Design of electrochemical active boron(B)site at solid materials to understand the relationships between the localized structure,charge state at the B site and electrocatalytic activity plays a crucial role in boostin...Design of electrochemical active boron(B)site at solid materials to understand the relationships between the localized structure,charge state at the B site and electrocatalytic activity plays a crucial role in boosting the green electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))via two-electron oxygen reduction(2eORR)pathway.Herein,we demonstrate a carbon(C)and nitrogen(N)localized bonding microenvironment to modulate the charge state of B site at the boron-carbon nitride solid(BCNs)to realize the efficient selective electrocatalytic H_(2)O_(2)production.The localized chemical structure of N-B-N,N-B-C and C-B-C bonds at B site can be regulated through solid-state reaction between boron nitride(BN)and porous carbon(C)at variable temperatures.The optimized BCN-1100 achieves an outstanding H_(2)O_(2)selectivity of 89%and electron transfer number of 2.2(at 0.55 V vs.RHE),with the production of 10.55mmol/L during 2.5 h and the catalytic stability duration for 15000 cycles.Further first-principles calculations identified the dependency of localized bonding microenvironment on the OOH~*adsorption energies and relevant charge states at the boron site.The localized structure of B site with BNC_(2)-Gr configuration is predicted to be the highest 2eORR activity.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22161036,11904187,21961024 and 21961025)Natural Science Foundation of Inner Mongolia(Nos.2018JQ05 and 2019BS02007)+2 种基金Incentive Funding from Nano Innovation Institute(NII)of Inner Mongolia Minzu Universitythe Inner Mongolia Autonomous Region Funding Project for Science&Technology Achievement Transformation(Nos.CGZH2018156 and 2019GG261)Doctoral Scientific Research Foundation of Inner Mongolia Minzu University(Nos.BS437 and BS480)。
文摘Design of electrochemical active boron(B)site at solid materials to understand the relationships between the localized structure,charge state at the B site and electrocatalytic activity plays a crucial role in boosting the green electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))via two-electron oxygen reduction(2eORR)pathway.Herein,we demonstrate a carbon(C)and nitrogen(N)localized bonding microenvironment to modulate the charge state of B site at the boron-carbon nitride solid(BCNs)to realize the efficient selective electrocatalytic H_(2)O_(2)production.The localized chemical structure of N-B-N,N-B-C and C-B-C bonds at B site can be regulated through solid-state reaction between boron nitride(BN)and porous carbon(C)at variable temperatures.The optimized BCN-1100 achieves an outstanding H_(2)O_(2)selectivity of 89%and electron transfer number of 2.2(at 0.55 V vs.RHE),with the production of 10.55mmol/L during 2.5 h and the catalytic stability duration for 15000 cycles.Further first-principles calculations identified the dependency of localized bonding microenvironment on the OOH~*adsorption energies and relevant charge states at the boron site.The localized structure of B site with BNC_(2)-Gr configuration is predicted to be the highest 2eORR activity.
