Electrocatalytic Overall Water Splitting Of Supported Ruthenium-based Catalysts On Modified Two-dimensional CTF/MOF

Along with the rise of population and the development of economy,global energy demand will increase continuously in the foreseeable future.However,traditional carbon-based energy sources have the disadvantages of non-renewable,low utilization rate and environmental pollution.For sustainable development,human beings must innovate on traditional technologies,and then obtain a new energy with high energy value and easy storage.Hydrogen,an eco-friendly fuel with high energy density,is recognized as a promising medium for storage of the energy from these sustainable resources.So far,the industrial hydrogen production method is mainly electrolytic alkaline aqueous solution.Electrochemical water splitting device involves cathode?HER,Hydrogen Evolution Reaction?and anode?OER,Oxygen Evolution Reaction?.Therefore,it is an important question for study to design a low-cost,high-efficiency catalyst to be used in electrochemical hydrogen production.Despite more than a decade of research in this field,there are still many challenges that humans need to overcome.?1?The catalysts are expensive precious metals and their oxides.?2?The rate of the HER reaction is usually influenced by the kinetic properties of the OER reaction.An OER catalyst with slowly kinetic feature will devastatively reduce the conversion rate of the electrolyzed water system.So designing a catalyst to replace or reduce the use of precious maters will be considered as the right direction of hydrogen evolution.Nano-porous materials can be used as effective supports for electrocatalysts,which have attracted people's attention in recent years.Nano-porous materials can provide many active sites during loading or reaction process due to their particularly large specific surface area and pore structure.In many nano-porous materials,covalent organic framework and metal organic framework are the most prominent materials,and the particularity of their two-dimensional structure will have a good application prospect for electrocatalytic water splitting.?1?A covalent triazine framework material with bulk defects?D-CTFs?was synthesized and dissolved in organic solvent by two ligands,with the action of Br?nsted acid catalyst.Because of the special anchoring structure of d-ctfs,it can be used as the support of supported catalyst.Ru/D-CTFs-900 and Ru-Ru O₂/D-CTFs-300were synthesized by one pot calcination.The two electrode materials were applied to the electrochemical overall water splitting experiments at room temperature and pressure.The electrolytic voltage is 1.47 V at 10 m A?cm^-2.This performance is relatively excellent in the work that has been reported until now.And in terms of electron utilization,Ru/D-CTFs-900 and Ru-Ru O₂/D-CTFs-300 show a Faraday efficiency of more than 98%.And they show excellent stability over 20 hours in the case of constant voltage test experiments.The comparative experiments show that CTFs with bulk defects are significantly better than perfect CTFs.The DTF calculation results show that the synergy between the defective supports and the supported metal is a key factor affecting the electrocatalytic performance.?2?Under hydrothermal conditions,heteroatoms are doped into known 2D MOF?Metal Organic Layer,MOL?materials to obtain Doping-MOL.Then the ruthenium nanoparticles were successfully loaded onto Doping-MOL?Ru/Doping-MOL?.The two electrode materials were applied to the electrochemical overall water splitting experiments at room temperature and pressure.The electrolytic voltage is 1.55 V at 10m A?cm^-2with lots of bubbles on the electrode.The results of comparative experiments show that the doping of ruthenium heteroatoms is the key factor affecting the electrocatalytic performance.