Mapping the kinetics of hydrogen evolution reaction on Ag via pseudo-single-crystal scanning electrochemical cell microscopy

Elucidating the structure-activity relationship in electrocatalysis is of fundamental interest for electrochemical energy conversion and storage.However,the heterogeneity in the surface structure of electrocatalysts,including the presence of various facets,poses an analytical challenge in revealing the true structure-activity relationship because the activity is conventionally measured on ensemble,resulting in an averaged activity that cannot be unequivocally associated with a single structural motif.Scanning electrochemical cell microscopy(SECCM)[1]combined with colocalized electron backscatter diffraction(EBSD)offers a direct way to reveal the correlative local electrochemical and structural information.Herein,we measured the hydrogen evolution reaction(HER)activity on Ag and its dependence on the crystal orientation.From the combined EBSD and SECCM mapping,it is found that Ag grains closer to{111}show a higher exchange current density,while those closer to{110}show a lower Tafel slope.The Tafel slope is also found to decrease with the step density increase.The ability to measure the electrocatalytic activity under a high mass-transfer rate allows us to reveal the activity difference at a high current density(up to 200 mA/cm^(2)).The approach reported here can be expanded to other systems to reveal the nature of active sites of electrocatalysis.

Integration strategies of hydrogen network in a refinery based on operational optimization of hydrotreating units

Inferior crude oil and fuel oil upgrading lead to escalating increase of hydrogen consumption in refineries.It is imperative to reduce the hydrogen consumption for energy-saving operations of refineries.An integration strategy of hydrogen network and an operational optimization model of hydrotreating(HDT)units are proposed based on the characteristics of reaction kinetics of HDT units.By solving the proposed model,the operating conditions of HDT units are optimized,and the parameters of hydrogen sinks are determined by coupling hydrodesulfurization(HDS),hydrodenitrification(HDN)and aromatic hydrogenation(HDA)kinetics.An example case of a refinery with annual processing capacity of eight million tons is adopted to demonstrate the feasibility of the proposed optimization strategies and the model.Results show that HDS,HDN and HDA reactions are the major source of hydrogen consumption in the refinery.The total hydrogen consumption can be reduced by 18.9%by applying conventional hydrogen network optimization model.When the hydrogen network is optimized after the operational optimization of HDT units is performed,the hydrogen consumption is reduced by28.2%.When the benefit of the fuel gas recovery is further considered,the total annual cost of hydrogen network can be reduced by 3.21×10~7CNY·a^(-1),decreased by 11.9%.Therefore,the operational optimization of the HDT units in refineries should be imposed to determine the parameters of hydrogen sinks base on the characteristics of reaction kinetics of the hydrogenation processes before the optimization of the hydrogen network is performed through the source-sink matching methods.