| Chlor-alkail is one of the national pillar industries,and its electricity consumption accounts for 10%of the whole chemical industry.The key to realizing the sustainable development of chlor-alkali electrolysis in the future is to reduce energy consumption and optimize resource utilization.However,the chlorine evolution reaction（CER）and oxygen evolution reaction（OER）at the anode are highly competitive,and the hydrogen evolution reaction（HER）is carried out in conditions of high salt,high alkali,and high temperature,which will result in higher energy consumption in the actual electrolysis process and limit its development.Ruthenium（Ru）-based materials have attracted extensive attention due to the inherent high selectivity and activity,but the development is limited by their low oxidation potential,instability in acidic media,and expensive characteristics.Therefore,the preparation of Ru-based catalysts with low loading,high activity,and high stability is significant for the development of chlor-alkali electrolysis.This thesis studies on the Ru-basde catalysts with low cost,high activity and high stability,and modified by morphology construction,crystal regulation and catalyst-support interaction.And the structure-activity relationship between phase composition and catalytic activity was studied by physical characterization and electrochemical performance tests.The following are the primary research findings:（1）Constructing strong oxide-support interaction（SOSI）is guiding for regulating the atomic configuration and electronic structure.Ru O2 anchored on the in-situ Ti O2 nanobelts was synthesized by combining hydrothermal and calcination methods,where Ru content is only 0.83 wt.%（Ru O2-Ti O2 NBs-Ti）.It is proved that there is a strong oxide-support interaction between Ru O2 and Ti O2 by physical characterization analysis.The as-made catalyst is beneficial to explore more active sites and selective sites,thus exhibiting the excellent CER activity.The Ti O2 nanobelts grown in-situ Ti plate have an open geometry,which is beneficial to accelerate the release of bubbles and slow down the corrosion of Cl2.The composite Ti O2（antase Ti O2 and rutile Ti O2）support could be propitious to stabilize Ru O2 in its most active state(Ru4+)and promote its activity.In 5.0 M Na Cl（p H=2）,it only needs the overpotential of130 m V at the current density of 50 m A cm-2 and could still maintain good catalytic activity at 300 m A cm-2 for 408 h.This work provides a new insight into designing a Ru-based CER catalyst with high efficiency at large current density.（2）It is significant to realize chlor-alkali electrolysis and hydrogen evolution co-production for the energy industry upgrade.We synthesize the strong catalyst-support interaction in Mo2C supported Ru O2 nanoparticles coated on Ti O2 nanorods（Ru O2-Mo2C-Ti O2）with a low loading of Ru（0.95wt.%）.The physical characterization proved that there was a strong electronic interaction of Ru O2 with Mo2C,thereby effectively improving the catalytic activity and stability of Ru O2.And the electron-poor Mo optimized the binding strength to H and exhibited a small overpotential in the wide p H range.For CER（5.0 M Na Cl,p H=2）,the overpotential is 110 m V at 50 m A cm-2,and it can run stably for 380 h at 500 m A cm-2 with little activity attenuation.It also shows a good performance for HER(η-10/-500=28/266 m V)in the solution consisting of 3.0 M Na Cl and 3.0 M Na OH.It can also run stably for 200 h at the current density of 500 m A cm-2.Moreover,for simulated chlor-alkali electrolysis（3.0 M Na OH+3.0 M Na Cl//5.0 M Na Cl,p H=2,90℃）when we integrated the catalyst into a self-made electrolyzer,the current density of10 m A cm-2 could be driven by only 2.23 V,as well as having satisfactory stability for 12 h at 50 m A cm-2.This performance exceeds the industrial electrolyzer（low steel//dimensionally stable electrode（DSA）,2.80 V）.Therefore,this work provides a reference for designing stable Ru-based CER catalysts. |
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