查看更多>>摘要：Significant improving g-C3N4's photocatalytic efficiency still remains a great challenge.In this work,we synthesized ultrathin and porous 2D g-C3N4 nanosheets with a controllable concentration of carbon vacancies and oxygen doping.Water vapor opens the heptazine units,introduces carbon vacancies,and acts as an oxygen source for oxygen doping under high temperatures.The synergistic effect of controllable carbon vacancies and oxygen doping can continuously regulate band structures and significantly improves the separation efficiency of photoexcited charges.As a result,the prepared g-C3N4 with vigoroso reduction potential exhibits a very high photocatalytic H2 evolution rate of 2.414 mmol g~(-1)h~(-1)under visible light and 7.414 mmol g~(-1)h~(-1)under ultraviolet-visible light,respectively,which outperforms the majority of the previously reported g-C3N4 with well-tuned band structure.This work offers a new design idea for highly active g-C3N4-based photocatalysts with a well-tuned band structure.
查看更多>>摘要：Electrochemical nitrogen reduction reaction can be adopted to generate renewable ammonia.That is recognized as a sustainable alternative to the Haber-Bosch process.However,the limited electrocatalytic activity remains the primary obstacle against viable application of the electrocatalytic ammonia fixation.Herein,a biomimetic three-dimensional NiCoP/CoMoP/Co(Mo3Se4)4@C/NF electrocatalyst is designed to have excellent NRR performance with an NH3 yield rate of 24.54 μg h~(-1)cm~(-2)and Faradaic efficiency of 23.15%.Based on the experimental and theoretical results,NiCoP/CoMoP/Co(Mo3Se4)4@C/NF electrocatalyst perfectly simulates the structural characteristics of biological nitrogenase,where Co(Mo3Se4)4 acts as the major active center while NiCoP and C0M0P contribute to controlling the electron transfer during NRR.Additionally,the coexistence of the three different heterojunction interfaces induces more effective electronic structure modulation compared with the single interface,thereby optimizing the reaction energy barrier of intermediates.This work has developed a synergistic strategy to boost the reaction kinetics via introducing multiple heterojunction interfaces.
NSTL