Surface Modulation of Hierarchical MoS2 Nanosheets by Ni Single Atoms for Enhanced Electrocatalytic Hydrogen Evolution

Abstract Surface modulation at the atomic level is an important approach for tuning surface chemistry and boosting the catalytic performance. Here, a surface modulation strategy is demonstrated through the decoration of isolated Ni atoms onto the basal plane of hierarchical MoS 2 nanosheets supported on multichannel carbon nanofibers for boosted hydrogen evolution activity. X‐ray absorption fine structure investigation and density functional theory (DFT) calculation reveal that the MoS 2 surface decorated with isolated Ni atoms displays highly strengthened H binding. Benefiting from the unique tubular structure and basal plane modulation, the newly developed MoS 2 catalyst exhibits excellent hydrogen evolution activity and stability. This single‐atom modification strategy opens up new avenues for tuning the intrinsic catalytic activity toward electrocatalytic water splitting and other energy‐related processes.