Nano‐Ni‐Induced Electronic Modulation ofMoS2Nanosheets Enables Energy‐SavingH2Production and Sulfide Degradation

Electrocatalytic hydrogen evolution and sulfion (S 2− ) recycling are promising strategies for boosting H 2 production and removing environmental pollutants. Here, a nano‐Ni‐functionalized molybdenum disulfide (MoS 2 ) nanosheet was assembled on steel mesh (Ni‐MoS 2 /SM) for use in sulfide oxidation reaction‐assisted, energy‐saving H 2 production. Experimental and theoretical calculation results revealed that anchoring nano‐Ni on high‐surface‐area slack MoS 2 nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH ad , thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction. Meanwhile, the Ni/MoS 2 ‐based hydrogen evolution reaction + sulfide oxidation reaction system achieved nearly 100% hydrogen production efficiency and only consumed 61% less power per kWh than the oxygen evolution reaction + hydrogen evolution reaction system, which suggested our proposed Ni‐MoS 2 and novel hydrogen production system are promising for sustainable energy production.