Reversing the activity center in doped Pd₁₇Se₁₅ to achieve high stability toward the electrochemical hydrogen evolution reaction

Abstract

The use of hydrogen, being an environmentally cleaner source of energy, may reduce the pressing problem of CO₂ emissions due to the burning of conventional fossil fuels. However, the prolonged production of hydrogen is a major issue and can be solved through designing a stable electrocatalyst. In this work, we have designed a Ni-doped Pd₁₇Se₁₅ catalyst that retains its activity for 20000 electrochemical cycles. The enhanced stability of this electrocatalyst can be attributed to the reversal of the activity center from the Pd to the Se center through Ni substitution. The concept of activating the chalcogen center and deactivating the Pd site is supported through theoretical calculations. This work provides a unique strategy of tuning catalysts toward higher activity and stability.