Compared to aqueous-phase electrocatalytic nitrogen reduction reaction(NRR),lithium-mediated NRR(Li-NRR)theoretically enhances the intrinsic activity of NH3 production through spontaneous exothermic reactions between ...Compared to aqueous-phase electrocatalytic nitrogen reduction reaction(NRR),lithium-mediated NRR(Li-NRR)theoretically enhances the intrinsic activity of NH3 production through spontaneous exothermic reactions between Li and N_(2).However,the in-situ generated solid electrolyte interphase(SEI)during the reaction slows down the Li^(+)transport and nucleation kinetics,which further hinders the subsequent activation and protonation processes.Herein,a sophisticated amorphous-crystalline heterostructured SEI of Zn-LiF is formed by additive engineering.The concerted electron interplay between amorphous and crystalline domains is prone to generate lithiophobic Zn and lithiophilic LiF sites,where lithiophobic Zn accelerates Li^(+)diffusion within the SEI and avoids high concentration polarization,and lithiophilic LiF ensures homogeneous nucleation of diffused Li^(+)and its participation in subsequent reactions.Therefore,compared to conventional SEI,a more than 8-fold performance improvement is achieved in the additive-engineered heterogeneous lithiophobic-lithiophilic SEI,which exhibits a high NH_(3)yield rate of 11.58 nmol s^(−1)cm^(−2)and a Faradaic efficiency of 32.97%.Thus,exploiting the synergistic effects in heterogeneous lithiophobic-lithiophilic structures to achieve functional complementarity between different components opens a new avenue toward high-performance Li-NRR.展开更多
A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocat...A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocatalytic performance for water oxidation, which will contribute to the development of highly efficient catalysts for oxygen evolution.展开更多
基金supported by the National Natural Science Foundation of China(22178361,22378402,52302310)the International Partnership Project of CAS(039GJHZ2022029GC)+3 种基金the National Key R&D Program of China(2020YFA0710200)the Foundation of the Innovation Academy for Green Manufacture Institute,Chinese Academy of Sciences(IAGM2022D07)QinChuangYuan Cites High-level Innovation and Entrepreneurship Talent Programs(QCYRCXM-2022-335)the Open Project Program of Anhui Province International Research Center on Advanced Building Materials(JZCL2303KF).
文摘Compared to aqueous-phase electrocatalytic nitrogen reduction reaction(NRR),lithium-mediated NRR(Li-NRR)theoretically enhances the intrinsic activity of NH3 production through spontaneous exothermic reactions between Li and N_(2).However,the in-situ generated solid electrolyte interphase(SEI)during the reaction slows down the Li^(+)transport and nucleation kinetics,which further hinders the subsequent activation and protonation processes.Herein,a sophisticated amorphous-crystalline heterostructured SEI of Zn-LiF is formed by additive engineering.The concerted electron interplay between amorphous and crystalline domains is prone to generate lithiophobic Zn and lithiophilic LiF sites,where lithiophobic Zn accelerates Li^(+)diffusion within the SEI and avoids high concentration polarization,and lithiophilic LiF ensures homogeneous nucleation of diffused Li^(+)and its participation in subsequent reactions.Therefore,compared to conventional SEI,a more than 8-fold performance improvement is achieved in the additive-engineered heterogeneous lithiophobic-lithiophilic SEI,which exhibits a high NH_(3)yield rate of 11.58 nmol s^(−1)cm^(−2)and a Faradaic efficiency of 32.97%.Thus,exploiting the synergistic effects in heterogeneous lithiophobic-lithiophilic structures to achieve functional complementarity between different components opens a new avenue toward high-performance Li-NRR.
基金supported by the National Natural Science Foundation of China(No.21371173,51402298,91545125)the China Postdoctoral Foundation(No.2014M550846)
文摘A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocatalytic performance for water oxidation, which will contribute to the development of highly efficient catalysts for oxygen evolution.
