引入内建电场增强光载流子分离以促进H2的生产OA北大核心CSTPCD

The construct of the internal electric field(IEF)is recognized as an effective driver for promoting charge migration and separation to enhance photocatalytic performance.In this study,one-dimensional nanorods of Mn0.2Cd0.8S(MCS)co-doped with interstitial chlorine(Clint)and substitutional chlorine(Clsub)were designed and synthesized using a one-step solvothermal method.The incorporation of Clint and Clsub led to an unbalanced charge distribution and the formation of IEF in the MCS nanorods,contributing to the improvement of photogenerated carrier kinetic behavior.Through density functional theory(DFT)calculations,the effect of Clint and Clsub doping on the activity of the MCS was visually explained by examining differences in electronic structure,charge distribution and H2 adsorption/desorption balance.Interestingly,the modulation of the energy band structure of MCS primarily resulted from the contribution of Clint,while Clsub playing a negligible role.Moreover,the Clsub further facilitated the optimization of Clint concerning the H2 adsorption-desorption Gibbs free energy(ΔGH*)of MCS.Ultimately,the ΔGH* of 0.9 Cl-MCS favored H2 production(1.14 vs.0.17 eV),leading to a 9 times increase in photocatalytic H2 production activity compared to MCS.This investigation presents a valuable approach for constructing IEF in bimetallic sulfide photocatalysts.