. The development of transitionmetal nanomaterials respresents a huge opportunity and is worthy of further studying to explore its great potential. At present, the controlled synthesize of copper and nickel nanomaterials have made great progress, however, to explore the influence factors in the process of generating copper and nickel nanomaterials, to design simple synthetic routes, to prepare a novel morphology of nanometer materials and expand its application still have the vital significance.This thesis is devoted to developing robust methods to synthesize Cu and Ni-based nanocatalytic materials. We started from Cu-BTC and Ni-BTC metal-organic frameworks and utilized them as precursors to synthesize Cu-BTC@GO and Ni-BTC@GO nanocomposites by rapping them with graphene (GO). Then, using the Cu-BTC@GO and Ni-BTC@GO nanocomposites as precursors, the Cu@GO and Ni@GO nanocatalytci materials were prepared by reducing such precursors in H2 atmosphere followed with the phosphorization. The structure, size, and morphology of Cu@GO and Ni@GO nanocomposites were studied and the catalytic performance for reduction of 4-NP was evaluated, to optimize and select the Cu@GO and Ni@GO nanocatalytic materials which has excellent performance. At the same time, we used Ni-BTC@GO as the precursor to prepare the Ni2P@GO through high temperature solid phase method, and studied the electrochemical hydrogen production performance.In the fist chapter of this thesis, we reviewed the progress of transition metal nanomaterials, and thus, to propose the research aim and content of this thesis.In the second chapter of this thesis, we used Cu-BTC and Ni-BTC as precursors to synthesize Cu-BTC@GO and Ni-BTC@GO nanocomposites. The structure, size, morphology and surface property were characterized by means of XRD, SEM, TEM and XPS. The catalytic performance of Cu-BTC@GO and Ni-BTC@GO nanocomposites for reduction of 4-NP was evaluated. It is revealed that the Cu-BTC@GO nanocomposites show superior catalytic performance for reduction of 4-NP. Then, using the Cu-BTC@GO and Ni-BTC@GO nanocomposites as precursors, the Cu@GO and Ni@GO nanocatalytci materials were prepared by reducing such precursors in H2 atmosphere followed with the phosphorization. The structure, size, and morphology of Cu@GO and Ni@GO nanocomposites were studied and the catalytic performance for reduction of 4-NP was evaluated, to optimize and select the Cu@GO and Ni@GO nano catalytic materials which has excellent performance.In the third chapter of this thesis, we synthesized Ni2P@GO nanocomposites using Ni-BTC@GO as precursor and hypophosphorous acid as phosphatizing agent and through controlling the ratio of Ni-BTC@GOprecursor and hypophosphorous acid, the morphology of Ni2P@GO can be modulated. The preparation, structure, size and morphology, and catalytic performance for photocatalytic hydrogen generation were studied. It is found that Ni2P@GO nanocomposites show excellent property for hydrogen generation. In comparison with the Ni2P prepared by direct reaction of nickel acetate with hypophosphorous acid, the Ni2P@GO synthesized using Ni-BTC@GO as precursor show superior catalyic performance for catalytic hydrogen generation. Thus, we developed a robust method for preparing Ni2P@GO nanocomposites with excellent electrocatalytic performance using hypophosphorous acid as phosphatizing agent and modulating the ratio of Ni-BTC@GO precursor and hypophosphorous acid.In the fourth chapter of this thesis, we summaried the scientific acheivement of this thesis and gave our prospect of future work.